Low temperature plasma reaction device and hydrogen sulfide decomposition method

11691119 · 2023-07-04

Assignee

Inventors

Cpc classification

International classification

Abstract

Described are a low temperature plasma reaction device and a hydrogen sulfide decomposition method. The reaction device includes: a first cavity; a second cavity, the second cavity being embedded inside or outside the first cavity; an inner electrode, the inner electrode being arranged in the first cavity; an outer electrode; and a barrier dielectric arranged between the outer electrode and the inner electrode. The hydrogen sulfide decomposition method includes: implementing dielectric barrier discharge at the outer electrode and the inner electrode of the low temperature plasma reaction device, introducing a raw material gas containing hydrogen sulfide into the first cavity to implement a hydrogen sulfide decomposition method, and continuously introducing a thermally conductive medium into the second cavity in order to control the temperature of the first cavity of the low temperature plasma reaction device.

Claims

1. A low-temperature plasma reaction apparatus, the reaction apparatus comprising: a first cavity provided with a first inlet and a first outlet, respectively; a second cavity nested outside or inside the first cavity, and a second inlet and a second outlet are respectively arranged on the second cavity; an inner electrode, at least part of the inner electrode extends into the first cavity; an outer electrode forming at least part of a sidewall of the first cavity or being disposed on the sidewall of the first cavity in a surrounding manner; and a barrier dielectric disposed between the inner electrode and the outer electrode such that a discharge region between the inner electrode and the outer electrode is separated by the barrier dielectric; both the inner electrode and the outer electrode are solid electrodes, and the shapes of the inner electrode and the outer electrode are matched with each other to form an isodiametric structure; the distance between an outer sidewall of the inner electrode and an inner sidewall of the outer electrode is denoted as L.sub.1, the thickness of the barrier dielectric is denoted as D.sub.1, L.sub.2=L.sub.1−D.sub.1, and the proportional relation between L.sub.2 and D.sub.1 is (0.1˜30):1; wherein the first inlet is disposed at an upper portion of the first cavity, and the first outlet is disposed at a lower part and/or a bottom of the first cavity; the first outlet includes a gas product outlet and a liquid product outlet, and the gas product outlet is disposed at the lower part of the first cavity, and the liquid product outlet is disposed at the bottom of the first cavity; the gas product outlet is disposed below the discharge region, and a proportional relationship between a height H.sub.1 of the gas product outlet with respect to the bottom of the first cavity and a length L.sub.3 of the discharge region is: H.sub.1:L.sub.3=1:(30˜300).

2. The low-temperature plasma reaction apparatus according to claim 1, wherein the second cavity is nested outside the first cavity, the reaction apparatus further comprising: a third cavity nested inside the first cavity, and the inner electrode forms at least part of a sidewall of the third cavity or is disposed on the sidewall of the third cavity in a surrounding manner.

3. The low-temperature plasma reaction apparatus according to claim 2, wherein the inner electrode forms at least part of a sidewall of the third cavity or is disposed on the outer sidewall of the third cavity in a surrounding manner.

4. The low-temperature plasma reaction apparatus according to claim 1, wherein the second cavity is nested inside the first cavity, and the inner electrode forms at least part of a sidewall of the second cavity or is disposed on the sidewall of the second cavity in a surrounding manner.

5. The low-temperature plasma reaction apparatus according to claim 4, wherein the inner electrode forms at least part of the sidewall of the second cavity or is disposed on outer sidewall of the second cavity in a surrounding manner.

6. The low-temperature plasma reaction apparatus according to claim 4, wherein the reaction apparatus further comprising: a third cavity nested outside the first cavity.

7. The low-temperature plasma reaction apparatus according to claim 2, wherein the third cavity is provided with a third inlet and a third outlet, respectively.

8. The low-temperature plasma reaction apparatus according to claim 1, wherein the barrier dielectric forms at least part of a sidewall of the first cavity, or the barrier dielectric is disposed on an inner sidewall of the first cavity in a surrounding manner.

9. The low-temperature plasma reaction apparatus according to claim 1, wherein the first cavity is formed by a barrier dielectric.

10. The low-temperature plasma reaction apparatus according to claim 1, wherein the outer electrode is disposed on an outer sidewall of the first cavity in a surrounding manner, and the barrier dielectric forms at least part of the sidewall of the first cavity.

11. The low-temperature plasma reaction apparatus according to claim 1, wherein the barrier dielectric is disposed on at least part of an outer surface of the inner electrode such that at least a part of the outer surface of the inner electrode is wrapped with the barrier dielectric.

12. The low-temperature plasma reaction apparatus according to claim 1, wherein the barrier dielectric is disposed between the inner electrode and the outer electrode in a surrounding manner, both the distance between the barrier dielectric and the inner electrode and the distance between the barrier dielectric and the outer electrode are greater than 0.

13. The low-temperature plasma reaction apparatus according to claim 1, wherein the number of the first cavity is 1; the first cavity is composed of at least two reaction tubes arranged in parallel and having top and bottoms respectively communicating with each other, and each reaction tube is provided with an inner electrode, an outer electrode and a barrier dielectric, respectively; a proportional relationship between L.sub.2 and D.sub.1 in each of said reaction tubes is: L.sub.2:D.sub.1=(0.1˜30):1; the inner electrodes in each of the reaction tubes are connected in parallel with each other; and the outer electrodes in each of the reaction tubes are connected in parallel with each other.

14. The low-temperature plasma reaction apparatus according to claim 1, wherein the reaction apparatus comprises two or more first cavities, and each of the first cavities is provided with an inner electrode, an outer electrode and a barrier dielectric, respectively; each of the inner electrodes are connected in parallel with each other; and each of the outer electrodes are connected in parallel with one another.

15. The low-temperature plasma reaction apparatus according to claim 1, wherein the material of the barrier dielectric is an electrically insulating material; each of the outer electrode and the inner electrode is independently selected from the group consisting of conductive materials.

16. The low-temperature plasma reaction apparatus according to claim 1, wherein the reaction apparatus further comprises a ground lead, one end of the ground lead is electrically connected to a grounding electrode, which is the outer electrode or the inner electrode, and the other of the outer electrode and the inner electrode is a high-voltage electrode.

17. The low-temperature plasma reaction apparatus according to claim 1, wherein the second inlet and the second outlet are disposed at a lower portion and an upper portion of the second cavity, respectively.

18. The low-temperature plasma reaction apparatus according to claim 7, wherein the third inlet and the third outlet are disposed at a lower portion and an upper portion of the third cavity, respectively.

19. A method for decomposing hydrogen sulfide, which is carried out in the low-temperature plasma reaction apparatus according to claim 1, the method comprising: connecting one of the outer electrode and the inner electrode of the low-temperature plasma reaction apparatus with a high-voltage power supply, the other one of the outer electrode and the inner electrode is grounded to carry out the dielectric barrier discharge; introducing a feed gas containing hydrogen sulfide into the first cavity from the first inlet of the first cavity of the low-temperature plasma reaction apparatus to carry out decomposition reaction of the hydrogen sulfide; discharging a material flow obtained after the decomposition via the first outlet; and continuously introducing a heat-conducting medium into the second cavity of the low-temperature plasma reaction apparatus from the second inlet and discharging the heat-conducting medium via the second outlet so as to control the temperature of the first cavity of the low-temperature plasma reaction apparatus.

20. The method according to claim 19, wherein the reaction apparatus comprises: a third cavity nested outside or inside said first cavity, the method further comprising: continuously introducing the heat-conducting medium into the third cavity of the low-temperature plasma reaction apparatus from a third inlet and discharging the heat-conducting medium via the third outlet, which is in synergy with continuously introducing the heat-conducting medium into the second cavity of the low-temperature plasma reaction apparatus from the second inlet and discharging the heat-conducting medium via the second outlet so as to control the temperature of the first cavity of the low-temperature plasma reaction apparatus.

21. The method according to claim 19, wherein the conditions of dielectric barrier discharge comprise: the discharge voltage is 2 kV˜80 kV; the discharge frequency is 200˜30000 Hz; the conditions of decomposition reaction comprise: the reaction temperature is 0˜800° C., the reaction pressure is 0-0.6 MPa; the residence time of the feed gas containing the hydrogen sulfide in the discharge region of the low-temperature plasma reaction apparatus is 1×10.sup.−5˜120 s.

22. The process according to claim 19, wherein the decomposition reaction of hydrogen sulfide is carried out in the presence of a carrier gas, which is at least one selected from the group consisting of nitrogen, hydrogen, helium, argon, water vapor, carbon monoxide, carbon dioxide, methane, ethane and propane.

Description

DESCRIPTION OF THE DRAWINGS

(1) FIG. 1a is a structurally schematic view of a preferred specific embodiment of the low-temperature plasma reaction apparatus provided by the invention, in which a second cavity is disposed outside a first cavity.

(2) FIG. 1b is a structurally schematic view of a preferred specific embodiment of the low-temperature plasma reaction apparatus provided by the invention, in which a second cavity is disposed inside a first cavity.

(3) FIG. 1c is a structurally schematic view of a preferred specific embodiment of the low-temperature plasma reaction apparatus provided by the invention, in which a third cavity is disposed, and the second cavity and the third cavity are respectively arranged inside and outside the first cavity.

(4) FIG. 2a is a structurally schematic view of another preferred specific embodiment of the low-temperature plasma reaction apparatus provided by the invention, in which a second cavity is disposed outside a first cavity.

(5) FIG. 2b is a structurally schematic view of another preferred specific embodiment of the low-temperature plasma reaction apparatus provided by the invention, in which a second cavity is disposed inside a first cavity.

(6) FIG. 2c is a structurally schematic view of another preferred specific embodiment of the low-temperature plasma reaction apparatus provided by the invention, in which a third cavity is disposed, and the second cavity and the third cavity are respectively arranged inside and outside the first cavity.

(7) FIG. 3a is a structurally schematic view of another preferred specific embodiment of the low-temperature plasma reaction apparatus provided by the invention, in which a second cavity is disposed outside a first cavity.

(8) FIG. 3b is a structurally schematic view of another preferred specific embodiment of the low-temperature plasma reaction apparatus provided by the invention, in which a second cavity is disposed inside a first cavity.

(9) FIG. 3c is a structurally schematic view of another preferred specific embodiment of the low-temperature plasma reaction apparatus provided by the invention, in which a third cavity is disposed, and the second cavity and the third cavity are respectively arranged inside and outside the first cavity.

(10) FIG. 4a is a structurally schematic view of another preferred specific embodiment of the low-temperature plasma reaction apparatus provided by the invention, in which a second cavity is disposed outside a first cavity.

(11) FIG. 4b is a structurally schematic view of another preferred specific embodiment of the low-temperature plasma reaction apparatus provided by the invention, in which a second cavity is disposed inside a first cavity.

(12) FIG. 4c is a structurally schematic view of another preferred specific embodiment of the low-temperature plasma reaction apparatus provided by the invention, in which a third cavity is disposed, and the second cavity and the third cavity are respectively arranged inside and outside the first cavity.

