Process for Producing Hydrogen from Hydrocarbons

Abstract

A process for producing hydrogen from a hydrocarbon gas comprising contacting at elevated temperature the hydrocarbon gas with a catalyst to catalytically convert the hydrocarbon gas to hydrogen and solid carbon; wherein, the catalyst comprises one or both of the following: (a) a calcined Fe-containing catalyst; or (b) a bimetallic M x Ni y -type catalyst supported on a substrate.

1 . A process for producing hydrogen from a hydrocarbon gas comprising contacting at elevated temperature the hydrocarbon gas with a catalyst to catalytically convert the hydrocarbon gas to hydrogen and solid carbon;
 wherein the catalyst comprises one or both of the following:   (a) a calcined Fe-containing catalyst; or   (b) a bimetallic M x Ni y -type catalyst supported on a substrate.   
     
     
         2 . The process according to  claim 1 , wherein the hydrocarbon gas is contacted with the calcined Fe-containing catalyst at a temperature in a temperature range of from 500° C. to 1200° C. 
     
     
         3 .- 4 . (canceled) 
     
     
         5 . The process according to  claim 1 , wherein the hydrocarbon gas may be contacted with the calcined Fe-containing catalyst at a pressure in a pressure range of from 1.75 bar to 10 bar. 
     
     
         6 . The process according to  claim 1 , wherein the Fe-containing catalyst may be selected from a group comprising stainless steel, carbon steel, rare earth doped stainless steel, low carbon stainless steel, and iron-containing metal alloys. 
     
     
         7 . The process according to  claim 1 , wherein the Fe-containing catalyst is an iron-containing metal alloy with a catalytic activator. 
     
     
         8 . The process according to  claim 7 , wherein the catalytic activator may be selected from a group consisting of nickel, molybdenum, ruthenium, tantalum, lanthanide metals, and titanium. 
     
     
         9 .- 10 . (canceled) 
     
     
         11 . The process according to  claim 1 , wherein prior to bringing the hydrocarbon gas into contact with the Fe-containing catalyst, said catalyst is calcined at a temperature greater than 700° C. for a period of from about one to two hours. 
     
     
         12 . The process according to  claim 11 , wherein after calcining, the calcined Fe-containing catalyst may be reduced at elevated temperatures. 
     
     
         13 . (canceled) 
     
     
         14 . The process according to  claim 12 , wherein the calcined Fe-containing catalyst may undergo reduction with methane contained in the hydrocarbon gas concurrently with the catalytic conversion of hydrocarbon gas into hydrogen and solid carbon. 
     
     
         15 .- 17 . (canceled) 
     
     
         18 . The process according to  claim 1 , wherein M is a transition metal or a lanthanide. 
     
     
         19 . The process according to  claim 18 , wherein M is Mo or La. 
     
     
         20 . The process according to  claim 19 , wherein the Mo x Ni y -type catalyst has a formula of Mo x Ni y Mg z O, wherein x=0.05-0.1, y=0.01-0.05, and z=0.4-0.5. 
     
     
         21 . The process according to  claim 19 , wherein the La x Ni y -type catalyst has a formula of La x Ni y Mg z O, wherein x=0.05-0.1, y=0.01-0.1, and z=0.8-0.9. 
     
     
         22 . (canceled) 
     
     
         23 . The process according to  claim 1 , wherein the substrate is mesh-like, filamentous, perforated or porous. 
     
     
         24 . (canceled) 
     
     
         25 . The process according to  claim 1 , wherein the substrate comprises a calcined Fe-containing catalyst. 
     
     
         26 . The process according to  claim 1 , wherein the hydrocarbon gas is catalytically converted to hydrogen and carbon by contacting the hydrocarbon gas with the supported bimetallic M x Ni y -type catalyst at a temperature of 400° C. to 950° C. 
     
     
         27 .- 30 . (canceled) 
     
     
         31 . The process according to  claim 1 , wherein there is negligible depletion of the bimetallic catalyst throughout the conversion process. 
     
     
         32 . The process according to  claim 1 , wherein the hydrocarbon gas is one or more chemical compounds that contain only carbon and hydrogen, having a carbon number of 6 or less. 
     
     
         33 . The process according to  claim 1 , wherein the hydrocarbon gas comprises methane. 
     
     
         34 . (canceled) 
     
     
         35 . The process according to  claim 1 , wherein the solid carbon is generated as graphitic particles. 
     
     
         36 . The process according to  claim 35 , wherein the graphitic particles are substantially spherical. 
     
     
         37 .- 39 . (canceled) 
     
     
         40 . The process according to  claim 36 , wherein the mean diameter of the spherical graphitic particles is 0.4-4 μm 
     
     
         41 . (canceled) 
     
     
         42 . A process for producing graphitic particles comprising contacting at elevated temperature hydrocarbon gas with a catalyst to catalytically convert the hydrocarbon gas to hydrogen and graphitic particles;
 wherein the catalyst comprises one or both of the following:   (a) a calcined Fe-containing catalyst; or   (b) a bimetallic M x Ni y -type catalyst supported on a substrate.   
     
     
         43 .- 45 . (canceled) 
     
     
         46 . The process according to  claim 42  further comprising the further step of thermally treating the recovered graphitic particles and converting any ambient amorphous carbon material to high quality graphite. 
     
     
         47 . A process for generating electricity from light hydrocarbons substantially in the absence of carbon dioxide emission, the process comprising the steps of:
 (i) contacting at an elevated temperature hydrocarbon gas with a catalyst to catalytically convert the hydrocarbon gas to hydrogen and solid carbon;   (ii) separating and recovering the hydrogen generated in step a);   (iii) using a first portion of recovered hydrogen in a fuel cell to generate electricity; and   (iv) combusting a second portion of recovered hydrogen to generate elevated temperature in step a);   wherein the catalyst comprises one or both of the following:
 (a) a calcined Fe-containing catalyst; or 
 (b) a bimetallic M x Ni y -type catalyst supported on a substrate. 
   
     
     
         48 .- 51 . (canceled)