ATOMIZING LIQUID GEL WITH REVERSIBLE PHASE TRANSITION CHARACTERISTICS, PREPARATION METHOD AND APPLICATIONS THEREOF

Abstract

An atomizing liquid gel with reversible phase transition characteristics includes: a sugar-based gelling agent, 0.1-3.0 wt %; an atomizing agent, 97.0-99.9 wt %; a molecule of the sugar-based gelling agent is a sugar molecule introduced with an amide group and/or an aryl group, and the sugar molecule optionally further includes at least one hydrophobic structural part selected from —C.sub.xH.sub.y, —O—C.sub.xB.sub.y and

##STR00001##

and x>2 and y>2. The atomizing liquid gel has characteristics of thermal reversible phase transition and/or shear reversible phase transition, a temperature of gel-sol phase transition is 100° C.-248° C., and a critical shear stress of the gel-sol phase transition is 40-800 Pa. Under heating and/or oscillation, the atomizing liquid gel converts from the gel state to a sol state, when the heating and/or oscillation are stopped, the atomizing liquid gel is quickly recovered from the sol state to the gel state.

Claims

1. An atomizing liquid gel with reversible phase transition characteristics, comprising: a sugar-based gelling agent, 0.1-3.0 wt %; an atomizing agent, 97.0-99.9 wt %; wherein a molecule of the sugar-based gelling agent is a sugar molecule introduced with an amide group and/or an aryl group, and the sugar molecule optionally further comprises at least one hydrophobic structural part selected from —C.sub.xH.sub.y, —O—C.sub.xH.sub.y and ##STR00032## and wherein x>2, y>2.

2. The atomizing liquid gel according to claim 1, wherein the sugar-based gelling agent is selected from at least one of five types of sugar-based gelling agents I-V; wherein a chemical structural formula of the sugar-based gelling agent I is as follows: ##STR00033## wherein, A is an arylene group, or a heteroarylene group with 1-4 nitrogen heteroatoms; and R is —C.sub.xH.sub.y, —O—C.sub.xH.sub.y, or ##STR00034## and x>2, y>2; a chemical structural formula of the sugar-based gelling agent II is as follows: ##STR00035## wherein, S is a monosaccharide group, a maltose group, a cellobiose group, or a lactose group; A is the arylene group, or the heteroarylene group with 1-4 nitrogen heteroatoms; and R′ is a C.sub.2-16 alkyl group, a C.sub.2-16 alkenyl group, or a C.sub.2-16 alkynyl group; a chemical structural formula of the sugar-based gelling agent III is as follows: ##STR00036## wherein, R.sub.1 is the C.sub.2-16 alkyl group, the C.sub.2-16 alkenyl group, or the C.sub.2-16 alkynyl group; and R.sub.2 is ##STR00037## a chemical structural formula of the sugar-based gelling agent IV is as follows: ##STR00038## wherein, S is the monosaccharide group, the maltose group, the cellobiose group or the lactose group; and A (R).sub.n is ##STR00039## and a chemical structural formula of the sugar-based gelling agent V is as follows: ##STR00040## wherein, A′ is an aromatic alkylene group, or a heteroarylene alkylene group with 1-4 nitrogen heteroatoms; and R′ is the C.sub.2-16 alkyl group, the C.sub.2-16 alkenyl group, or the C.sub.2-16 alkynyl group.

3. The atomizing liquid gel according to claim 1, wherein the chemical structural formula of the sugar-based gelling agent I is as follows: ##STR00041## the chemical structural formula of the sugar-based gelling agent II is as follows: ##STR00042## the chemical structural formula of the sugar-based gelling agent III is as follows: ##STR00043## the chemical structural formula of the sugar-based gelling agent IV is as follows: ##STR00044## and the chemical structural formula of the sugar-based gelling agent V is as follows: ##STR00045##

4. The atomizing liquid gel according to claim 1, wherein, based on a mass percentage of an atomizing liquid of the atomizing liquid gel, the atomizing liquid comprises: the atomizing agent, wherein the atomizing agent accounts for 90-100 wt % of the atomizing liquid; nicotine, wherein the nicotine accounts for 0-10 wt % of the atomizing liquid; and a perfume, wherein the perfume accounts for 0-10 wt % of the atomizing liquid; the atomizing agent is a mixture of glycerol and propylene glycol, wherein a volume ratio of the glycerol and the propylene glycol is 3:7-7:3.

