Process for conversion of coal to hydrocarbon and other values

Claim 2

A process for conversion of coal to gaseous hydrocarbons and volatile distillates comprising the steps of: reacting coal or peat and a hydrosulfide, a sulfide or a polysulfide of an alkali metal, hydrates thereof, or mixtures thereof in presence of water, wherein water is added during the reaction, at a rate sufficient to hydrogenate the coal or peat to obtain the desired end product cut of gas or liquid or mixtures of both, adding sulfur or hydrogen sulfide or neither, said hydrogen sulfide being added, on space time velocity basis, from about 10 to about 30 ml/min/liter, said reaction being at a temperature between 50° C. and up to 450° C. at a pressure from subatmospheric to about 5 atm., and recovering volatile liquid distillates and hydrocarbon gases as hydrocarbon values.

Claim 3

A process for conversion of coal to gaseous hydrocarbons and volatile distillates comprising the steps of: reacting coal or peat and a hydrosulfide, a sulfide or a polysulfide of an alkali metal, hydrates thereof, or mixtures thereof in presence of water, wherein water is present during the reaction, at a rate equivalent to about the amount of hydrocarbon recovered to about 130% of the hydrocarbon recovered, adding sulfur or hydrogen sulfide or neither, said hydrogen sulfide being added, on space time velocity basis, from about 10 to about 30 ml/min/liter, said reaction being at a temperature between 50° C. and up to 450° C. at a pressure from subatmospheric to about 5 atm., and recovering volatile liquid distillates and hydrocarbon gases as hydrocarbon values.

Claim 4

A process for conversion of coal to gaseous hydrocarbons and volatile distillates comprising the steps of: reacting coal or peat and a hydrosulfide, a sulfide or a polysulfide of an alkali metal, hydrates thereof, or mixtures thereof in presence of water, wherein water is present during the reaction, at a rate equivalent to about the amount of hydrocarbon recovered to about 130% of the hydrocarbon recovered, adding sulfur or hydrogen sulfide or neither, said hydrogen sulfide being added, on space time velocity basis, from about 10 to about 30 ml/min/liter, said reaction being at a temperature between 50° C. and up to 450° C. at a pressure from subatmospheric to about 5 atm., and recovering volatile liquid distillates and hydrocarbon gases as hydrocarbon values.

Claim 5

A process for conversion of coal to gaseous hydrocarbons and volatile distillates comprising the steps of: reacting coal or peat and an alkali metal hydrosulfide, a sulfide, a polysulfide, hydrates thereof, or mixtures thereof, at a temperature of 50° C. and above, at a pressure from subatmospheric to about 5 atm., in the presence of water, such that the amount of water used is from about six to about seven moles per three moles of carbon in said coal, or in the presence of water and hydrogen sulfide, said hydrogen sulfide being added, on a space time velocity basis, from about 10 to about 30 ml/min/liter, continuing said reaction at a temperature up to about 425° C. and recovering volatile liquid distillates and hydrocarbon gases as hydrocarbon values.

Claim 6

A process for conversion of coal to gaseous hydrocarbons and volatile distillates comprising the steps of: reacting coal or peat and an alkali metal hydrosulfide, a sulfide, a polysulfide, hydrates thereof, or mixtures thereof, at a temperature of 50° C. and above, at a pressure from subatmospheric to about 5 atm., in the presence of water, such that the amount of water used is from about six to about seven moles per three moles of carbon in said coal, or in the presence of water and hydrogen sulfide, said hydrogen sulfide being added, on a space time velocity basis, from about 10 to about 30 ml/min/liter, continuing said reaction at a temperature up to about 425° C. and recovering volatile liquid distillates and hydrocarbon gases as hydrocarbon values.

Claim 7

The process as defined in claim 3, wherein elemental sulfur is added to an alkanolic solution of said alkali metal hydrosulfide used as a reagent.

Claim 8

The process as defined in claim 3, wherein said alkali metal hydrosulfide is potassium hydrosulfide.