DESCRIPTION OF REFERENCE SIGNS

(13) 1. First cavity 2. Second cavity 3. Inner electrode 4. Outer electrode 5. Ground lead 6. Barrier dielectric 7. Third cavity 11. First inlet 12. Gas product outlet 13. Liquid product outlet 21. Second inlet 22. Second outlet 71. Third inlet 72. Third outlet

DETAILED DESCRIPTION OF THE PREFERRED EMBODIMENTS

(14) The endpoints and any value of the ranges disclosed herein are not limited to the precise ranges or values, such ranges or values shall be comprehended as comprising the values adjacent to the ranges or values. As for numerical ranges, the endpoint values of the various ranges, the endpoint values and the individual point value of the various ranges, and the individual point values may be combined with one another to produce one or more new numerical ranges, which should be deemed have been specifically disclosed herein.

(15) The following content in conjunction with FIG. 1a provides the structure of a preferred embodiment of the low-temperature plasma reaction apparatus of the present invention, specifically:

(16) the reaction apparatus has a coaxial jacket cylinder structure, and the reaction apparatus comprises:

(17) a first cavity 1 provided with a first inlet 11 and a first outlet, respectively;

(18) a second cavity 2 nested outside the first cavity 1, and a second inlet 21 and a second outlet 22 are respectively arranged on the second cavity 2;

(19) an inner electrode 3 disposed in the first cavity 1;

(20) an outer electrode 4 forming at least part of the sidewall of the first cavity 1 or is disposed on the outer sidewall of the first cavity 1 in a surrounding manner; and

(21) a barrier dielectric forming at least part of the sidewall of the first cavity 1 or is disposed on the inner sidewall of the first cavity 1 in a surrounding manner, and the barrier dielectric is disposed between the inner electrode 3 and the outer electrode 4 such that a discharge region between the inner electrode 3 and the outer electrode 4 is spaced by the barrier dielectric;
both the inner electrode 3 and the outer electrode 4 are solid electrodes, and the shapes of the inner electrode 3 and the outer electrode 4 are matched with each other to form an isodiametric structure;
the distance between the outer sidewall of the inner electrode 3 and the inner sidewall of the outer electrode 4 is denoted as L.sub.1, the thickness of the barrier dielectric 6 is denoted as D.sub.1, L.sub.2=L.sub.1−D.sub.1, and the proportional relation between L.sub.2 and D.sub.1 is (0.1˜100):1, preferably (0.1˜30):1, more preferably (0.2˜15):1.

(22) According to the invention, the outer electrode 4 is preferably disposed on the outer sidewall of the first cavity 1 in a surrounding manner, and the barrier dielectric forms at least part of the sidewall of the first cavity 1.

(23) The following content in conjunction with FIG. 1b provides the structure of a preferred embodiment of the low-temperature plasma reaction apparatus of the present invention, specifically:

(24) the reaction apparatus has a coaxial jacket cylinder structure, and the reaction apparatus comprises:

(25) a first cavity 1 provided with a first inlet 11 and a first outlet, respectively;

(26) a second cavity 2 nested inside the first cavity 1, and a second inlet 21 and a second outlet 22 are respectively arranged on the second cavity 2;

(27) an inner electrode 3 disposed in the first cavity 1;

(28) an outer electrode 4 forming at least part of the sidewall of the first cavity 1 or is disposed on the outer sidewall of the first cavity 1 in a surrounding manner; and

(29) a barrier dielectric forming at least part of the sidewall of the first cavity 1 or is disposed on the inner sidewall of the first cavity 1 in a surrounding manner, and the barrier dielectric is disposed between the inner electrode 3 and the outer electrode 4 such that a discharge region between the inner electrode 3 and the outer electrode 4 is spaced by the barrier dielectric;
both the inner electrode 3 and the outer electrode 4 are solid electrodes, and the shapes of the inner electrode 3 and the outer electrode 4 are matched with each other to form an isodiametric structure;
the distance between the outer sidewall of the inner electrode 3 and the inner sidewall of the outer electrode 4 is denoted as L.sub.1, the thickness of the barrier dielectric 6 is denoted as D.sub.1, L.sub.2=L.sub.1−D.sub.1, and the proportional relation between L.sub.2 and D.sub.1 is (0.1˜100):1, preferably (0.1˜30):1, more preferably (0.2˜15):1.

(30) FIG. 1c illustrates a structure of a preferred embodiment of the low-temperature plasma reaction apparatus of the present invention, the low-temperature plasma reaction apparatus illustrated in FIG. 1c differs from the low-temperature plasma reaction apparatus illustrated in FIG. 1a and FIG. 1b in that: the low-temperature plasma reaction apparatus in FIG. 1c further comprises a third cavity 7, the third cavity 7 and the second cavity 2 are respectively disposed on both sides of the first cavity 1; in addition, a heat-conducting medium is continuously introduced into and discharged from both the third cavity 7 and the second cavity 2. In the third cavity, the heat-conducting medium is introduced into the third cavity from the third inlet 71 and is discharged via the third outlet 72.

(31) The following content in conjunction with FIG. 2a provides the structure of a preferred embodiment of the low-temperature plasma reaction apparatus of the present invention, specifically:

(32) the reaction apparatus has a coaxial jacket cylinder structure, and the reaction apparatus comprises:

(33) a first cavity 1 provided with a first inlet 11 and a first outlet, respectively;

(34) a second cavity 2 nested outside the first cavity 1, and a second inlet 21 and a second outlet 22 are respectively arranged on the second cavity 2;

(35) an inner electrode 3 disposed in the first cavity 1;

(36) an outer electrode 4 forming at least part of the sidewall of the first cavity 1 or is disposed on the inner sidewall of the first cavity 1 in a surrounding manner; and

(37) a barrier dielectric 6 disposed on at least a part of an outer surface of the inner electrode 3 such that the outer surface of the inner electrode 3 at least partially protruding into the first cavity 1 is wrapped with the barrier dielectric 6, and the disposed position of said barrier dielectric 6 causes that a discharge region between the inner electrode and the outer electrode is spaced by the barrier dielectric;
both the inner electrode 3 and the outer electrode 4 are solid electrodes, and the shapes of the inner electrode 3 and the outer electrode 4 are matched with each other to form an isodiametric structure;
the distance between the outer sidewall of the inner electrode 3 and the inner sidewall of the outer electrode 4 is denoted as L.sub.1, the thickness of the barrier dielectric 6 is denoted as D.sub.1, L.sub.2=L.sub.1−D.sub.1, and the proportional relation between L.sub.2 and D.sub.1 is (0.1˜100):1, preferably (0.1˜30):1, more preferably (0.2˜15):1.

(38) The following content in conjunction with FIG. 2b provides the structure of a preferred embodiment of the low-temperature plasma reaction apparatus of the present invention, specifically:

(39) the reaction apparatus has a coaxial jacket cylinder structure, and the reaction apparatus comprises:

(40) a first cavity 1 provided with a first inlet 11 and a first outlet, respectively;

(41) a second cavity 2 nested inside the first cavity 1, and a second inlet 21 and a second outlet 22 are respectively arranged on the second cavity 2;

(42) an inner electrode 3 disposed in the first cavity 1;

(43) an outer electrode 4 forming at least part of the sidewall of the first cavity 1 or is disposed on the inner sidewall of the first cavity 1 in a surrounding manner; and

(44) a barrier dielectric 6 disposed on at least a part of an outer surface of the inner electrode 3 such that the outer surface of the inner electrode 3 at least partially protruding into the first cavity 1 is wrapped with the barrier dielectric 6, and the disposed position of said barrier dielectric 6 causes that a discharge region between the inner electrode and the outer electrode is spaced by the barrier dielectric;
both the inner electrode 3 and the outer electrode 4 are solid electrodes, and the shapes of the inner electrode 3 and the outer electrode 4 are matched with each other to form an isodiametric structure;
the distance between the outer sidewall of the inner electrode 3 and the inner sidewall of the outer electrode 4 is denoted as L.sub.1, the thickness of the barrier dielectric 6 is denoted as D.sub.1, L.sub.2=L.sub.1−D.sub.1, and the proportional relation between L.sub.2 and D.sub.1 is (0.1˜100):1, preferably (0.1˜30):1, more preferably (0.2˜15):1.

(45) FIG. 2c illustrates a structure of a preferred embodiment of the low-temperature plasma reaction apparatus of the present invention, the low-temperature plasma reaction apparatus illustrated in FIG. 2c differs from the low-temperature plasma reaction apparatus illustrated in FIG. 2a and FIG. 2b in that: the low-temperature plasma reaction apparatus in FIG. 2c further comprises a third cavity 7, the third cavity 7 and the second cavity 2 are respectively disposed on both sides of the first cavity 1; in addition, a heat-conducting medium is continuously introduced into and discharged from both the third cavity 7 and the second cavity 2. In the third cavity, the heat-conducting medium is introduced into the third cavity from the third inlet 71 and is discharged via the third outlet 72.

(46) The following content in conjunction with FIG. 3a provides the structure of a preferred embodiment of the low-temperature plasma reaction apparatus of the present invention, specifically:

(47) the reaction apparatus has a coaxial jacket cylinder structure, and the reaction apparatus comprises:

(48) a first cavity 1 provided with a first inlet 11 and a first outlet, respectively;

(49) a second cavity 2 nested outside the first cavity 1, and a second inlet 21 and a second outlet 22 are respectively arranged on the second cavity 2;

(50) an inner electrode 3 disposed in the first cavity 1;

(51) an outer electrode 4 forming at least part of the sidewall of the first cavity 1 or is disposed on the outer sidewall of the first cavity 1 in a surrounding manner; and

(52) the barrier dielectric 6 is disposed between the inner electrode 3 and the outer electrode 4 in a surrounding manner, both the distance between the barrier dielectric and the inner electrode 3 and the distance between the barrier dielectric and the outer electrode 4 are greater than 0, and the disposed position of said barrier dielectric 6 causes that a discharge region between the inner electrode and the outer electrode is spaced by the barrier dielectric;
both the inner electrode 3 and the outer electrode 4 are solid electrodes, and the shapes of the inner electrode 3 and the outer electrode 4 are matched with each other to form an isodiametric structure;
the distance between the outer sidewall of the inner electrode 3 and the inner sidewall of the outer electrode 4 is denoted as L.sub.1, the thickness of the barrier dielectric 6 is denoted as D.sub.1, L.sub.2=L.sub.1−D.sub.1, and the proportional relation between L.sub.2 and D.sub.1 is (0.1˜100):1, preferably (0.1˜30):1, more preferably (0.2˜15):1.

(53) The following content in conjunction with FIG. 3b provides the structure of a preferred embodiment of the low-temperature plasma reaction apparatus of the present invention, specifically:

(54) the reaction apparatus has a coaxial jacket cylinder structure, and the reaction apparatus comprises:

(55) a first cavity 1 provided with a first inlet 11 and a first outlet, respectively;

(56) a second cavity 2 nested inside the first cavity 1, and a second inlet 21 and a second outlet 22 are respectively arranged on the second cavity 2;

(57) an inner electrode 3 disposed in the first cavity 1;

(58) an outer electrode 4 forming at least part of the sidewall of the first cavity 1 or is disposed on the inner sidewall of the first cavity 1 in a surrounding manner; and

(59) the barrier dielectric 6 is disposed between the inner electrode 3 and the outer electrode 4 in a surrounding manner, both the distance between the barrier dielectric and the inner electrode 3 and the distance between the barrier dielectric and the outer electrode 4 are greater than 0, and the disposed position of said barrier dielectric 6 causes that a discharge region between the inner electrode and the outer electrode is spaced by the barrier dielectric;
both the inner electrode 3 and the outer electrode 4 are solid electrodes, and the shapes of the inner electrode 3 and the outer electrode 4 are matched with each other to form an isodiametric structure;
the distance between the outer sidewall of the inner electrode 3 and the inner sidewall of the outer electrode 4 is denoted as L.sub.1, the thickness of the barrier dielectric 6 is denoted as D.sub.1, L.sub.2=L.sub.1−D.sub.1, and the proportional relation between L.sub.2 and D.sub.1 is (0.1˜100):1, preferably (0.1˜30):1, more preferably (0.2˜15):1.