5. The atomizing liquid gel according to claim 1, wherein the atomizing liquid gel with the reversible phase transition characteristics is the atomizing liquid gel having characteristics of thermal reversible phase transition and/or shear reversible phase transition; a temperature of gel-sol phase transition of the atomizing liquid gel is 100° C.-248° C., and a critical shear stress of the gel-sol phase transition of the atomizing liquid gel is 40-800 Pa.

6. A preparation method of the atomizing liquid gel according to claim 1, comprising: heating and dissolving the sugar-based gelling agent in an atomizing liquid to obtain a mixture, stirring the mixture until the sugar-based gelling agent is completely dissolved, and slowly cooling the mixture to form the atomizing liquid gel.

7. An application of the atomizing liquid gel according to claim 1, comprising: directly injecting a molten atomizing liquid gel solution into a liquid storage tank of an electronic cigarette atomizer, and after the molten atomizing liquid gel solution is cooled and gelled, an atomizing liquid gel cartridge suitable for electronic cigarettes is obtained.

8. An application of the atomizing liquid gel according to claim 1, comprising: directly injecting a molten atomizing liquid gel solution into an aerosol generating device made of a porous material, and after being cooled and gelled, the molten atomizing liquid gel solution is fixed into the porous material.

9. The application according to claim 8, wherein the porous material is selected from a single material or a composite material of a metal, an alloy, ceramics, a microelectromechanical system (MEMS) element, a carbon-based material and a high-molecular polymer.

10. An application of the atomizing liquid gel according to claim 1, comprising: coating a molten atomizing liquid gel solution to an inner surface of a cigarette paper of a heat-not-burn cigarette through sizing, and after being cooled and gelled, the molten atomizing liquid gel solution is fixed into fiber pores of the cigarette paper.

Description

DETAILED DESCRIPTION OF THE EMBODIMENTS

[0090] For the convenience of understanding, the technical solution of the present invention is further illustrated through specific embodiments. It should be understood by other skilled persons that the illustrated embodiments are merely intended to assist in the understanding of the present invention and therefore should not be regarded as a specific limitation of the present invention.

[0091] In the following embodiments, the gel-sol phase transition temperature is tested by the following method: a falling-ball method is used for determination, and the specific steps are as follows. The gel is placed in a test tube with a diameter of 10 mm, and a glass bead with a diameter of 5 mm and a mass of 0.24 g is placed on the top of the gel. Subsequently, the test tube is placed in a constant temperature oil bath, and heated at the heating rate of 1.5° C./min. The temperature at which the glass bead is completely submerged in the solution corresponds to the gel-sol phase transition temperature. The test is repeated twice to obtain an average value.

[0092] In the following embodiments, the critical shear stress of the gel-sol phase transition is tested according to the international standard method ISO 3219 (1993) Plastics-Polymers/Resins in the Liquid State or as Emulsions or Dispersions-Determination of Viscosity Using a Rotational Viscometer with Defined Shear Rate.

Embodiment 1

[0093] The present embodiment provides an atomizing liquid gel 1 with thermal reversible phase transition characteristics, which includes: a sugar-based gelling agent, 0.8 wt %; an atomizing liquid, 99.2 wt %. Based on the mass percentage of the atomizing liquid, the atomizing liquid includes: an atomizing agent, which accounts for 92.0 wt % of the atomizing liquid; nicotine, which accounts for 2.0 wt % of the atomizing liquid; a perfume, which accounts for 6.0 wt % of the atomizing liquid. The atomizing agent is a mixture of glycerol and propylene glycol, in which a volume ratio of the glycerol and the propylene glycol is 5:5.

