Process for autothermal generation of hydrogen
원문보기
IPC분류정보
국가/구분
United States(US) Patent
등록
국제특허분류(IPC7판)
C01B-003/26
C01B-003/00
출원번호
US-0165731
(2005-06-24)
등록번호
US-7429373
(2008-09-30)
발명자
/ 주소
Pez,Guido Peter
Quinn,Robert
Nataraj,Shankar
출원인 / 주소
Air Products and Chemicals, Inc.
대리인 / 주소
Gourley,Keith D.
인용정보
피인용 횟수 :
5인용 특허 :
12
초록▼
Process for producing hydrogen comprising reacting at least one hydrocarbon and steam in the presence of a complex metal oxide and a steam-hydrocarbon reforming catalyst in a production step under reaction conditions sufficient to form hydrogen gas and a spent complex metal oxide, wherein the comple
Process for producing hydrogen comprising reacting at least one hydrocarbon and steam in the presence of a complex metal oxide and a steam-hydrocarbon reforming catalyst in a production step under reaction conditions sufficient to form hydrogen gas and a spent complex metal oxide, wherein the complex metal oxide is represented by the formula description="In-line Formulae" end="lead"AxByOn description="In-line Formulae" end="tail" wherein A represents at least one metallic element having an oxidation state ranging from +1 to +3, inclusive, wherein the metallic element is capable of forming a metal carbonate; x is a number from 1 to 10, inclusive; B represents at least one metallic element having an oxidation state ranging from +1 to +7, inclusive; y is a number from 1 to 10, inclusive; and n represents a value such that the complex metal oxide is rendered electrically neutral.
대표청구항▼
The invention claimed is: 1. A process for producing hydrogen in a reactor comprising: reacting at least one hydrocarbon and steam in the presence of a complex metal oxide and a steam-hydrocarbon reforming catalyst in a production step under reaction conditions sufficient to form hydrogen gas, a me
The invention claimed is: 1. A process for producing hydrogen in a reactor comprising: reacting at least one hydrocarbon and steam in the presence of a complex metal oxide and a steam-hydrocarbon reforming catalyst in a production step under reaction conditions sufficient to form hydrogen gas, a metal carbonate and a reduced metal oxide; and reacting the reduced metal oxide, the metal carbonate and an oxygen source gas in a regeneration step under reaction conditions sufficient to oxidize the metal oxide, release carbon dioxide, and regenerate the complex metal oxide, wherein the complex metal oxide is represented by the formula description="In-line Formulae" end="lead"AxByOn description="In-line Formulae" end="tail" wherein A represents at least one metallic element having an oxidation state ranging from +1 to +3, inclusive, wherein the metallic element is capable of forming the metal carbonate; x is a number from 1 to 10, inclusive; B represents at least one metallic element having an oxidation state ranging from +1 to +7, inclusive; y is a number from 1 to 10, inclusive; and n represents a value such that the complex metal oxide is rendered electrically neutral. 2. The process of claim 1 further comprising purging the reactor with a purge gas to displace combustible components from the reactor and withdrawing a purge gas effluent therefrom prior to the regeneration step. 3. The process of claim 1 wherein A in the complex metal oxide represents at least one metallic element selected from the group consisting of elements of Groups 1, 2, and 3, and the Lanthanide elements of the IUPAC Periodic Table of the Elements; and B represents at least one metallic element selected from the group consisting of elements of Groups 4 to 15 of the IUPAC Periodic Table of the Elements. 4. The process of claim 1 wherein B in the complex metal oxide is selected from the group consisting of vanadium, chromium, manganese, iron, cobalt, copper, nickel, and mixtures thereof. 5. The process of claim 1 wherein the production step is characterized by a production temperature in the range of 350�� C. to 900�� C. and a production pressure ranging from 1 to 100 atmospheres. 6. The process of claim 1 wherein the molar ratio of steam to the at least one hydrocarbon ranges from 1:1 to 20:1. 7. The process of claim 1 wherein the molar ratio of steam to the at least one hydrocarbon in the feed gas during the production step is less than 150% of the theoretical amount. 8. The process of claim 2 wherein the regeneration step is characterized by a regeneration temperature in the range of 450�� C. to 900�� C. 9. The process of claim 2 wherein the production step is characterized by a production temperature and the regeneration step is characterized by a regeneration temperature, wherein the regeneration temperature is greater than the production temperature and wherein difference between the regeneration temperature and the production temperature is 100�� C. or less. 10. The process of claim 1 wherein the steam-hydrocarbon reforming catalyst contains one or more components selected from the group consisting of nickel, cobalt, ruthenium, osmium, rhodium, palladium, platinum, iridium, and oxides of the foregoing metals, and a catalyst support. 11. The process of claim 1 wherein the at least one hydrocarbon is selected from the group consisting of aliphatic hydrocarbons having from 1 to 20 carbon atoms. 