(60) FIG. 3c illustrates a structure of a preferred embodiment of the low-temperature plasma reaction apparatus of the present invention, the low-temperature plasma reaction apparatus illustrated in FIG. 3c differs from the low-temperature plasma reaction apparatus illustrated in FIG. 3a and FIG. 3b in that: the low-temperature plasma reaction apparatus in FIG. 3c further comprises a third cavity 7, the third cavity 7 and the second cavity 2 are respectively disposed on both sides of the first cavity 1; in addition, a heat-conducting medium is continuously introduced into and discharged from both the third cavity 7 and the second cavity 2. In the third cavity, the heat-conducting medium is introduced into the third cavity from the third inlet 71 and is discharged via the third outlet 72.

(61) The following content in conjunction with FIG. 4a provides the structure of another preferred embodiment of the low-temperature plasma reaction apparatus of the present invention, specifically:

(62) the reaction apparatus has a jacket cylinder structure, and the reaction apparatus comprises:

(63) a first cavity formed by at least two reaction tubes arranged in parallel and having top and bottoms respectively communicating with each other; the first cavity 1 is provided with a first inlet 11 and a first outlet, respectively;

(64) a second cavity 2 nested outside the first cavity 1, and a second inlet 21 and a second outlet 22 are respectively arranged on the second cavity 2;

(65) an inner electrode 3 disposed in each of the reaction tubes, respectively;

(66) an outer electrode 4 forming at least part of the sidewall of each of the reaction tubes or is disposed on the sidewall of each of the reaction tubes in a surrounding manner; and

(67) the barrier dielectric 6 is disposed between the inner electrode 3 and the outer electrode 4 in each of the reaction tubes by a surrounding manner, and the disposed position of said barrier dielectric 6 causes that a discharge region between the inner electrode 3 and the outer electrode 4 is spaced by the barrier dielectric;
wherein in each of the reaction tubes, the distance between the outer sidewall of the inner electrode 3 and the inner sidewall of the outer electrode 4 is denoted as L.sub.1, the thickness of the barrier dielectric 6 is denoted as D.sub.1, L.sub.2=L.sub.1−D.sub.1, and the proportional relation between L.sub.2 and D.sub.1 is (0.1˜100):1, preferably (0.1˜30):1, more preferably (0.2˜15):1.

(68) The following content in conjunction with FIG. 4b provides the structure of another preferred embodiment of the low-temperature plasma reaction apparatus of the present invention, specifically:

(69) the reaction apparatus has a jacket cylinder structure, and the reaction apparatus comprises:

(70) a first cavity formed by at least two reaction tubes arranged in parallel and having top and bottoms respectively communicating with each other; the first cavity 1 is provided with a first inlet 11 and a first outlet, respectively;

(71) a second cavity 2 nested inside the first cavity 1, and a second inlet 21 and a second outlet 22 are respectively arranged on the second cavity 2;

(72) an inner electrode 3 disposed in each of the reaction tubes, respectively;

(73) an outer electrode 4 forming at least part of the sidewall of each of the reaction tubes or is disposed on the sidewall of each of the reaction tubes in a surrounding manner; and

(74) the barrier dielectric 6 is disposed between the inner electrode 3 and the outer electrode 4 in each of the reaction tubes by a surrounding manner, and the disposed position of said barrier dielectric 6 causes that a discharge region between the inner electrode 3 and the outer electrode 4 is spaced by the barrier dielectric;
wherein in each of the reaction tubes, the distance between the outer sidewall of the inner electrode 3 and the inner sidewall of the outer electrode 4 is denoted as L.sub.1, the thickness of the barrier dielectric 6 is denoted as D.sub.1, L.sub.2=L.sub.1−D.sub.1, and the proportional relation between L.sub.2 and D.sub.1 is (0.1˜100):1, preferably (0.1˜30):1, more preferably (0.2˜15):1.

(75) FIG. 4c illustrates a structure of a preferred embodiment of the low-temperature plasma reaction apparatus of the present invention, the low-temperature plasma reaction apparatus illustrated in FIG. 4c differs from the low-temperature plasma reaction apparatus illustrated in FIG. 4a and FIG. 4b in that: the low-temperature plasma reaction apparatus in FIG. 4c further comprises a third cavity 7, the third cavity 7 and the second cavity 2 are respectively disposed on both sides of the first cavity 1; in addition, a heat-conducting medium is continuously introduced into and discharged from both the third cavity 7 and the second cavity 2. In the third cavity, the heat-conducting medium is introduced into the third cavity from the third inlet 71 and is discharged via the third outlet 72.

(76) In the present invention, when the second cavity 2 or the third cavity 7 is disposed in the first cavity 1, in order to facilitate description, the second cavity 2 or the third cavity 7 disposed in the first cavity 1 is named as an “internal cavity”.

(77) Preferably, the inner electrode 3 forms at least part of the sidewall of the internal cavity or is disposed on the sidewall of the internal cavity in a surrounding manner.

(78) According to a preferred specific embodiment, the inner electrode 3 is disposed on the outer sidewall of the third cavity 7 in a surrounding manner.

(79) According to a preferred specific embodiment, the inner electrode 3 is disposed on the inner sidewall of the third cavity 7 in a surrounding manner, and at least a portion of the sidewall of the third cavity 7 is formed by the barrier dielectric 6. That is, in the specific embodiment, the reaction apparatus of the present invention may be a dual barrier dielectric apparatus.

(80) In FIGS. 1a, 1b, 1c, 2a, 2b, 2c, 3a, 3b, 3c, 4a, 4b, and 4c, the following preferable technical features are also provided:

(81) the reaction apparatus preferably further comprises a ground lead 5, one end of the ground lead 5 is electrically connected with the inner electrode 3 or the outer electrode 4.

(82) In the present invention, one of the inner electrode 3 and the outer electrode 4 is a grounding electrode, and the other is a high-voltage electrode.

(83) Preferably, the first inlet 11 is disposed at an upper portion of the first cavity 1, and the first outlet is disposed at a lower portion and/or a bottom of the first cavity 1.

(84) Preferably, the second inlet 21 and the second outlet 22 are respectively arranged at a lower portion and an upper portion of the second cavity 2.

(85) It is preferable that the third inlet 71 and the third outlet 72 are respectively arranged at a lower portion and an upper portion of the third cavity 7.

(86) Preferably, in the specific embodiments shown in FIGS. 1a, 1b, 1c, 2a, 2b, 2c, 3a, 3b and 3c, the first outlet comprises a gas product outlet 12 and a liquid product outlet 13, and the gas product outlet 12 is disposed at the lower part of the first cavity 1 and the liquid product outlet 13 is disposed at the bottom of the first cavity 1.

(87) Preferably, in the specific embodiments shown in FIGS. 1a, 1b, 1c, 2a, 2b, 2c, 3a, 3b and 3c, the gas product outlet 12 is disposed below the discharge region, and the proportional relationship between the height H.sub.1 of the disposed position of said gas product outlet 12 relative to the bottom of the first cavity 1 and the length L.sub.3 of the discharge region is: H.sub.1:L.sub.3=1:(0.05˜25,000); preferably H.sub.1:L.sub.3=1:(0.1˜10,000); more preferably H.sub.1:L.sub.3=1:(0.5˜1,000).

(88) Preferably, in the specific embodiments shown in FIGS. 4a, 4b and 4c, the first outlet comprises a gas product outlet 12 and a liquid product outlet 13, and the gas product outlet 12 is arranged at the lower part of all the reaction tubes, and the liquid product outlet 13 is arranged at the bottom of all the reaction tubes. It is preferable that each of the reaction tubes has the same size

(89) Preferably, in the specific embodiments shown in FIGS. 4a, 4b and 4c, the gas product outlet 12 is disposed below all the discharge region, and the proportional relationship between the height H.sub.1 of the disposed position of said gas product outlet 12 relative to the bottom of the first cavity 1 and the length L.sub.3 of the discharge region is: H.sub.1:L.sub.3=1:(0.05˜25,000); preferably H.sub.1:L.sub.3=1:(0.1˜10,000); more preferably H.sub.1:L.sub.3=1:(0.5˜1,000).

(90) Unless otherwise specified, the pressures in the present invention refer to the absolute pressures.

(91) The low-temperature plasma reaction apparatus provided by the invention also have the following specific advantages:

(92) (1) The reaction apparatus uses a conductive solid material to form the ground lead for grounding, as compared with a liquid grounding electrode, the solid grounding electrode has the advantages that the micro-discharge current generated by discharge is larger when the solid grounding electrode is matched with the structure of the invention, thereby being more conducive to the discharge decomposition reaction of hydrogen sulfide molecules.
(2) The jacket structure is arranged on the outer side and/or the inner side of the electrode of the reaction apparatus, the temperature control of the reaction apparatus may be implemented by controlling the temperature of the heat-conducting medium in the jacket, such that the sulphur generated by the decomposition of hydrogen sulfide discharge can smoothly flow out from the discharge region, the sulphur is prevented from being solidified to block the reaction apparatus, and the discharge process is carried out continuously and stably.
(3) The reaction apparatus controls the proportional relation between L.sub.2 and the thickness D.sub.1 of the barrier dielectric to be (0.1˜100):1, preferably (0.1˜30):1, more preferably (0.2˜15):1, which is in combination with the other structure of the reaction apparatus in the invention, thus the conversion of the hydrogen sulfide can be obviously improved and the decomposition energy consumption can be reduced.

(93) The present invention will be described in detail by means of the examples. In the following examples, each of the used raw materials is commercially available unless otherwise specified.

(94) The thickness of the barrier dielectrics in the following examples and comparative examples is identical.

(95) The conversion of hydrogen sulfide in the following examples are obtained through calculation according to the following formula:
Conversion of hydrogen sulfide %=mole number of the converted hydrogen sulfide/mole number of initial hydrogen sulfide×100%.

(96) The energy consumption for decomposing hydrogen sulfide in the following examples is measured through detection with an oscilloscope and calculation by using the Lissajous figure.

Example 1

(97) The low-temperature plasma reaction apparatus illustrated in FIG. 1a is used for performing the hydrogen sulfide decomposition reaction, the specific structure and structural parameters of the low-temperature plasma reaction apparatus are shown as follows, the inner electrode in the example is exactly the high-voltage electrode.