[0094] The chemical structural formula of the sugar-based gelling agent is as follows:

##STR00021##

[0095] The atomizing liquid gel 1 solution of the present embodiment is directly injected into a liquid storage tank of an e-cigarette atomizer. After the solution is cooled and gelled, an atomizing liquid gel cartridge 1 suitable for e-cigarette is prepared, which is used in the e-cigarette. The gel-sol phase transition temperature is 125° C., which is close to the evaporation and atomization temperature of the atomizing liquid. After being heated to 220° C., the atomizing liquid gel converts from the gel state to a sol state, the atomizing agent fixed in the gel is released together with the dissolved substances of nicotine and aroma components to form an inhalable aerosol. The heating is stopped after smoking a few puffs. When the temperature of the e-cigarette drops below the gel-sol phase transition temperature, the gel at the sol state is recovered to the gel state, and the atomizing agent, nicotine and aroma component molecules that have not been atomized in the gel are refixed in the gel network. It can be seen that the atomizing liquid gel 1 prepared by the present embodiment has obvious thermal reversible phase transition characteristics. After repeated smoking for several times, the phase transition property of the atomizing liquid gel 1 is still very obvious. Therefore, the atomizing liquid gel 1 prepared by the present embodiment is suitable for the e-cigarette products that require high-temperature atomization of the atomizing liquid.

Embodiment 2

[0096] The present embodiment provides an atomizing liquid gel 2 with shear reversible phase transition characteristics, and the chemical structure formula of the sugar-based gelling agent used is as follows:

##STR00022##

[0097] The other preparation conditions and the proportion of each component are the same as those in embodiment 1.

[0098] The molten atomizing liquid gel 2 solution of the present embodiment is directly injected into a liquid storage tank of an atomizer, and an atomizing liquid gel cartridge 2 is prepared after the solution is cooled and gelled, which is used in a high-frequency bulk acoustic wave oscillation atomization device. The critical shear stress of the gel-sol phase transition is 185 Pa. Under high shear and violent oscillation (the frequency of sound wave is 2.4 MHz), the gel network structure is destroyed, the viscosity of the gel decreases, and the trapped atomizing liquid is released to produce an inhalable aerosol. After smoking for several times, the oscillation is stopped, the gel is quickly self-assembled, and the viscosity of the gel increases again. The above process can be repeated many times. In conclusion, the atomizing liquid gel of the present invention can be applied to a high-frequency bulk acoustic wave oscillation atomization device.

Embodiment 3

[0099] The present embodiment provides an atomizing liquid gel 3 with thermal reversible phase transition characteristics, and the chemical structure formula of the sugar-based gelling agent used is as follows:

##STR00023##

[0100] The other preparation conditions and the proportion of each component are the same as those in embodiment 1.

[0101] The sugar-based gelling agent of present embodiment has the advantages as follows.

[0102] 1. In the sugar-based gelling agent, one side is a hydrophobic hydrocarbyl fragment, and the other side is a hydrophilic glycosyl ligand, which is similar to a surfactant. The strong hydrogen bonding interaction in the glycosyl ligand leads to the extension of unidirectional molecular self-assembly, resulting in the formation of a fiber or ribbon-like 3D network. The amphipathic structure is suitable for gelation of complex atomizing liquid systems containing polar components such as glycerol and propylene glycol, and non-polar volatile components such as aromatic alcohols.

[0103] 2. The hydrophobic hydrocarbyl fragment on one side increases the length of the hydrocarbon chain, and correspondingly introduces Van der Waals' force. Moreover, the introduction of intermediate group of aromatic ring can correspondingly introduce π-π stacking effect, or introduce Van der Waals' force and π-π stacking effect, which can not only enhance the intermolecular hydrogen bonding strength of the sugar-based gelling agent, but also weaken the influence of the solvation of glycerol and propylene glycol on the intermolecular hydrogen bonding interaction of the gelling agent, thereby improving the stability of the sugar-based gelling agent to fix the atomizing liquid, further increasing the diversity of gelation, and increasing the gelation temperature.

[0104] 3. The sugar-based gelling agent uses a cyclic sugar with more directed hydroxyl groups as the sugar-based raw material, and introduces additional hydrogen bond groups (such as amide groups) into the sugar-based raw material to prepare the sugar-based gelling agent. In addition to the original intermolecular hydrogen bonding interaction, such sugar-based gelling agent molecules can further form a strong cooperative hydrogen bond network, and increase the hydrogen bond driving ability for self-assembly. As a result, the competitiveness of hydrogen bonds of alcoholic hydroxyl groups in glycerol and propylene glycol is weakened, the network structure formed is more rigid, and the thermal stability and thermal reversible phase transition temperature are improved.