Claim 9

The process as defined in claim 3, wherein said alkali metal hydrosulfide is sodium hydrosulfide.

Claim 10

The process as defined in claim 3, wherein said alkali metal sulfide is a mixture of rubidium, potassium, and sodium hydrosulfides and sulfides.

Claim 11

A process for conversion of coal to gaseous hydrocarbons and volatile distillates comprising the steps: reacting coal or peat having oxygen, sulfur or nitrogen present in bound form with an alkali metal hydrosulfide, sulfide or polysulfide or mixtures of same or of mixed alkali metals thereof, as a reagent; said reaction being conducted at a pressure from subatmospheric to about 5 atm. between the temperatures of 50° C. to 450° C. in presence of water or steam or steam and hydrogen sulfide, said water or steam being added being in relationship to the amount of hydrocarbon recovered and being from about the amount equivalent to about 130% in excess of the amount of hydrocarbon values recovered; recovering volatile distillates or gaseous hydrocarbons as hydrocarbon values, and reconstituting said reagent.

Claim 12

A process for conversion of coal to gaseous hydrocarbons and volatile distillates comprising the steps: reacting coal or peat having oxygen, sulfur or nitrogen present in bound form with an alkali metal hydrosulfide, sulfide or polysulfide or mixtures of same or of mixed alkali metals thereof, as a reagent; said reaction being conducted at a pressure from subatmospheric to about 5 atm. between the temperatures of 50° C. to 450° C. in presence of water or steam or steam and hydrogen sulfide, said water or steam being added being in relationship to the amount of hydrocarbon recovered and being from about the amount equivalent to about 130% in excess of the amount of hydrocarbon values recovered; recovering volatile distillates or gaseous hydrocarbons as hydrocarbon values, and reconstituting said reagent.

Claim 13

The process as defined in claim 8, wherein hydrogen sulfide is recovered.

Claim 14

The process as defined in claim 8, wherein the coal is lignite coal.

Claim 15

The process as defined in claim 8, wherein the coal is sub-lignite.

Claim 16

The process as defined in claim 8, wherein the coal is bituminous or sub-bituminous coal.

Claim 17

The process as defined in claim 8, wherein peat is reacted.

Claim 18

The process as defined in claim 8, wherein the alkali metal is potassium.

Claim 19

The process as defined in claim 8, wherein the hydrosulfide, sulfide, or polysulfide is of an alkali metal mixture of rubidium, potassium, and sodium.

Claim 20

The process as defined in claim 8, wherein the alkali metal is sodium.

Claim 21

The process as defined in claim 8, wherein part of the distillate is returned as an alcoholic solution to take part in the reaction of coal or peat and said reagent.

Claim 22

The process as defined in claim 8, wherein the reaction is conducted at a temperature between 135° C. and 450° C.

Claim 23

The process as defined in claim 17, wherein the reaction is conducted at a temperature between 170° C. and 380° C.

Claim 24

A continuous process for conversion of carbonaceous values in coal or peat and the like to gaseous hydrocarbons and volatile distillates comprising the steps of: introducing continuously into a reaction zone, maintained above 50° C. and up to 450° C., at a pressure from subatmospheric to about 5 atm., said carbonaceous values as coal or peat; introducing continuously, as a reagent, a hydrosulfide, a sulfide or polysulfide of an alkali metal or hydrates thereof, a mixture of alkali metal sulfides, or mixtures of hydrosulfides, sulfides and polysulfides thereof as said reagent; introducing water or steam in said reaction zone for hydrogenation of coal or peat at a temperature between 160° C. and up to 450° C. at a rate dependent upon the preselected end product cut desired; reacting continuously said carbonaceous values in coal or peat and said reagent in said zone at a predetermined temperature in the presence of said introduced water or steam to hydrogenate said carbonaceous values; recovering volatile and/or gaseous products from said reaction zone as hydrocarbon values; recovering hydrogen sulfide or carbonyl sulfide from said reaction zone; recovering residues including coal or peat ash from said reaction zone; recovering unreacted reagent or converting residues from said coal or peat including alkali metal values as alkali metal hydroxide from said residues; reacting said alkali metal hydroxides with hydrogen sulfide given off during said reaction and reconstituting said reagent, and introducing a sufficient amount of said reconstituted reagent in said reaction zone so as to continue said hydrogenation reaction of said carbonaceous material and said reagent.