(98) The reaction apparatus comprises:

(99) A first cavity 1 provided with a first inlet 11, a gas product outlet 12 and a liquid product outlet 13, respectively, wherein all the sidewall of the first cavity 1 is formed by the barrier dielectric 6, the material forming the barrier dielectric 6 is a hard glass;
a second cavity 2 is nested outside the first cavity 1, and a second inlet 21 and a second outlet 22 are respectively arranged on the second cavity 2;
an inner electrode 3 arranged at the central axis position of the first cavity 1, the material forming the inner electrode 3 is stainless steel, and the inner electrode 3 is connected with a high-voltage power supply;
an outer electrode 4 wrapped on the outer sidewall of the first cavity 1, the material forming the outer electrode 4 is stainless steel metal foil, the outer electrode 4 is grounded, and a lower edge of the inner electrode 3 in the example is lower than that of the outer electrode 4;
the ratio of L.sub.2 to the thickness D.sub.1 of the barrier dielectric 6 is 6:1; and H.sub.1:L.sub.3=1:46;
the volume of the first cavity 1 of the reaction apparatus in the example is 0.2 L.

(100) In the example, the mixed gas enters the first cavity 1 of the reaction apparatus from the upper part of the first cavity 1 of the reaction apparatus, a gas product is discharged via a gas product outlet 12 disposed at the lower part of the first cavity 1 of the reaction apparatus, and elemental sulphur is discharged from a liquid product outlet 13 disposed at the bottom of the reaction apparatus; and the heat-conducting medium of the example is introduced from the lower portion of the second cavity 2 of the reaction apparatus and is discharged from the upper portion of the second cavity 2 of the reaction apparatus.

(101) The operation steps of the low-temperature plasma reaction apparatus are as follows: introducing nitrogen into the first cavity 1 of the low-temperature plasma reaction apparatus from the first inlet 11 to purge air in the discharge region, and discharging the gas via the gas product outlet 12 and the liquid product outlet 13; in the meanwhile, introducing a heat-conducting medium (particularly dimethyl silicone oil) into the second cavity 2 from the second inlet 21, discharging the introduced heat-conducting medium via the second outlet 22, and maintaining the temperature of the heat-conducting medium at 145° C.;

(102) subsequently introducing a H.sub.2S/Ar mixed gas into the first cavity 1 of the low-temperature plasma reaction apparatus from the first inlet 11, wherein the volume fraction of H.sub.2S is 20%; controlling the flow rate of the mixed gas such that the average residence time of the gas in the discharge region is 9.5 s, and the reaction pressure in the first cavity 1 of the reactor in the example is kept at 0.03 MPa. After introducing the H.sub.2S/Ar mixed gas into the reaction apparatus for 30 minutes, switching on an alternating current (AC) high-voltage power supply, and forming a plasma discharge field between the inner electrode 3 and the solid grounding electrode by adjusting the voltage and frequency of the high-voltage power supply. Wherein the discharge conditions are as follows: the voltage is 16.8 kV, the frequency is 7.5 kHz, and the current is 0.75 A. The hydrogen sulfide gas is ionized in the discharge region and decomposed into hydrogen and elemental sulphur, the elemental sulphur generated by discharge flows down slowly along the first cavity wall, and liquid products are discharged intermittently. The reacted gas flows out from a gas product outlet 12.

(103) Results: the conversion of H.sub.2S is measured to be 73.9% after continuously performing the hydrogen sulfide decomposition reaction of this example for 20 minutes; and no abnormality has been discovered after performing the continuous discharge for 100 hours, both the discharge condition and the H.sub.2S conversion are kept stable. In addition, the decomposition energy consumption of the example is 13 eV/H.sub.2S molecules (the energy consumed by decomposition of 1 molecule of H.sub.2S is 13 eV).

Comparative Example 1

(104) The comparative example employs a low-temperature plasma reaction apparatus similar to that of example 1 to carry out a hydrogen sulfide decomposition reaction, except for the following aspects:

(105) the grounding electrode in the comparative example is a liquid grounding electrode, which is a mixture of LiCl and AlCl.sub.3 in a molten state in a molar ratio of 1:1, the liquid grounding electrode is also a heat-conducting medium, it is maintained at a temperature of 145° C., and placed in the second cavity of the reaction apparatus;
the flow rate of the mixture is controlled such that the average residence time of the gas in the discharge region is 18.5 s;
the volume of the first cavity of the reaction apparatus of the comparative example is 0.05 L.

(106) The rest parts of the comparative example are same as those in the example 1.

(107) Moreover, the comparative example uses the same operation method as in example 1 for performing the decomposition reaction of hydrogen sulfide.

(108) Results: the conversion of H.sub.2S is measured to be 15.6% after continuously performing the hydrogen sulfide decomposition reaction of the comparative example for 20 minutes; and the conversion of H.sub.2S is reduced to 5.1% after the continuous discharge for 1.5 hours.

(109) The decomposition energy consumption of the comparative example is 102 eV/H.sub.2S molecules.

Comparative Example 2

(110) The comparative example employs a low-temperature plasma reaction apparatus similar to that of the comparative example 1 to carry out a hydrogen sulfide decomposition reaction, except for the following aspects:

(111) the ratio of L.sub.2 to the thickness D.sub.1 of the barrier dielectric in the comparative example is 0.08:1;

(112) the flow rate of the mixture is controlled such that the average residence time of the gas in the discharge region is 7.3 s;

(113) the volume of the first cavity of the comparative example is 0.02 L.

(114) The rest parts of the comparative example are same as those in the comparative example 1.

(115) Results: the conversion of H.sub.2S is measured to be 17.1% after continuously performing the hydrogen sulfide decomposition reaction of the comparative example for 20 minutes; and the conversion of H.sub.2S is reduced to 3.9% after the continuous discharge for 1.5 hours.

(116) The decomposition energy consumption of the comparative example is 125 eV/H.sub.2S molecules.

Example 2

(117) The example uses a plasma reaction apparatus similar to that of example 1 to carry out the decomposition reaction of hydrogen sulfide, except for that in this example:

(118) all sidewalls of the first cavity 1 are formed by outer electrode 4, the material forming the outer electrode 4 is stainless steel metal foil, the outer electrode 4 is grounded, and the inner electrode 3 is connected with a high-voltage power supply;

(119) the barrier dielectric 6 is disposed on the inner sidewall of the first cavity 1 in a surrounding manner;

(120) the ratio of L.sub.2 to the thickness D.sub.1 of the barrier dielectric 6 is 20:1; and H.sub.1:L.sub.3=1:100.

(121) In the example, a H.sub.2S/Ar mixed gas is introduced into a first cavity 1 of the low-temperature plasma reaction apparatus from a first inlet 11, wherein the volume fraction of H.sub.2S is 30%, the flow rate of the mixed gas is controlled such that the average residence time of the gas in a discharge region is 7.8 s, and the reaction pressure in the first cavity 1 of the reactor in the example is kept at 0.04 MPa. After introducing the H.sub.2S/Ar mixed gas into the reaction apparatus for 30 minutes, an AC high-voltage power supply is switched on, and a plasma discharge field is formed between the inner electrode 3 and the solid grounding electrode by adjusting the voltage and frequency of the high-voltage power supply. Wherein the discharge conditions are as follows: the voltage is 19.8 kV, the frequency is 10.5 kHz, and the current is 1.25 A.

(122) The rest parts of the example are same as those in the example 1.

(123) Results: the conversion of H.sub.2S is measured to be 72.8% after continuously performing the hydrogen sulfide decomposition reaction of the example for 20 minutes; and no abnormality has been discovered after performing the continuous discharge for 100 hours, both the discharge condition and the H.sub.2S conversion are kept stable. In addition, the decomposition energy consumption of the example is 14.2 eV/H.sub.2S molecules.

Example 3

(124) The example uses a plasma reaction apparatus similar to that of example 1 to carry out the decomposition reaction of hydrogen sulfide, except for that in this example:

(125) all sidewalls of the first cavity 1 are formed by outer electrode 4, the material forming the outer electrodes 4 is copper foil, the outer electrode 4 is grounded, and the inner electrode 3 is connected with a high-voltage power supply;

(126) the barrier dielectric 6 is disposed on the inner sidewall of the first cavity 1 in a surrounding manner;

(127) the ratio of L.sub.2 to the thickness D.sub.1 of the barrier dielectric 6 is 0.5:1; and H.sub.1:L.sub.3=1:200.

(128) In the example, a H.sub.2S/Ar mixed gas is introduced into a first cavity 1 of the low-temperature plasma reaction apparatus from a first inlet 11, wherein the volume fraction of H.sub.2S is 25%, the flow rate of the mixed gas is controlled such that the average residence time of the gas in a discharge region is 10.3 s, and the reaction pressure in the first cavity 1 of the reactor in the example is kept at 0.05 MPa. After introducing the H.sub.2S/Ar mixed gas into the reaction apparatus for 30 minutes, an AC high-voltage power supply is switched on, and a plasma discharge field is formed between the inner electrode 3 and the solid grounding electrode by adjusting the voltage and frequency of the high-voltage power supply. Wherein the discharge conditions are as follows: the voltage is 12.8 kV, the frequency is 4.7 kHz, and the current is 1.12 A.

(129) The rest parts of the example are same as those in the example 1.

(130) Results: the conversion of H.sub.2S is measured to be 73.2% after continuously performing the hydrogen sulfide decomposition reaction of the example for 20 minutes; and no abnormality has been discovered after performing the continuous discharge for 100 hours, both the discharge condition and the H.sub.2S conversion are kept stable. In addition, the decomposition energy consumption of the example is 14.8 eV/H.sub.2S molecules.

Example 4

(131) This example uses a plasma reaction apparatus similar to that of example 1 to carry out the decomposition reaction of hydrogen sulfide, except for that in this example: the ratio of L.sub.2 to the thickness D.sub.1 of the barrier dielectric 6 is 35:1.

(132) The rest parts of the example are same as those in the example 1.

(133) Results: the conversion of H.sub.2S is measured to be 71.6% after continuously performing the hydrogen sulfide decomposition reaction of the example for 20 minutes; and no abnormality has been discovered after performing the continuous discharge for 100 hours, both the discharge condition and the H.sub.2S conversion are kept stable. In addition, the decomposition energy consumption of the example is 22.3 eV/H.sub.2S molecules.

Example 5

(134) The plasma reaction apparatus illustrated in FIG. 2a is used for performing hydrogen sulfide decomposition reaction, and the specific structure and structural parameters of the plasma reaction apparatus are shown as follows:

(135) the reaction apparatus comprises:

(136) a first cavity 1 provided with a first inlet 11, a gas product outlet 12 and a liquid product outlet 13, respectively;

(137) a second cavity 2 nested outside the first cavity 1, and a second inlet 21 and a second outlet 22 are respectively arranged on the second cavity 2;

(138) an inner electrode 3 arranged at the central axis position of the first cavity 1, the material forming the inner electrode 3 is stainless steel, and the inner electrode 3 is connected with a high-voltage power supply;

(139) an outer electrode 4 disposed on an inner sidewall of the first cavity 1, the material forming the outer electrode 4 is stainless steel metal foil, the outer electrode 4 is grounded, and a lower edge of the inner electrode 3 in the example is lower than a lower edge of the solid grounding electrode;
a barrier dielectric 6 arranged on the outer surface of the inner electrode 3 and the part of inner electrode 3 which extending into the first cavity 1 is covered by barrier dielectric 6, the upper edge of the barrier dielectric 6 is higher than that of the solid grounding electrode, and the material forming the barrier dielectric 6 is hard glass.
The ratio of L.sub.2 to the thickness D.sub.1 of the barrier dielectric 6 is 8:1; and H.sub.1:L.sub.3=1:40;
the volume of the first cavity 1 of the reaction apparatus in the example is 0.2 L.