[0105] The atomizing liquid gel 3 solution of the present embodiment is directly injected into a liquid storage tank of an e-cigarette atomizer. After the solution is cooled and gelled, an atomizing liquid gel cartridge 3 suitable for e-cigarette is prepared, which is used in the e-cigarette. The gel-sol phase transition temperature is 205° C., which is close to the evaporation and atomization temperature of the atomizing liquid. After being heated to 220° C., the atomizing liquid gel converts from the gel state to a sol state, the atomizing agent fixed in the gel is released together with the dissolved substances of nicotine and aroma components to form an inhalable aerosol. The heating is stopped after smoking a few puffs. When the temperature of the e-cigarette drops below the gel-sol phase transition temperature, the gel at the sol state is recovered to the gel state, and the atomizing agent, nicotine and aroma component molecules that have not been atomized in the gel are refixed in the gel network. It can be seen that the atomizing liquid gel 3 prepared by the present embodiment has obvious thermal reversible phase transition characteristics. After repeated smoking for several times, the phase transition property of the atomizing liquid gel 3 is still very obvious. Therefore, the atomizing liquid gel 3 prepared by the present embodiment is suitable for the e-cigarette products that require high-temperature atomization of the atomizing liquid.

Embodiment 4

[0106] The present embodiment provides an atomizing liquid gel 4 with shear reversible phase transition characteristics, and the chemical structure formula of the sugar-based gelling agent used is as follows:

##STR00024##

[0107] The other preparation conditions and the proportion of each component are the same as those in embodiment 1.

[0108] The molten atomizing liquid gel 4 solution of the present embodiment is directly injected into a liquid storage tank of an atomizer, and an atomizing liquid gel cartridge 4 is prepared after the solution is cooled and gelled, which is in a high-frequency bulk acoustic wave oscillation atomization device. The critical shear stress of the gel-sol phase transition is 580 Pa. Under high shear and violent oscillation (the frequency of sound wave is 2.4 MHz), the gel network structure is destroyed, the viscosity of the gel decreases, and the trapped atomized liquid is released to produce an inhalable aerosol. After smoking for several times, the oscillation is stopped, the gel is quickly self-assembled, and the viscosity of the gel increases again. The above process can be repeated many times. In conclusion, the atomizing liquid gel of the present invention can be applied to a high-frequency bulk acoustic wave oscillation atomization device.

Embodiments 5-6

[0109] These embodiments respectively provide an atomizing liquid gel 5 and an atomizing liquid gel 6 with thermal reversible phase transition characteristics, and the chemical structure formulas of the sugar-based gelling agent used are respectively presented as follows:

##STR00025##

[0110] The other preparation conditions and the proportion of each component are the same as those in embodiment 1.

[0111] The atomizing liquid gel 5 solution and the atomizing liquid gel 6 solution of these embodiments are directly injected into an aerosol generating device made of a porous material, respectively. After being cooled and gelled, the solution is fixed in the porous material, respectively. The gel-sol phase transition temperature is 230° C. and 235° C., respectively. After repeated smoking for several times, the phase transition properties of the atomizing liquid gel 5 and the atomizing liquid gel 6 are still very obvious. Therefore, the atomizing liquid gel 5 and atomizing liquid gel 6 prepared by these embodiments are suitable for the e-cigarette products that require high-temperature atomization of the atomizing liquid.

Embodiments 7-9

[0112] These embodiments provide atomizing liquid gels 7-9 with thermal reversible phase transition characteristics, and the chemical structure formulas of the sugar-based gelling agent used are respectively presented as follows:

##STR00026##

[0113] The other preparation conditions and the proportion of each component are the same as those in embodiment 1.

