A method of converting methane to an oxygenate. The method includes converting methane to an oxygenate with a transition metal ion loaded zeolite catalyst in an aqueous medium in the presence of gaseous O.sub.2 and CO at a temperature lower than 200 C. Also disclosed are a two-metal ion zeolite catalyst for converting methane to methanol and a method for preparing the two-metal ion zeolite catalyst.

The invention relates to a method for separating formic acid from a reaction mixture which comprises, in addition to formic acid, a polyoxometalate ion of general formula [PMo.sub.xV.sub.yO.sub.40].sup.n, where 6x11, 1y6, x+y=12 and 3<n<10, where n, x and y are each integers, wherein the separation occurs by means of an extraction using a linear primary alcohol, wherein the carbon chain of the alcohol comprises 5 to 12 carbon atoms, and the reaction mixture is present in a protic solvent.

The invention relates to a method for separating formic acid from a reaction mixture which comprises, in addition to formic acid, a polyoxometalate ion of general formula [PMo.sub.xV.sub.yO.sub.40].sup.n, where 6x11, 1y6, x+y=12 and 3<n<10, where n, x and y are each integers, wherein the separation occurs by means of an extraction using a linear primary alcohol, wherein the carbon chain of the alcohol comprises 5 to 12 carbon atoms, and the reaction mixture is present in a protic solvent.

This disclosure describes systems and methods for using pyrolysis tail gas as the source for additional hydrogen to be used in the pyrolysis reaction. Tail gas is separated from the pyrolysis products and a portion of the tail gas is converted into formic acid (HCOOH). The formic acid is then injected into the pyrolysis reactor where it becomes the donor of two monohydrogen atoms and is ultimately converted into CO.sub.2 under reaction conditions. In this fashion, a closed loop pyrolysis hydrogen donor system may be created utilizing a generally non-toxic intermediary derived from the pyrolysis reaction products. This disclosure also describes using a ruthenium catalyst supported on particles of activated carbon to improve the yield of pyrolysis reactions.

This disclosure describes systems and methods for using pyrolysis tail gas as the source for additional hydrogen to be used in the pyrolysis reaction. Tail gas is separated from the pyrolysis products and a portion of the tail gas is converted into formic acid (HCOOH). The formic acid is then injected into the pyrolysis reactor where it becomes the donor of two monohydrogen atoms and is ultimately converted into CO.sub.2 under reaction conditions. In this fashion, a closed loop pyrolysis hydrogen donor system may be created utilizing a generally non-toxic intermediary derived from the pyrolysis reaction products. This disclosure also describes using a ruthenium catalyst supported on particles of activated carbon to improve the yield of pyrolysis reactions.

Disclosed is a method of catalytic oxidation of lignite using oxygen as an oxidant at atmospheric pressure, belonging to a method of mild oxidation of lignite. The method is used to mildly oxidize the lignite using the oxygen as the oxidant under the action of a nitroxide radical catalyst and a metal salt or metal oxide cocatalyst; the process comprises the following steps: pulverizing the lignite to 200 meshes or less, drying a pulverized coal sample at a temperature of 80 C. in vacuum for 10 h, weighing 0.5 g of the treated coal sample, sequentially adding 10 ml of acetic acid, 0.5 mmol of a catalyst and 0.15 to 0.25 mmol of a cocatalyst into a round-bottom flask, connecting a tee joint to an upper orifice of a condenser pipe, replacing oxygen in vacuum for three times so that the round-bottom flask is filled with the oxygen, keeping oxygen pressure at 0.1 MPa, reacting at a temperature of 80 C. to 120 C. for 4 to 12 h; filtering after the reaction is finished; decompressing a filtrate to remove the acetic acid, adding a small amount of ethyl acetate to dissolve, then using an excess CH.sub.2N.sub.2/ether solution to esterify for 10 h at room temperature, using 0.45 m filter paper to filter, and analyzing an esterified product through a gas chromatography-mass spectrometer. The method has the advantages of using the oxygen as the oxidant, having low price, having no toxicity, and achieving environmental protection and mild conditions.

Disclosed is a method of catalytic oxidation of lignite using oxygen as an oxidant at atmospheric pressure, belonging to a method of mild oxidation of lignite. The method is used to mildly oxidize the lignite using the oxygen as the oxidant under the action of a nitroxide radical catalyst and a metal salt or metal oxide cocatalyst; the process comprises the following steps: pulverizing the lignite to 200 meshes or less, drying a pulverized coal sample at a temperature of 80 C. in vacuum for 10 h, weighing 0.5 g of the treated coal sample, sequentially adding 10 ml of acetic acid, 0.5 mmol of a catalyst and 0.15 to 0.25 mmol of a cocatalyst into a round-bottom flask, connecting a tee joint to an upper orifice of a condenser pipe, replacing oxygen in vacuum for three times so that the round-bottom flask is filled with the oxygen, keeping oxygen pressure at 0.1 MPa, reacting at a temperature of 80 C. to 120 C. for 4 to 12 h; filtering after the reaction is finished; decompressing a filtrate to remove the acetic acid, adding a small amount of ethyl acetate to dissolve, then using an excess CH.sub.2N.sub.2/ether solution to esterify for 10 h at room temperature, using 0.45 m filter paper to filter, and analyzing an esterified product through a gas chromatography-mass spectrometer. The method has the advantages of using the oxygen as the oxidant, having low price, having no toxicity, and achieving environmental protection and mild conditions.

Methods for catalytic generation of formic acid at an oxygen partial pressure of less than 1 bar and regeneration of the catalyst used in this process, wherein a polyoxometallate ion of the general formula [PMo.sub.xV.sub.yO.sub.40].sup.n, which serves as the catalyst, is brought in contact with an alpha-hydroxyaldehyde, an alpha-hydroxycarboxylic acid, a carbohydrate, a glycoside or a polymer containing a carbon chain with at least one OH group bound as a repeatedly occurring substituent to the carbon chain and/or an O, N or S atom occurring repeatedly in the carbon chain in a liquid solution in a vessel, at a temperature above 70 C. and below 120 C.

Methods for catalytic generation of formic acid at an oxygen partial pressure of less than 1 bar and regeneration of the catalyst used in this process, wherein a polyoxometallate ion of the general formula [PMo.sub.xV.sub.yO.sub.40].sup.n, which serves as the catalyst, is brought in contact with an alpha-hydroxyaldehyde, an alpha-hydroxycarboxylic acid, a carbohydrate, a glycoside or a polymer containing a carbon chain with at least one OH group bound as a repeatedly occurring substituent to the carbon chain and/or an O, N or S atom occurring repeatedly in the carbon chain in a liquid solution in a vessel, at a temperature above 70 C. and below 120 C.

Methods for catalytic generation of formic acid at an oxygen partial pressure of less than 1 bar and regeneration of the catalyst used in this process, wherein a polyoxometallate ion of the general formula [PMo.sub.xV.sub.yO.sub.40].sup.n, which serves as the catalyst, is brought in contact with an alpha-hydroxyaldehyde, an alpha-hydroxycarboxylic acid, a carbohydrate, a glycoside or a polymer containing a carbon chain with at least one OH group bound as a repeatedly occurring substituent to the carbon chain and/or an O, N or S atom occurring repeatedly in the carbon chain in a liquid solution in a vessel, at a temperature above 70 C. and below 120 C.