(140) In the example, the mixed gas enters the first cavity 1 of the reaction apparatus from the upper part of the first cavity 1 of the reaction apparatus, a gas product is discharged via a gas product outlet 12 disposed at the lower part of the first cavity 1 of the reaction apparatus, and elemental sulphur is discharged from a liquid product outlet 13 disposed at the bottom of the reaction apparatus; and the heat-conducting medium of the present embodiment is introduced from the lower portion of the second cavity 2 of the reaction apparatus and is discharged from the upper portion of the second cavity 2 of the reaction apparatus.

(141) The operation steps of the plasma reaction apparatus are as follows:

(142) introducing nitrogen into the first cavity 1 of the low-temperature plasma reaction apparatus from the first inlet 11 to purge air in the discharge region, and discharging the gas via the gas product outlet 12 and the liquid product outlet 13; in the meanwhile, introducing a heat-conducting medium (particularly dimethyl silicone oil) into the second cavity 2 from the second inlet 21, discharging the introduced heat-conducting medium via the second outlet 22, and maintaining the temperature of the heat-conducting medium at 145° C.

(143) Subsequently introducing a H.sub.2S/Ar mixed gas into the first cavity 1 of the low-temperature plasma reaction apparatus from the first inlet 11, wherein the volume fraction of H.sub.2S is 20%; controlling the flow rate of the mixed gas such that the average residence time of the gas in the discharge region is 9.2 s, and the reaction pressure in the first cavity 1 of the reactor in the example is kept at 0.03 MPa. After introducing the H.sub.2S/Ar mixed gas into the reaction apparatus for 30 minutes, switching on the AC high-voltage power supply, and forming a plasma discharge field between the inner electrode 3 and the solid grounding electrode by adjusting the voltage and frequency of the high-voltage power supply. Wherein the discharge conditions are as follows: the voltage is 18.5 kV, the frequency is 1.5 kHz, and the current is 1.05 A. The hydrogen sulfide gas is ionized in the discharge region and decomposed into hydrogen and elemental sulphur, the elemental sulphur generated by discharge flows down slowly along the first cavity wall and flows out from the liquid product outlet 13. The reacted gas flows out from a gas product outlet 12.

(144) Results: the conversion of H.sub.2S is measured to be 74.2% after continuously performing the hydrogen sulfide decomposition reaction of this example for 20 minutes; and no abnormality has been discovered after performing the continuous discharge for 100 hours, both the discharge condition and the H.sub.2S conversion are kept stable. In addition, the decomposition energy consumption of the example is 12.5 eV/H.sub.2S molecules (the energy consumed by decomposition of 1 molecule of H.sub.2S is 12.5 eV).

Comparative Example 3

(145) This comparative example employs a plasma reaction apparatus similar to that of example 5 to carry out a hydrogen sulfide decomposition reaction, except for the following aspects:

(146) the grounding electrode in the comparative example is a liquid grounding electrode, which is a mixture of LiCl and AlCl.sub.3 in a molten state in a molar ratio of 1:1, the liquid grounding electrode is also a heat-conducting medium, it is maintained at a temperature of 145° C., and placed in the second cavity of the reaction apparatus;
the flow rate of the mixture is controlled such that the average residence time of the gas in the discharge region is 20.1 s;
the volume of the first cavity of the reaction apparatus of the comparative example is 0.05 L.

(147) The rest parts of the comparative example are same as those in the example 5.

(148) Moreover, the comparative example uses the same operation method as in example 5 for performing the decomposition reaction of hydrogen sulfide.

(149) Results: the conversion of H.sub.2S is measured to be 16.0% after continuously performing the hydrogen sulfide decomposition reaction of the comparative example for 20 minutes; and the conversion of H.sub.2S is reduced to 6.3% after the continuous discharge for 1.5 hours.

(150) The decomposition energy consumption of this comparative example is 105 eV/H.sub.2S molecules.

Comparative Example 4

(151) The comparative example employs a plasma reaction apparatus similar to that of the comparative example 3 to carry out a hydrogen sulfide decomposition reaction, except for the following aspects:

(152) the ratio of L.sub.2 to the thickness D.sub.1 of the barrier dielectric in the comparative example is 0.08:1;

(153) the flow rate of the mixture is controlled such that the average residence time of the gas in the discharge region is 17.3 s;

(154) the volume of the first cavity of the comparative example is 0.02 L.

(155) The rest parts of the comparative example are same as those in the comparative example 3.

(156) Results: the conversion of H.sub.2S is measured to be 19.5% after continuously performing the hydrogen sulfide decomposition reaction of the comparative example for 20 minutes; and the conversion of H.sub.2S is reduced to 4.7% after the continuous discharge for 1.5 hours.

(157) The decomposition energy consumption of the comparative example is 135 eV/H.sub.2S molecules.

Example 6

(158) The example uses a plasma reaction apparatus similar to that of example 5 to carry out the decomposition reaction of hydrogen sulfide, except for that in this example:

(159) all sidewall of the first cavity 1 is formed by outer electrode 4, the material forming the outer electrode 4 is stainless steel metal foil, the outer electrode 4 is grounded, and the inner electrode 3 is connected with a high-voltage power supply;

(160) the ratio of L.sub.2 to the thickness D.sub.1 of the barrier dielectric 6 is 25:1; and H.sub.1:L.sub.3=1:120.

(161) In the example, a H.sub.2S/Ar mixed gas is introduced into a first cavity 1 of the plasma reaction apparatus from a first inlet 11, wherein the volume fraction of H.sub.2S is 30%, the flow rate of the mixed gas is controlled such that the average residence time of the gas in a discharge region is 8.5 s, and the reaction pressure in the first cavity 1 of the reactor in the example is kept at 0.04 MPa. After introducing the H.sub.2S/Ar mixed gas into the reaction apparatus for 30 minutes, an AC high-voltage power supply is switched on, and a plasma discharge field is formed between the inner electrode 3 and the solid grounding electrode by adjusting the voltage and frequency of the high-voltage power supply. Wherein the discharge conditions are as follows: the voltage is 19.5 kV, the frequency is 5.5 kHz, and the current is 1.45 A.

(162) The rest parts of the example are same as those in the example 5.

(163) Results: the conversion of H.sub.2S is measured to be 73.5% after continuously performing the hydrogen sulfide decomposition reaction of the example for 20 minutes; and no abnormality has been discovered after performing the continuous discharge for 100 hours, both the discharge condition and the H.sub.2S conversion are kept stable. In addition, the decomposition energy consumption of the example is 13.2 eV/H.sub.2S molecules.

Example 7

(164) The example uses a plasma reaction apparatus similar to that of example 5 to carry out the decomposition reaction of hydrogen sulfide, except for that in this example:

(165) The outer electrode 4 is arranged on the inner sidewall of the first cavity 1, the material forming the outer electrode 4 is copper foil, the outer electrode 4 is grounded, and the inner electrode 3 is connected with a high-voltage power supply;

(166) the barrier dielectric 6 is arranged on the outer surface of the inner electrode 3 and part of inner electrode 3 which extending into the first cavity 1 is covered by barrier dielectric 6, the upper edge of the barrier dielectric 6 is higher than that of the outer electrode 4, and the material forming the barrier dielectric 6 is ceramic;
the ratio of L.sub.2 to the thickness D.sub.1 of the barrier dielectric 6 is 0.7:1; and H.sub.1:L.sub.2=1:250.

(167) In the example, a H.sub.2S/Ar mixed gas is introduced into a first cavity 1 of the low-temperature plasma reaction apparatus from a first inlet 11, wherein the volume fraction of H.sub.2S is 25%, the flow rate of the mixed gas is controlled such that the average residence time of the gas in a discharge region is 12.5 s, and the reaction pressure in the first cavity 1 of the reactor in the example is kept at 0.05 MPa. After introducing the H.sub.2S/Ar mixed gas into the reaction apparatus for 30 minutes, an AC high-voltage power supply is switched on, and a plasma discharge field is formed between the inner electrode 3 and the solid grounding electrode by adjusting the voltage and frequency of the high-voltage power supply. Wherein the discharge conditions are as follows: the voltage is 8.5 kV, the frequency is 2.5 kHz, and the current is 1.08 A.

(168) The rest parts of the example are same as those in the example 5.

(169) Results: the conversion of H.sub.2S is measured to be 73.8% after continuously performing the hydrogen sulfide decomposition reaction of the example for 20 minutes; and no abnormality has been discovered after performing the continuous discharge for 100 hours, both the discharge condition and the H.sub.2S conversion are kept stable. In addition, the decomposition energy consumption of the example is 13.8 eV/H.sub.2S molecules.

Example 8

(170) This example uses a plasma reaction apparatus similar to that of example 5 to carry out the decomposition reaction of hydrogen sulfide, except for that in this example: the ratio of L.sub.2 to the thickness D.sub.1 of the barrier dielectric 6 is 35:1.

(171) The rest parts of the example are same as those in the example 5.

(172) Results: the conversion of H.sub.2S is measured to be 71.0% after continuously performing the hydrogen sulfide decomposition reaction of the example for 20 minutes; and no abnormality has been discovered after performing the continuous discharge for 100 hours, both the discharge condition and the H.sub.2S conversion are kept stable. In addition, the decomposition energy consumption of the example is 23.8 eV/H.sub.2S molecules.

Example 9

(173) The low-temperature plasma reaction apparatus illustrated in FIG. 3a is used for performing hydrogen sulfide decomposition reaction, and the specific structure and structural parameters of the low-temperature plasma reaction apparatus are shown as follows:

(174) the reaction apparatus comprises:

(175) a first cavity 1 provided with a first inlet 11, a gas product outlet 12 and a liquid product outlet 13, respectively, wherein the sidewall of the first cavity 1 is formed by an outer electrode 4, the material forming the outer electrode 4 is stainless steel metal foil, and the outer electrode 4 is grounded;
a second cavity 2 nested outside the first cavity 1, and a second inlet 21 and a second outlet 22 are respectively arranged on the second cavity 2;
an inner electrode 3 arranged at the central axis position of the first cavity 1, the material forming the inner electrode 3 is stainless steel, and the inner electrode 3 is connected with a high-voltage power supply;
the lower edge of the inner electrode 3 in this example is lower than the lower edge of the solid grounding electrode;
a barrier dielectric 6, the material forming the barrier dielectric 6 is hard glass;
the ratio of L.sub.2 to the thickness D.sub.1 of the barrier dielectric 6 is 6:1; and H.sub.1:L.sub.3=1:46;
the volume of the first cavity 1 of the reaction apparatus in the example is 0.2 L.

(176) In the example, the mixed gas enters the first cavity 1 of the reaction apparatus from the upper part of the first cavity of the reaction apparatus, a gas product is discharged via a gas product outlet 12 disposed at the lower part of the first cavity 1 of the reaction apparatus, and elemental sulphur is discharged from a liquid product outlet 13 disposed at the bottom of the reaction apparatus; and the heat-conducting medium of the present embodiment is introduced from the lower portion of the second cavity 2 of the reaction apparatus and is discharged from the upper portion of the second cavity 2 of the reaction apparatus.