[0114] The molten atomizing liquid gel 7-9 solutions of these embodiments are directly coated on an inner surface of a cigarette paper suitable for heat-not-burn cigarettes by sizing. Due to the good creep recovery and thixotropy, the gel can penetrate into the fibrous pores of cigarette paper when heated in the sol state and be fixed in these pores after cooling into a gel. Subsequently, the cigarette paper with fixed gels is made into a heat-not-burn cigarette, and is sucked with the matching combination of the heat-not-burn cigarettes. When the heat-not-burn cigarette is baked at low temperature, the gel in the cigarette paper undergoes a sol-phase transition, and the fixed atomizing liquid is heated and atomized. Moreover, the generated aerosol of atomizing agent, nicotine and aroma component will be released together with the substances evaporated by heating the cigarette filling, which will increase the amount of smoke, and enhance the flavor and fragrance. In the production and storage process of cigarettes, the gel fixed in the cigarette paper remains stable properties due to the thermal stability and chemical stability of the supermolecular structure of the gel.

Embodiment 10

[0115] The present embodiment provides an atomizing liquid gel 10 with thermal reversible phase transition characteristics, and the chemical structure formula of the sugar-based gelling agent used is as follows:

##STR00027##

[0116] The other preparation conditions and the proportion of each component are the same as those in embodiment 1.

[0117] The atomizing liquid gel 10 solution of the present embodiment is directly injected into a liquid storage tank of an e-cigarette atomizer. After the solution is cooled and gelled, an atomizing liquid gel cartridge 10 suitable for e-cigarette is prepared, which is used in the e-cigarette. The gel-sol phase transition temperature is 145° C., which is close to the evaporation and atomization temperature of the atomizing liquid. After being heated to 220° C., the atomizing liquid gel converts from the gel state to a sol state, the atomizing agent fixed in the gel is released together with the dissolved substances of nicotine and aroma components to form an inhalable aerosol. The heating is stopped after smoking a few puffs. When the temperature of the e-cigarette drops below the gel-sol phase transition temperature, the gel at the sol state is recovered to the gel state, and the atomizing agent, nicotine and aroma component molecules that have not been atomized in the gel are refixed in the gel network. It can be seen that the atomizing liquid gel 10 prepared by the present embodiment has obvious thermal reversible phase transition characteristics. After repeated smoking for several times, the phase transition property of the atomizing liquid gel 10 is still very obvious. Therefore, the atomizing liquid gel 10 prepared by the present embodiment is suitable for the e-cigarette products that require high-temperature atomization of the atomizing liquid.

Embodiment 11

[0118] The present embodiment provides an atomizing liquid gel 11 with shear reversible phase transition characteristics, and the chemical structure formula of the sugar-based gelling agent used is as follows:

##STR00028##

[0119] The other preparation conditions and the proportion of each component are the same as those in embodiment 1.

[0120] The molten atomizing liquid gel 11 solution of the present embodiment is directly injected into a liquid storage tank of an atomizer, and an atomizing liquid gel cartridge 11 is prepared after the solution is cooled and gelled, which is used in a high-frequency bulk acoustic wave oscillation atomization device. The critical shear stress of the gel-sol phase transition is 200 Pa. Under high shear and violent oscillation (the frequency of sound wave is 2.4 MHz), the gel network structure is destroyed, the viscosity of the gel decreases, and the trapped atomized liquid is released to produce an inhalable aerosol. After smoking for several times, the oscillation is stopped, the gel is quickly self-assembled, and the viscosity of the gel increases again. The above process can be repeated many times. In conclusion, the atomizing liquid gel of the present invention can be applied to a high-frequency bulk acoustic wave oscillation atomization device.

Embodiment 12

[0121] The present embodiment provides an atomizing liquid gel 12 with thermal reversible phase transition characteristics, and the chemical structure formula of the sugar-based gelling agent used is as follows:

##STR00029##

[0122] The other preparation conditions and the proportion of each component are the same as those in embodiment 1.

[0123] The atomizing liquid gel 12 solution of the present embodiment is directly injected into an aerosol generating device made of a porous material. After being cooled and gelled, the solution is fixed in the porous material. The gel-sol phase transition temperature is 155° C. After repeated smoking for several times, the phase transition property of the atomizing liquid gel 12 is still very obvious. Therefore, the atomizing liquid gel 12 prepared by the present embodiment is suitable for the e-cigarette products that require high-temperature atomization of the atomizing liquid.

Embodiment 13

[0124] The present embodiment provides an atomizing liquid gel 13 with thermal reversible phase transition characteristics, and the chemical structure formula of the sugar-based gelling agent used is as follows:

##STR00030##

[0125] The other preparation conditions and the proportion of each component are the same as those in embodiment 1.