Claim 25

A continuous process for conversion of carbonaceous values in coal or peat and the like to gaseous hydrocarbons and volatile distillates comprising the steps of: introducing continuously into a reaction zone, maintained above 50° C. and up to 450° C., at a pressure from subatmospheric to about 5 atm., said carbonaceous values as coal or peat; introducing continuously, as a reagent, a hydrosulfide, a sulfide or polysulfide of an alkali metal or hydrates thereof, a mixture of alkali metal sulfides, or mixtures of hydrosulfides, sulfides and polysulfides thereof as said reagent; introducing water or steam in said reaction zone for hydrogenation of coal or peat at a temperature between 160° C. and up to 450° C. at a rate dependent upon the preselected end product cut desired; reacting continuously said carbonaceous values in coal or peat and said reagent in said zone at a predetermined temperature in the presence of said introduced water or steam to hydrogenate said carbonaceous values; recovering volatile and/or gaseous products from said reaction zone as hydrocarbon values; recovering hydrogen sulfide or carbonyl sulfide from said reaction zone; recovering residues including coal or peat ash from said reaction zone; recovering unreacted reagent or converting residues from said coal or peat including alkali metal values as alkali metal hydroxide from said residues; reacting said alkali metal hydroxides with hydrogen sulfide given off during said reaction and reconstituting said reagent, and introducing a sufficient amount of said reconstituted reagent in said reaction zone so as to continue said hydrogenation reaction of said carbonaceous material and said reagent.

Claim 26

The process as defined in claim 20, wherein said carbonaceous material is wood.

Claim 27

The process as defined in claim 20, wherein the reaction zone is maintained at a set, predetermined temperature for production of gaseous hydrocarbons.

Claim 28

The process as defined in claim 20, wherein the reaction zone is maintained at a temperature suitable for recovery of a predetermined hydrocarbon cut.

Claim 29

The process as defined in claim 20, wherein an alcohol solution containing a portion of said dissolved distillate is recycled to said reaction zone.

Claim 30

The process as defined in claim 20, wherein lignite coal is the coal being reacted.

Claim 31

The process as defined in claim 20, wherein potassium sulfide, potassium polysulfide, potassium hydrosulfide or a mixture of same is used as a reagent.

Claim 32

The process as defined in claim 20, wherein the temperature in said reaction zone is between 135° C. to 450° C.

Claim 33

The process as defined in claim 20, wherein the temperature in said reaction zone is in stages between 170° C. to 450° C.

Claim 34

The process as defined in claim 20, wherein a mixture of rubidium, potassium, and sodium polysulfides, sulfides, hydrosulfides, or mixtures thereof is used as the reagent.

Claim 35

The process as defined in claim 20, wherein industrial sodium hydrosulfide as the reagent.

Claim 36

The process as defined in claim 20, wherein the reagent is resonstituted by reacting an alkali metal hydroxide in a saturated alcoholic solution with hydrogen sulfide, precipitating said reagent as a mixture of a sulfide and hydrosulfide of said alkali metal and recovering said precipitate as a reagent for reacting the same with said coal or peat or gaseous products thereof.

Claim 37

The process as defined in claim 20, wherein sad hydrocarbon products are distilled for recovery of a desired product cut.

Claim 38

The process as defined in claim 20, wherein said hydrocarbon product, in liquid or gaseous form, is treated in separate stages with said alkali reagent with increasing sulfur content of said reagent at discrete and decreasing temperature ranges below 400° C. but at a temperature above 100° C.

Claim 39

The process as defined in claim 33, wherein the gaseous hydrocarbon is scrubbed in an alkali metal hydroxide solution thereby removing hydrogen sulfide from said gaseous hydrocarbon as a reaction product with said alkali metal and further recovering said reagent for recycle of same.