(177) The operation steps of the low-temperature plasma reaction apparatus are as follows: introducing nitrogen into the first cavity 1 of the low-temperature plasma reaction apparatus from the first inlet 11 to purge air in the discharge region, and discharging the gas via the gas product outlet 12 and the liquid product outlet 13; in the meanwhile, introducing a heat-conducting medium (particularly dimethyl silicone oil) into the second cavity 2 from the second inlet 21, discharging the introduced heat-conducting medium via the second outlet 22, and maintaining the temperature of the heat-conducting medium at 145° C.

(178) Subsequently introducing a H.sub.2S/Ar mixed gas into the first cavity 1 of the low-temperature plasma reaction apparatus from the first inlet 11, wherein the volume fraction of H.sub.2S is 20%; controlling the flow rate of the mixed gas such that the average residence time of the gas in the discharge region is 11.2 s, and the reaction pressure in the first cavity 1 of the reactor in the example is kept at 0.03 MPa. After introducing the H.sub.2S/Ar mixed gas into the reaction apparatus for 30 minutes, switching on the AC high-voltage power supply, and forming a plasma discharge field between the inner electrode 3 and the solid grounding electrode by adjusting the voltage and frequency of the high-voltage power supply. Wherein the discharge conditions are as follows: the voltage is 17.2 kV, the frequency is 8.5 kHz, and the current is 0.80 A. The hydrogen sulfide gas is ionized in the discharge region and decomposed into hydrogen and elemental sulphur, the elemental sulphur generated by discharge flows down slowly along the first cavity wall and flows out intermittently from the liquid product outlet 13. The reacted gas flows out from a gas product outlet 12.

(179) Results: the conversion of H.sub.2S is measured to be 74.1% after continuously performing the hydrogen sulfide decomposition reaction of this example for 20 minutes; and no abnormality has been discovered after performing the continuous discharge for 100 hours, both the discharge condition and the H.sub.2S conversion are kept stable. In addition, the decomposition energy consumption of the example is 13.2 eV/H.sub.2S molecules (the energy consumed by decomposition of 1 molecule of H.sub.2S is 13.2 eV).

Comparative Example 5

(180) This comparative example employs a low-temperature plasma reaction apparatus similar to that of example 9 to carry out the hydrogen sulfide decomposition reaction, except for the following aspects:

(181) the grounding electrode in the comparative example is a liquid grounding electrode, which is a mixture of LiCl and AlCl.sub.3 in a molten state in a molar ratio of 1:1, the liquid grounding electrode is also a heat-conducting medium, it is maintained at a temperature of 145° C., and placed in the second cavity of the reaction apparatus;
the flow rate of the mixture is controlled such that the average residence time of the gas in the discharge region is 18.5 s;
the volume of the first cavity of the reaction apparatus of this comparative example is 0.05 L.

(182) The rest parts of the comparative example are same as those in the example 9.

(183) Moreover, the comparative example uses the same operation method as in example 9 for performing the decomposition reaction of hydrogen sulfide.

(184) Results: the conversion of H.sub.2S is measured to be 15.4% after continuously performing the hydrogen sulfide decomposition reaction of the comparative example for 20 minutes; and the conversion of H.sub.2S is reduced to 5.0% after the continuous discharge for 1.5 hours.

(185) The decomposition energy consumption of this comparative example is 104 eV/H.sub.2S molecules.

Comparative Example 6

(186) The comparative example employs a low-temperature plasma reaction apparatus similar to that of the comparative example 5 to carry out a hydrogen sulfide decomposition reaction, except for the following aspects:

(187) the ratio of L.sub.2 to the thickness D.sub.1 of the barrier dielectric in the comparative example is 0.08:1;

(188) the flow rate of the mixture is controlled such that the average residence time of the gas in the discharge region is 16.9 s;

(189) the volume of the first cavity of the present comparative example is 0.02 L.

(190) The rest parts of the comparative example are same as those in the comparative example 5.

(191) Results: the conversion of H.sub.2S is measured to be 19.4% after continuously performing the hydrogen sulfide decomposition reaction of the comparative example for 20 minutes; and the conversion of H.sub.2S is reduced to 5.1% after the continuous discharge for 1.5 hours.

(192) The decomposition energy consumption of the comparative example is 147 eV/H.sub.2S molecules.

Example 10

(193) The example uses a plasma reaction apparatus similar to that of example 9 to carry out the decomposition reaction of hydrogen sulfide, except for that in this example:

(194) the outer electrode 4 is arranged on the inner sidewall of the first cavity 1, the material forming the outer electrode 4 is stainless steel metal foil, the outer electrode 4 is grounded, and the inner electrode 3 is connected with a high-voltage power supply;
the ratio of L.sub.2 to the thickness D.sub.1 of the barrier dielectric 6 is 20:1; and H.sub.1:L.sub.3=1:300.

(195) In the example, a H.sub.2S/Ar mixed gas is introduced into a first cavity 1 of the plasma reaction apparatus from a first inlet 11, wherein the volume fraction of H.sub.2S is 30%, the flow rate of the mixed gas is controlled such that the average residence time of the gas in a discharge region is 9.6 s, and the reaction pressure in the first cavity 1 of the reactor in the example is kept at 0.04 MPa. After introducing the H.sub.2S/Ar mixed gas into the reaction apparatus for 30 minutes, an AC high-voltage power supply is switched on, and a plasma discharge field is formed between the inner electrode 3 and the solid grounding electrode by adjusting the voltage and frequency of the high-voltage power supply. Wherein the discharge conditions are as follows: the voltage is 18.5 kV, the frequency is 10.5 kHz, and the current is 1.05 A.

(196) The rest parts of the example are same as those in the example 9.

(197) Results: the conversion of H.sub.2S is measured to be 73.4% after continuously performing the hydrogen sulfide decomposition reaction of the example for 20 minutes; and no abnormality has been discovered after performing the continuous discharge for 100 hours, both the discharge condition and the H.sub.2S conversion are kept stable. In addition, the decomposition energy consumption of the example is 14.1 eV/H.sub.2S molecules.

Example 11

(198) The low-temperature plasma reaction apparatus illustrated in FIG. 4a is used for performing hydrogen sulfide decomposition reaction, and the specific structure and structural parameters of the low-temperature plasma reaction apparatus are shown as follows:

(199) the reaction apparatus comprises:

(200) a first cavity 1 provided with a reactor inlet 11, a gas product outlet 12 and a liquid product outlet 13, respectively, four reaction tubes are arranged in parallel in the first cavity 1, the top and the bottom of each reaction tube are respectively communicated correspondingly, such that the raw materials feeding from the reactor inlet can enter into each reaction tube respectively, the gaseous products generated in each reaction tube can be discharged via the gas product outlet 12, and the liquid products generated in each reaction tube can be discharged via the liquid product outlet 13, the four reaction tubes are completely identical in size, all sidewalls of the reaction tubes are formed by barrier dielectric 6, and the material forming the barrier dielectric 6 is hard glass;
a second cavity 2 nested outside the first cavity 1, a second inlet 21 and a second outlet 22 are respectively arranged on the second cavity 2, the heat-conducting medium introduced from the second inlet 21 can be distributed among the reaction tubes of the first cavity 1, and the heat-conducting medium is discharged via the second outlet 22;
inner electrodes 3 respectively arranged at the central axis positions of the reaction tubes, the material forming the inner electrodes 3 is stainless steel, the inner electrodes 3 in the reaction tubes are connected in parallel, and the inner electrodes 3 are connected with a high-voltage power supply;
outer electrodes 4 respectively arranged on the outer sidewalls of the reaction tubes in a surrounding manner, the material forming the outer electrodes 4 is stainless steel metal foil, the outer electrodes 4 are grounded, and the lower edges of the inner electrodes 3 in the example are flush with the lower edges of the outer electrodes 4.
The ratio of L.sub.2 to the thickness D.sub.1 of the barrier dielectric 6 is 8:1; and H.sub.1:L.sub.3=1:32;
The volume of the first cavity 1 of the entire reactor in this example is 1 L.

(201) In the embodiment, the mixed gas enters the first cavity 1 of the reactor from the upper part of the first cavity 1 of the reactor, a gas product is discharged via a gas product outlet 12 disposed at the lower part of the first cavity 1 of the reactor, and elemental sulphur is discharged from a liquid product outlet 13 disposed at the bottom of the reactor; and the heat-conducting medium of the present embodiment is introduced from the lower portion of the second cavity 2 of the reactor and is discharged from the upper portion of the second cavity 2 of the reactor.

(202) Operation Steps:

(203) introducing nitrogen into the first cavity 1 of the high-flux low-temperature plasma reactor from the reactor inlet to purge air in the discharge region, and discharging the gas from the gas product outlet 12 and the liquid product outlet 13; in the meanwhile, introducing a heat-conducting medium (particularly dimethyl silicone oil) into the second cavity 2 from the second inlet 21, discharging the introduced heat-conducting medium via the second outlet 22, and maintaining the temperature of the heat-conducting medium at 145° C.;
subsequently introducing a H.sub.2S/Ar mixed gas into the first cavity 1 of the high-flux low-temperature plasma reactor from the reactor inlet, wherein the volume fraction of H.sub.2S is 65%; controlling the flow rate of the mixed gas such that the average residence time of the gas in the discharge region is 9.7 s, and the reaction pressure in the first cavity 1 of the reactor in the example is kept at 0.15 MPa. After introducing the H.sub.2S/Ar mixed gas into the reactor for 30 minutes, switching on an AC high-voltage power supply, and forming a plasma discharge field between the inner electrode 3 and the solid grounding electrode by adjusting the voltage and the frequency of the high-voltage power supply. Wherein the discharge conditions are as follows: the voltage is 13.8 kV, the frequency is 0.8 kHz, and the current is 2.2 A. The hydrogen sulfide gas is ionized in the discharge region and decomposed into hydrogen and elemental sulphur, the elemental sulphur generated by discharge flows down slowly along the first cavity wall and flows out from the liquid product outlet 13. The reacted gas flows out from a gas product outlet 12.

(204) Results: the conversion of H.sub.2S is measured to be 73.6% after continuously performing the hydrogen sulfide decomposition reaction of this example for 20 minutes; and no abnormality has been discovered after performing the continuous discharge for 100 hours, both the discharge condition and the H.sub.2S conversion are kept stable. In addition, the decomposition energy consumption of the example is 14.2 eV/H.sub.2S molecules (the energy consumed by decomposition of 1 molecule of H.sub.2S is 14.2 eV).

Comparative Example 7

(205) This comparative example employs a low-temperature plasma reaction apparatus similar to that of example 11 for the hydrogen sulfide decomposition reaction, except for the following aspects:

(206) the grounding electrode in the comparative example is a liquid grounding electrode, which is a mixture of LiCl and AlCl.sub.3 in a molten state in a molar ratio of 1:1, the liquid grounding electrode is also a heat-conducting medium, it is maintained at a temperature of 145° C., and placed in the second cavity of the reaction apparatus;
the flow rate of the mixture is controlled such that the average residence time of the gas in the discharge region is 20.5 s;
the volume of the first cavity of the reaction apparatus of this comparative example is 0.05 L.