[0126] The atomizing liquid gel 13 solution of the present embodiment is directly injected into a liquid storage tank of an e-cigarette atomizer. After the solution is cooled and gelled, an atomizing liquid gel cartridge 13 suitable for e-cigarette is prepared, which is used in the e-cigarette. The gel-sol phase transition temperature is 225° C., which is close to the evaporation and atomization temperature of the atomizing liquid. After being heated to 220° C., the atomizing liquid gel converts from the gel state to a sol state, the atomizing agent fixed in the gel is released together with the dissolved substances of nicotine and aroma components to form an inhalable aerosol. The heating is stopped after smoking a few puffs. When the temperature of the e-cigarette drops below the gel-sol phase transition temperature, the gel at the sol state is recovered to the gel state, and the atomizing agent, nicotine and aroma component molecules that have not been atomized in the gel are refixed in the gel network. It can be seen that the atomizing liquid gel 13 prepared by the present embodiment has obvious thermal reversible phase transition characteristics. After repeated smoking for several times, the phase transition property of the atomizing liquid gel 13 is still very obvious. Therefore, the atomizing liquid gel 13 prepared by the present embodiment is suitable for the e-cigarette products that require high-temperature atomization of the atomizing liquid.

[0127] The atomizing liquid gel cartridge 13 is used in a high-frequency bulk acoustic wave oscillation atomization device. The critical shear stress of the gel-sol phase transition is 690 Pa. Under high shear and violent oscillation (the frequency of sound wave is 2.4 MHz), the gel network structure is destroyed, the viscosity of the gel decreases, and the trapped atomized liquid is released to produce an inhalable aerosol. After smoking for several times, the oscillation is stopped, the gel is quickly self-assembled, and the viscosity of the gel increases again. The above process can be repeated many times. In conclusion, the atomizing liquid gel of the present invention can be applied to a high-frequency bulk acoustic wave oscillation atomization device.

Embodiment 14

[0128] The present embodiment provides an atomizing liquid gel 14 with thermal reversible phase transition characteristics, and the chemical structure formula of the sugar-based gelling agent used is as follows:

##STR00031##

[0129] The other preparation conditions and the proportion of each component are the same as those in embodiment 1.

[0130] The atomizing liquid gel 14 solution of the present embodiment is directly injected into a liquid storage tank of an e-cigarette atomizer. After the solution is cooled and gelled, an atomizing liquid gel cartridge 14 suitable for e-cigarette is prepared, which is used in the e-cigarette. The gel-sol phase transition temperature is 175° C., which is close to the evaporation and atomization temperature of the atomizing liquid. After being heated to 220° C., the atomizing liquid gel converts from the gel state to a sol state, the atomizing agent fixed in the gel is released together with the dissolved substances of nicotine and aroma components to form an inhalable aerosol. The heating is stopped after smoking a few puffs. When the temperature of the e-cigarette drops below the gel-sol phase transition temperature, the gel at the sol state is recovered to the gel state, and the atomizing agent, nicotine and aroma component molecules that have not been atomized in the gel are refixed in the gel network. It can be seen that the atomizing liquid gel 14 prepared by the present embodiment has obvious thermal reversible phase transition characteristics. After repeated smoking for several times, the phase transition property of the atomizing liquid gel 14 is still very obvious. Therefore, the atomizing liquid gel 14 prepared by the present embodiment is suitable for the e-cigarette products that require high-temperature atomization of the atomizing liquid.

[0131] The atomizing liquid gel cartridge 14 is used in a high-frequency bulk acoustic wave oscillation atomization device. The critical shear stress of the gel-sol phase transition is 440 Pa. Under high shear and violent oscillation (the frequency of sound wave is 2.4 MHz), the gel network structure is destroyed, the viscosity of the gel decreases, and the trapped atomized liquid is released to produce an inhalable aerosol. After smoking for several times, the oscillation is stopped, the gel is quickly self-assembled, and the viscosity of the gel increases again. The above process can be repeated many times. In conclusion, the atomizing liquid gel of the present invention can be applied to a high-frequency bulk acoustic wave oscillation atomization device.