12. The process of claim 11 wherein the at least one hydrocarbon is methane obtained as a component of natural gas. 13. The process of claim 12 wherein the molar ratio of steam to methane ranges from 1.3:1 to 4:1, inclusive. 14. The process of claim 11 wherein the yield of hydrogen produced per mole of the at least one hydrocarbon consumed is within ��10% of the maximum yield of hydrogen that can be realized at thermoneutral conditions. 15. The process of claim 2 where the regeneration step is carried out at a pressure lower than the pressure of the production step. 16. A process for producing hydrogen comprising (a) providing a reactor containing a complex metal oxide and a steam-hydrocarbon reforming catalyst, wherein the complex metal oxide is represented by the formula: description="In-line Formulae" end="lead"AxByOn description="In-line Formulae" end="tail" wherein A represents at least one metallic element having an oxidation state ranging from +1 to +3, inclusive, wherein such metallic element is capable of forming a metal carbonate; x is a number from 1 to 10, inclusive; B represents at least one metallic element having an oxidation state ranging from +1 to +7, inclusive; y is a number from 1 to 10; inclusive and n represents a value such that the complex metal oxide is rendered electrically neutral; (b) introducing a feed gas containing at least one hydrocarbon and steam into the reactor in a production step, reacting the at least one hydrocarbon and the steam in the presence of the complex metal oxide and the steam-hydrocarbon reforming catalyst under reaction conditions sufficient to form hydrogen, a metal carbonate and a reduced metal oxide, and withdrawing from the reactor a product gas comprising hydrogen; (c) terminating the introduction of the at least one hydrocarbon and optionally purging the reactor with a purge gas to displace combustible components from the reactor and withdrawing a purge gas effluent therefrom; (d) regenerating the reactor in a regeneration step by reacting the reduced metal oxide, the metal carbonate and an oxygen source gas under reaction conditions sufficient to regenerate the complex metal oxide; (e) optionally purging the reactor with a purge gas; (f) pressurizing the reactor by introducing a pressurizing gas into the reactor at pressure; and (g) repeating (b) through (f) in a cyclic manner. 17. The process of claim 16 wherein the pressurizing gas is obtained from the group consisting of hot reactor feed, hot reactor effluent, steam, feed to a pressure swing adsorption system, and product gas. 18. The process of claim 16 that further comprises, prior to purging the reactor in (c), depressurizing the reactor by withdrawing a depressurization gas therefrom. 19. The process of claim 16 wherein the feed gas contains up to 25 vol % hydrogen. 20. The process of claim 19 wherein the feed gas is pre-reformed natural gas. 21. The process of claim 16 that further comprises cooling the product gas and removing non-hydrogen components therefrom in a pressure swing adsorption process to yield a high-purity hydrogen product comprising at least 99 vol % hydrogen. 22. The process of claim 16 that further comprises providing at least one additional reactor containing the complex metal oxide and the steam-hydrocarbon reforming catalyst, and operating the at least one additional reactor by carrying out steps (b) through (f) such that each of the reactors proceeds through the production step (b) during a different time period. 23. The process of claim 16 wherein a portion of the product gas from the production step is retained and is introduced into the reactor with the feed gas in a succeeding production step. 24. The process of claim 16 wherein the purge gas is selected from the group consisting of steam, nitrogen, and a mixture thereof. 25. The process of claim 16 wherein the feed gas comprises methane and the yield of hydrogen produced per mole of methane consumed is within ��10% of the maximum yield of hydrogen that can be realized at thermoneutral conditions.
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이 특허에 인용된 특허 (12)
Cole Jerald A., Autothermal methods and systems for fuels conversion.
Sioui, Daniel R.; Towler, Gavin P.; Oroskar, Anil R.; Zhou, Lubo; Dunne, Stephen R.; Kulprathipanja, Santi; Galperin, Leonid B.; Modica, Frank S.; Voskoboinikov, Timur V., Hydrogen generation via methane cracking for integrated heat and electricity production using a fuel cell.
Richter Ekkehard (Essen DEX) Krbacher Werner (Mlheim DEX) Knoblauch Karl (Essen DEX) Giessler Klaus (Gelsenkirchen DEX) Harder Klaus-Burkhard (Oberhausen DEX), Method of separating highly adsorbable components in a gas stream in a pressure-sensing adsorber system.
McCarron ; III Eugene M. (Greenville DE) Parise John B. (East Setauket NY), Process for preparation of metal oxides of molybdenum or mlybdenum and tungsten.
Garg, Diwakar; Quinn, Robert; Wilhelm, Frederick Carl; Alptekin, Gokhan; Dubovik, Margarita; Schaefer, Matthew, Hydrogen production using complex metal oxide pellets.
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