(207) The rest parts of the comparative example are same as those in the example 11.

(208) Moreover, the comparative example uses the same operation method as in example 11 for performing the decomposition reaction of hydrogen sulfide.

(209) Results: the conversion of H.sub.2S is measured to be 14.9% after continuously performing the hydrogen sulfide decomposition reaction of the comparative example for 20 minutes; and the conversion of H.sub.2S is reduced to 6.9% after the continuous discharge for 1.5 hours.

(210) The decomposition energy consumption of this comparative example is 111 eV/H.sub.2S molecules.

Comparative Example 8

(211) The comparative example employs a low-temperature plasma reaction apparatus similar to that of the comparative example 7 to carry out a hydrogen sulfide decomposition reaction, except for the following aspects:

(212) the ratio of L.sub.2 to the thickness D.sub.1 of the barrier dielectric in the comparative example is 0.08:1;

(213) the flow rate of the mixture is controlled such that the average residence time of the gas in the discharge region is 18.4 s;

(214) the volume of the first cavity of the present comparative example is 0.02 L.

(215) The rest parts of the comparative example are same as those in the comparative example 7.

(216) Results: the conversion of H.sub.2S is measured to be 21.7% after continuously performing the hydrogen sulfide decomposition reaction of the comparative example for 20 minutes; and the conversion of H.sub.2S is reduced to 7.8% after the continuous discharge for 1.5 hours.

(217) The decomposition energy consumption of this comparative example is 151 eV/H2S molecule.

Example 12

(218) This example uses a plasma reaction apparatus similar to that of example 11 to carry out the decomposition reaction of hydrogen sulfide, except for that in this example:

(219) the ratio of L.sub.2 to the thickness D.sub.1 of the barrier dielectric 6 is 35:1.

(220) The rest parts of the example are same as those in the example 11.

(221) Results: the conversion of H.sub.2S is measured to be 67.2% after continuously performing the hydrogen sulfide decomposition reaction of the example for 20 minutes; and no abnormality has been discovered after performing the continuous discharge for 100 hours, both the discharge condition and the H.sub.2S conversion are kept stable. In addition, the decomposition energy consumption of the example is 23.6 eV/H.sub.2S molecules.

Example 13

(222) The hydrogen sulfide decomposition reaction is performed by using the low-temperature plasma reaction apparatus illustrated in FIG. 1b, and the low-temperature plasma reaction apparatus of this example differs from the low-temperature plasma reaction apparatus shown in FIG. 1a of the example 1 in the following aspects:

(223) in this example, the second cavity 2 is disposed inside the first cavity 1, and sidewalls of the first cavity 1 are formed by a barrier dielectric 6, the outer electrode 4 is disposed at an outer sidewall of the first cavity 1 in a surrounding manner, the material forming the outer electrode 4 is a stainless steel metal foil, and the outer electrode 4 is grounded;

(224) all sidewall of the second cavity 2 is formed by inner electrode 3, the material forming the inner electrode 3 is stainless steel, and the inner electrode 3 is connected with a high-voltage power supply;

(225) the ratio of L.sub.2 to the thickness D.sub.1 of the barrier dielectric 6 is 20:1; and H.sub.1:L.sub.3=1:100.

(226) The rest parts of the specific structure and structural parameters of this example are same with those in the example 1.

(227) In the example, a H.sub.2S/Ar mixed gas is introduced into a first cavity 1 of the low-temperature plasma reaction apparatus from a first inlet 11, wherein the volume fraction of H.sub.2S is 30%, the flow rate of the mixed gas is controlled such that the average residence time of the gas in a discharge region is 16.7 s, and the reaction pressure in the first cavity 1 of the reactor is kept at 0.2 MPa. After introducing the H.sub.2S/Ar mixed gas into the reaction apparatus for 30 minutes, an AC high-voltage power supply is switched on, and a plasma discharge field is formed between the inner electrode 3 and the solid grounding electrode by adjusting the voltage and frequency of the high-voltage power supply. Wherein the discharge conditions are as follows: the voltage is 21.3 kV, the frequency is 8.0 kHz, and the current is 1.17 A.

(228) The rest parts of the example are same as those in the example 1.

(229) Results: the conversion of H.sub.2S is measured to be 79.5% after continuously performing the hydrogen sulfide decomposition reaction of the example for 20 minutes; and no abnormality has been discovered after performing the continuous discharge for 100 hours, both the discharge condition and the H.sub.2S conversion are kept stable. In addition, the decomposition energy consumption of the example is 11.3 eV/H.sub.2S molecules.

Example 14

(230) The hydrogen sulfide decomposition reaction is performed by using the low-temperature plasma reaction apparatus illustrated in FIG. 1c, and the low-temperature plasma reaction apparatus of this example differs from the low-temperature plasma reaction apparatus shown in FIG. 1a of the example 1 in the following aspects:

(231) in this example, the second cavity 2 is disposed inside the first cavity 1, and the sidewalls of the first cavity 1 are formed by an outer electrode 4, the material forming the outer electrode 4 is copper foil, and the outer electrode 4 is grounded;

(232) in the example, the third cavity 7 is disposed outside the first cavity 1, the sidewall of the third cavity 7 is formed with stainless steel, the heat-conducting medium in the third cavity 7 is same as that in the second cavity 2, and the temperature of the heat-conducting medium is kept at 230° C.;
the sidewalls of the first cavity 1 are formed by barrier dielectric 6, the solid grounding electrode is disposed on the outer sidewall of the first cavity 1 in a surrounding manner, the material forming the solid grounding electrode is copper foil;
all sidewall of the second cavity 2 is formed by inner electrode 3, the material forming the inner electrode 3 is stainless steel, and the inner electrode 3 is connected with a high-voltage power supply;
the ratio of L.sub.2 to the thickness D.sub.1 of the barrier dielectric 6 is 0.5:1; and H.sub.1:L.sub.3=1:200.

(233) The rest parts of the specific structure and structural parameters of this example are same with those in the example 1.

(234) In the example, a H.sub.2S/CO.sub.2 mixed gas is introduced into a first cavity 1 of the low-temperature plasma reaction apparatus from a first inlet 11, wherein the volume fraction of H.sub.2S is 25%, the flow rate of the mixed gas is controlled such that the average residence time of the gas in a discharge region is 11.5 s, and the reaction pressure in the first cavity 1 of the reactor is kept at 0.1 MPa. After introducing the H.sub.2S/CO.sub.2 mixed gas into the reaction apparatus for 30 minutes, an AC high-voltage power supply is switched on, and a plasma discharge field is formed between the inner electrode 3 and the solid grounding electrode by adjusting the voltage and frequency of the high-voltage power supply. Wherein the discharge conditions are as follows: the voltage is 13.5 kV, the frequency is 2.4 kHz, and the current is 1.34 A.

(235) The rest parts of the example are same as those in the example 1.

(236) Results: the conversion of H.sub.2S is measured to be 76.7% after continuously performing the hydrogen sulfide decomposition reaction of the example for 20 minutes; and no abnormality has been discovered after performing the continuous discharge for 100 hours, both the discharge condition and the H.sub.2S conversion are kept stable. In addition, the decomposition energy consumption of the example is 12.9 eV/H.sub.2S molecules.

Example 15

(237) The hydrogen sulfide decomposition reaction is performed by using the low-temperature plasma reaction apparatus illustrated in FIG. 2b, and the low-temperature plasma reaction apparatus of this example differs from the low-temperature plasma reaction apparatus shown in FIG. 2a of the example 5 in the following aspects:

(238) In this example, the second cavity 2 is disposed inside the first cavity 1, and the outer electrode 3 is disposed on the inner sidewall of the first cavity 1 in a surrounding manner, the material forming the outer electrode 4 is a stainless steel metal foil, and the outer electrode 4 is grounded;

(239) all sidewall of the second cavity 2 is formed by inner electrode 3, the material forming the inner electrode 3 is stainless steel, and the inner electrode 3 is connected with a high-voltage power supply;

(240) moreover, the temperature of the heat-conducting medium in this example is kept at 182° C.

(241) The barrier dielectric 6 is disposed on the outer sidewall of the second cavity 2 in a surrounding manner;

(242) the ratio of L.sub.2 to the thickness D.sub.1 of the barrier dielectric 6 is 25:1; and H.sub.1:L.sub.3=1:120.

(243) The rest parts of the specific structure and structural parameters of this example are same with those in the example 5.

(244) In the example, a H.sub.2S/Ar mixed gas is introduced into a first cavity 1 of the plasma reaction apparatus from a first inlet 11, wherein the volume fraction of H.sub.2S is 30%, the flow rate of the mixed gas is controlled such that the average residence time of the gas in a discharge region is 10.7 s, and the reaction pressure in the first cavity 1 of the reactor is kept at 0.21 MPa. After introducing the H.sub.2S/Ar mixed gas into the reaction apparatus for 30 minutes, an AC high-voltage power supply is switched on, and a plasma discharge field is formed between the inner electrode 3 and the solid grounding electrode by adjusting the voltage and frequency of the high-voltage power supply. Wherein the discharge conditions are as follows: the voltage is 25.1 kV, the frequency is 13.3 kHz, and the current is 0.86 A.

(245) The rest parts of the example are same as those in the example 5.

(246) Results: the conversion of H.sub.2S is measured to be 77.5% after continuously performing the hydrogen sulfide decomposition reaction of the example for 20 minutes; and no abnormality has been discovered after performing the continuous discharge for 100 hours, both the discharge condition and the H.sub.2S conversion are kept stable. In addition, the decomposition energy consumption of the example is 10.3 eV/H.sub.2S molecules.

Example 16

(247) The hydrogen sulfide decomposition reaction is performed by using the low-temperature plasma reaction apparatus illustrated in FIG. 2c, and the low-temperature plasma reaction apparatus of this example differs from the low-temperature plasma reaction apparatus shown in FIG. 2a of the example 5 in the following aspects:

(248) in this example, the second cavity 2 is disposed inside the first cavity 1, the outer electrode 4 is disposed on an inner sidewall of the first cavity 1, the material forming the outer electrode 4 is a copper foil, and the outer electrode 4 is grounded;

(249) all sidewall of the second cavity 2 is formed by an inner electrode 3, the material forming the inner electrode 3 is stainless steel, and the inner electrode 3 is connected with a high-voltage power supply;

(250) a barrier dielectric 6 is disposed on the outer surface of the part of the inner electrode 3 extending into the first cavity 1, the upper edge of the barrier dielectric 6 is higher than the upper edge of the solid grounding electrode, and the material forming the barrier dielectric 6 is ceramic;
in this example, the third cavity 7 is disposed outside the first cavity 1, a sidewall of the third cavity 7 is formed with stainless steel, and the heat-conducting medium in the third cavity 7 is same as that in the second cavity 2.
The ratio of L.sub.2 to the thickness D.sub.1 of the barrier dielectric 6 is 0.7:1; and H.sub.1:L.sub.3=1:250.

(251) The rest parts of the specific structure and structural parameters of this example are same with those in the example 5.