Claim 40

The process as defined in claim 20, wherein, as said reagent there is used a theoretical composition K 2 S 3 , on basis of material balance.

Claim 41

The process as defined in claim 20, wherein anthracite coal or oxidized anthracite coal is reacted with said reagent.

Claim 42

A process for converting coal to hydrocarbon distillates, comprising contacting said coal with a reagent comprising of alkali metal sulfides, hydrosulfides, polysulfides, hydrates thereof or mixtures thereof, heating the resulting system to above 100° C., at ambient pressure, passing steam through said system in the absence of extrinsic air at temperatures between 100° C. and 450° C., recovering a hydrocarbon distillate consisting of both saturated and unsaturated hydrocarbons having a carbon content between one and six and hydrogen and leaving behind an inorganic residue.

Claim 43

A process for converting coal to hydrocarbon distillates, comprising contacting said coal with a reagent comprising of alkali metal sulfides, hydrosulfides, polysulfides, hydrates thereof or mixtures thereof, heating the resulting system to above 100° C., at ambient pressure, passing steam through said system in the absence of extrinsic air at temperatures between 100° C. and 450° C., recovering a hydrocarbon distillate consisting of both saturated and unsaturated hydrocarbons having a carbon content between one and six and hydrogen and leaving behind an inorganic residue.

Claim 44

The process of claim 37, comprising using potassium hydrosulfide and potassium pentasulfide, said hydrosulfide being present in at least a stoichiometrically equal amount to said potassium pentasulfide, the sulfur content of said potassium pentasulfide being above that of the monosulfide ion and at least numerically equal on an atom number basis to the total number of oxygen, sulfur and nitrogen atoms present in said coal.

Claim 45

The process of claim 37, wherein the alkali metal sulfide is potassium sulfide and the alkali metal polysulfide is potassium pentasulfide and wherein the number of sulfur atoms in the potassium pentasulfide above that of the potassium monosulfide ion is at least numerically equal to the number of atoms of oxygen, sulfur and nitrogen in said coal.

Claim 46

The process of claim 38, wherein said potassium monosulfide is present in an amount at least stoichiometrically equal to said potassium pentasulfide.

Claim 47

The process of claim 37, wherein the alkali metal hydrosulfide is sodium hydrosulfide and the alkali metal polysulfide is sodium tetrasulfide and wherein the number of sulfur atoms in the sodium tetrasulfide above those of the sodium monosulfide ion is at least numerically equal to the number of atoms of oxygen, sulfur and nitrogen in said coal on a dry ashless basis and wherein the sodium hydrosulfide is present in at least stoichiometric equality with the sodium tetrasulfide present.

Claim 48

The process of claim 37, wherein the coal is lignite, sub-bituminous coal, low rank bituminous coal or oxidized higher rank coal.

Claim 49

The process of claim 37, wherein hydrogen sulfide is removed with an ethanol or methanol solution of an alkali metal hydroxide to constitute fresh reagent.

Claim 50

The process of claim 37, comprising using a mixture of potassium hydrosulfide and potassium pentasulfide in an alkanol.

Claim 51

The process of claim 37, wherein said steam is introduced after the temperature of the coal and reagent is above 100° C.

Claim 52

The process of claim 37, wherein the reagent consists of alkali metal hydrosulfide, alkali metal sulfides, and alkali metal polysulfides.

Claim 53

The process of claim 37, wherein the reagent consists of alkali metal hydrosulfides.

Claim 54

The process of claim 37, wherein the reagent consists of alkali metal sulfides.

Claim 55

The process of claim 37, wherein the reagent consists of alkali metal polysulfides.

Claim 56

The process of claim 37, wherein the reagent is alkali metal polysulfides and alkali metal monosulfides in which the said polysulfides are present in a quantity which is not greater than stoichiometrically equal to the monosulfides.

Claim 57

The process of claim 37, wherein said temperature is between 100° C. and 400° C.