(252) In the example, a H.sub.2S/CO mixed gas is introduced into a first cavity of the plasma reaction apparatus from a first inlet, wherein the volume fraction of H.sub.2S is 25%, the flow rate of the mixed gas is controlled such that the average residence time of the gas in a discharge region is 3.0 s, and the reaction pressure in the first cavity 1 of the reactor is kept at 0.16 MPa. After introducing the H.sub.2S/CO mixed gas into the reaction apparatus for 30 minutes, an AC high-voltage power supply is switched on, and a plasma discharge field is formed between the inner electrode 3 and the solid grounding electrode by adjusting the voltage and frequency of the high-voltage power supply. Wherein the discharge conditions are as follows: the voltage is 5.1 kV, the frequency is 900 Hz, and the current is 1.15 A.

(253) The rest parts of the example are same as those in the example 5.

(254) Results: the conversion of H.sub.2S is measured to be 76.9% after continuously performing the hydrogen sulfide decomposition reaction of the example for 20 minutes; and no abnormality has been discovered after performing the continuous discharge for 100 hours, both the discharge condition and the H.sub.2S conversion are kept stable. In addition, the decomposition energy consumption of the example is 12.7 eV/H.sub.2S molecules.

Example 17

(255) The hydrogen sulfide decomposition reaction is performed by using the low-temperature plasma reaction apparatus illustrated in FIG. 3b, and the low-temperature plasma reaction apparatus of this example differs from the low-temperature plasma reaction apparatus shown in FIG. 3a of the example 9 in the following aspects:

(256) in this example, the second cavity 2 is disposed inside the first cavity 1, and the outer electrode 3 is disposed on the inner sidewall of the first cavity 1 in a surrounding manner, the material forming the outer electrode 4 is a stainless steel metal foil, and the outer electrode 4 is grounded;

(257) all sidewall of the second cavity 2 is formed by inner electrode 3, the material forming the inner electrode 3 is stainless steel, and the inner electrode 3 is connected with a high-voltage power supply;

(258) the barrier dielectric 6 is disposed between the solid grounding electrode and the high-voltage electrode and does not directly contact with the solid grounding electrode and the high-voltage electrode;

(259) the ratio of L.sub.2 to the thickness D.sub.1 of the barrier dielectric 6 is 20:1; and H.sub.1:L.sub.3=1:300.

(260) The rest parts of the specific structure and structural parameters of this example are same with those in the example 9.

(261) In the example, a H.sub.2S/H.sub.2 mixed gas is introduced into a first cavity 1 of the low-temperature plasma reaction apparatus from a first inlet 11, wherein the volume fraction of H.sub.2S is 30%, the flow rate of the mixed gas is controlled such that the average residence time of the gas in a discharge region is 11.4 s, and the reaction pressure in the first cavity 1 of the reactor is kept at 0.08 MPa. After introducing the H.sub.2S/H.sub.2 mixed gas into the reaction apparatus for 30 minutes, an AC high-voltage power supply is switched on, and a plasma discharge field is formed between the inner electrode 3 and the solid grounding electrode by adjusting the voltage and frequency of the high-voltage power supply. Wherein the discharge conditions are as follows: the voltage is 25.4 kV, the frequency is 10.5 kHz, and the current is 0.94 A.

(262) The rest parts of the example are same as those in the example 9.

(263) Results: the conversion of H.sub.2S is measured to be 76.2% after continuously performing the hydrogen sulfide decomposition reaction of the example for 20 minutes; and no abnormality has been discovered after performing the continuous discharge for 100 hours, both the discharge condition and the H.sub.2S conversion are kept stable. In addition, the decomposition energy consumption of the example is 10.5 eV/H.sub.2S molecules.

Example 18

(264) The hydrogen sulfide decomposition reaction is performed by using the low-temperature plasma reaction apparatus illustrated in FIG. 3c, and the low-temperature plasma reaction apparatus of this example differs from the low-temperature plasma reaction apparatus shown in FIG. 3a of the example 9 in the following aspects:

(265) in this example, the second cavity 2 is disposed inside the first cavity 1, the outer electrode 4 is disposed on an inner sidewall of the first cavity 1, the material forming the outer electrode 4 is a copper foil, and the outer electrode 4 is grounded;

(266) all sidewall of the second cavity 2 is formed by inner electrode 3, the material forming the inner electrode 3 is stainless steel, and the inner electrode 3 is connected with a high-voltage power supply;

(267) in this example, the third cavity 7 is disposed outside the first cavity 1, a sidewall of the third cavity 7 is formed with stainless steel, and the heat-conducting medium in the third cavity 7 is same as that in the second cavity 2.

(268) The ratio of L.sub.2 to the thickness D.sub.1 of the barrier dielectric 6 is 0.5:1; and H.sub.1:L.sub.3=1:280.

(269) The rest parts of the specific structure and structural parameters of this example are same with those in the example 9.

(270) In the example, a H.sub.2S/CO mixed gas is introduced into a first cavity of the plasma reaction apparatus from a first inlet 11, wherein the volume fraction of H.sub.2S is 5%, the flow rate of the mixed gas is controlled such that the average residence time of the gas in a discharge region is 3.0 s, and the reaction pressure in the first cavity 1 of the reactor is kept at 0.24 MPa. After introducing the H.sub.2S/CO mixed gas into the reaction apparatus for 30 minutes, an AC high-voltage power supply is switched on, and a plasma discharge field is formed between the inner electrode 3 and the solid grounding electrode by adjusting the voltage and frequency of the high-voltage power supply. Wherein the discharge conditions are as follows: the voltage is 10.7 kV, the frequency is 900 Hz, and the current is 1.95 A.

(271) The rest parts of the example are same as those in the example 9.

(272) Results: the conversion of H.sub.2S is measured to be 78.7% after continuously performing the hydrogen sulfide decomposition reaction of the example for 20 minutes; and no abnormality has been discovered after performing the continuous discharge for 100 hours, both the discharge condition and the H.sub.2S conversion are kept stable. In addition, the decomposition energy consumption of the example is 13.5 eV/H.sub.2S molecules.

Example 19

(273) The hydrogen sulfide decomposition reaction is performed by using the low-temperature plasma reaction apparatus illustrated in FIG. 4b, and the low-temperature plasma reaction apparatus of this example differs from the low-temperature plasma reaction apparatus shown in FIG. 4a of the example 11 in the following aspects:

(274) in this example, the second cavity 2 is disposed inside the first cavity 1; all sidewall of the second cavity 2 is formed by inner electrodes 3, the material forming the inner electrodes 3 is stainless steel, and the inner electrodes 3 are connected with a high-voltage power supply;
the barrier dielectric 6 is disposed on the inner sidewall of the first cavity 1 in a surrounding manner, the outer electrode 4 forms the sidewall of the first cavity 1, and the outer electrodes 4 are grounded;
the rest parts of the specific structure and structural parameters of this example are same with those in the example 11.

(275) In the example, a H.sub.2S/Ar mixed gas is introduced into a first cavity 1 of the high-flux low-temperature plasma reaction apparatus from a reactor inlet 11, wherein the volume fraction of H.sub.2S is 45%, the flow rate of the mixed gas is controlled such that the average residence time of the gas in a discharge region is 0.9 s. After introducing the H.sub.2S/Ar mixed gas into the reactor for 30 minutes, an AC high-voltage power supply is switched on, and a plasma discharge field is formed between the inner electrode 3 and the solid grounding electrode by adjusting the voltage and frequency of the high-voltage power supply. Wherein the discharge conditions are as follows: the voltage is 12.7 kV, the frequency is 1.0 kHz, and the current is 4.1 A. The hydrogen sulfide gas is ionized in the discharge region and decomposed into hydrogen and elemental sulphur, and the elemental sulphur generated by discharge flows down slowly along the first cavity wall and discharges from the liquid product outlet 13. The reacted gas flows out from a gas product outlet 12.

(276) The rest parts of the example are same as those in the example 11.

(277) The conversion of H.sub.2S is measured to be 77.6% after continuously performing the hydrogen sulfide decomposition reaction of the example for 20 minutes; and no abnormality has been discovered after performing the continuous discharge for 100 hours, both the discharge condition and the H.sub.2S conversion are kept stable. In addition, the decomposition energy consumption of the example is 19.3 eV/H.sub.2S molecules (the energy required for decomposition of 1 molecule of H.sub.2S is 19.3 eV).

Example 20

(278) The hydrogen sulfide decomposition reaction is performed by using the low-temperature plasma reaction apparatus illustrated in FIG. 4c, and the low-temperature plasma reaction apparatus of this example differs from the low-temperature plasma reaction apparatus shown in FIG. 4a of the example 11 in the following aspects:

(279) in this example, the second cavity 2 is disposed inside the first cavity 1; all sidewall of the second cavity 2 are formed by inner electrodes 3, the material forming the inner electrodes 3 is stainless steel, and the inner electrodes 3 are connected with a high-voltage power supply;
in the example, the third cavity 7 is disposed outside the first cavity 1, a sidewall of the third cavity 7 is formed with stainless steel, and the heat-conducting medium in the third cavity 7 is same as that in the second cavity 2.
the rest parts of the specific structure and structural parameters of this example are same with those in the example 11.

(280) In the example, a H.sub.2S/Ar mixed gas is introduced into a first cavity 1 of the high-flux low-temperature plasma reaction apparatus from a reactor inlet, wherein the volume fraction of H.sub.2S is 65%, the flow rate of the mixed gas is controlled such that the average residence time of the gas in a discharge region is 0.9 s, and the reaction pressure in the first cavity 1 of the reactor is kept at 0.07 MPa. After introducing the H.sub.2S/Ar mixed gas into the reactor for 30 minutes, an AC high-voltage power supply is switched on, and a plasma discharge field is formed between the inner electrode 3 and the solid grounding electrode by adjusting the voltage and frequency of the high-voltage power supply. Wherein the discharge conditions are as follows: the voltage is 10.4 kV, the frequency is 1.2 kHz, and the current is 3.1 A. The hydrogen sulfide gas is ionized in the discharge region and decomposed into hydrogen and elemental sulphur, and the elemental sulphur generated by discharge flows down slowly along the first cavity wall and discharges from the liquid product outlet 13. The reacted gas flows out from a gas product outlet 12.

(281) The rest parts of the example are same as those in the example 11.

(282) The conversion of H.sub.2S is measured to be 78.4% after continuously performing the hydrogen sulfide decomposition reaction of the example for 20 minutes; and no abnormality has been discovered after performing the continuous discharge for 100 hours, both the discharge condition and the H.sub.2S conversion are kept stable. In addition, the decomposition energy consumption of the example is 17.9 eV/H.sub.2S molecules (the energy required for decomposition of 1 molecule of H2S is 17.9 eV).

(283) It is revealed from the above results that the conversion of hydrogen sulfide can be significantly improved compared with the prior art when the low-temperature plasma reaction apparatus provided by the invention is used for decomposition of hydrogen sulfide, and the reaction apparatus provided by the invention can maintain high conversion of hydrogen sulfide and low energy consumption of decomposition for a long period.

(284) The above content describes in detail the preferred embodiments of the invention, but the invention is not limited thereto. A variety of simple modifications can be made in regard to the technical solutions of the invention within the scope of the technical concept of the invention, including a combination of individual technical features in any other suitable manner, such simple modifications and combinations thereof shall also be regarded as the content disclosed by the invention, each of them falls into the protection scope of the invention.