EP2167423A1 - Production of hydrogen gas from sulfur-containing compounds - Google Patents
Production of hydrogen gas from sulfur-containing compoundsInfo
- Publication number
- EP2167423A1 EP2167423A1 EP08768528A EP08768528A EP2167423A1 EP 2167423 A1 EP2167423 A1 EP 2167423A1 EP 08768528 A EP08768528 A EP 08768528A EP 08768528 A EP08768528 A EP 08768528A EP 2167423 A1 EP2167423 A1 EP 2167423A1
- Authority
- EP
- European Patent Office
- Prior art keywords
- stream
- water
- gas
- sulfuric acid
- sulfur
- Prior art date
- Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
- Withdrawn
Links
Classifications
-
- C—CHEMISTRY; METALLURGY
- C25—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES; APPARATUS THEREFOR
- C25B—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES FOR THE PRODUCTION OF COMPOUNDS OR NON-METALS; APPARATUS THEREFOR
- C25B1/00—Electrolytic production of inorganic compounds or non-metals
- C25B1/01—Products
- C25B1/02—Hydrogen or oxygen
-
- C—CHEMISTRY; METALLURGY
- C01—INORGANIC CHEMISTRY
- C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
- C01B17/00—Sulfur; Compounds thereof
- C01B17/48—Sulfur dioxide; Sulfurous acid
- C01B17/50—Preparation of sulfur dioxide
- C01B17/508—Preparation of sulfur dioxide by oxidation of sulfur compounds
-
- C—CHEMISTRY; METALLURGY
- C01—INORGANIC CHEMISTRY
- C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
- C01B17/00—Sulfur; Compounds thereof
- C01B17/48—Sulfur dioxide; Sulfurous acid
- C01B17/50—Preparation of sulfur dioxide
- C01B17/54—Preparation of sulfur dioxide by burning elemental sulfur
-
- C—CHEMISTRY; METALLURGY
- C01—INORGANIC CHEMISTRY
- C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
- C01B17/00—Sulfur; Compounds thereof
- C01B17/69—Sulfur trioxide; Sulfuric acid
- C01B17/74—Preparation
-
- C—CHEMISTRY; METALLURGY
- C25—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES; APPARATUS THEREFOR
- C25B—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES FOR THE PRODUCTION OF COMPOUNDS OR NON-METALS; APPARATUS THEREFOR
- C25B1/00—Electrolytic production of inorganic compounds or non-metals
- C25B1/01—Products
- C25B1/22—Inorganic acids
Definitions
- This invention relates to the preparation of hydrogen gas using electrolytic processing of sulfurous acid.
- Hydrogen (H 2 ) is a valuable feedstock in refineries for an assortment of hydrogenation processes. Hydrogen is also seeing greater value as a fuel source, both in direct combustion and in fuel cells. Public discussions addressing the reduction of carbon dioxide (CO 2 ) emissions often refer to an alternative of a "hydrogen economy.” Thus, methods for the economic generation and recovery of hydrogen while avoiding or reducing the co-production of CO 2 are currently of interest.
- H 2 S hydrogen sulfide
- Many of the processes for generating hydrogen from H 2 S suffer from problems associated with the co-generation of elemental sulfur. While elemental sulfur is a relatively benign solid at ambient conditions, it can be a problem in terms of disposal. Most sulfur is used in the formation of sulfuric acid, an important industrial product. However, local markets may be saturated with sulfur, and long term storage of solid, block sulfur is undesirable.
- U.S. patent 5,843,395 teaches the thermal disassociation of H 2 S containing waste gas at about 1,000 0 C to about 1,900 0 C to provide hydrogen and sulfur, the hydrogen taken off by membrane separation. Any waste heat is used to pre-heat the waste gas prior to the dissociation step.
- U.S. patent 4,836,992 teaches the use of an electrolytic cell to make H 2 from H 2 SO 3 , made from mixing SO 2 with NaOH, NaSO 3 or H 2 SO 4 , thus yielding by-products Of H 2 SO 4 and NaOH upon the electrolytic conversion. The SO 2 is provided from the burning of waste gases.
- patent 4,519,881 teaches the use of a three-chamber electrolytic cell to regenerate sodium hydroxide from caustic solutions containing sulfides.
- the process produces hydrogen sulfide by the electrolysis of sodium sulfide and hydrogen ions and also produces hydrogen.
- the process is not compatible with a natural gas stream and does not generate hydrogen gas directly from the sulfurous acid solution.
- the described and claimed invention is a process for producing hydrogen gas comprising (a) combusting sulfur (S) or hydrogen sulfide (H 2 S) with oxygen (O 2 ) to obtain sulfur dioxide (SO 2 ) and water (H 2 O), plus heat; (b) adding water to the product of (a) to obtain a sulfurous acid solution (H 2 SO 3 and H 2 O); (c) applying electrical current to the sulfurous acid solution of (b) to obtain sulfuric acid (H 2 SO 4 ) and hydrogen gas (H 2 ); and, (d) separating the sulfuric acid from the hydrogen gas to obtain separated components of the sulfuric acid and the hydrogen gas, wherein the heat generated in (a) is used to generate at least a portion of the electricity for the electrical current for (c).
- the oxygen in (a) is provided at least in part by the introduction of air, e.g., by providing an air stream into the combustion reaction.
- Oxygen for combustion can be generated from a cryogenic air separation unit (ASU), or from a membrane process, or from a pressure-swing adsorption unit, all of which reduce the nitrogen content of the gas to be processed.
- the SO 2 can be captured in a relatively pure form by using a liquid solvent, such as a diamine, applied to various flue sources containing the SO 2 , for example from combusting acid gas, disulfide oil, or coal, which will all contain CO 2 .
- the sulfur or hydrogen sulfide is provided in (a) by the introduction of combustible compositions, gaseous, liquid or solid, which compositions contain sulfur and/or hydrogen sulfide.
- combustible compositions gaseous, liquid or solid, which compositions contain sulfur and/or hydrogen sulfide.
- examples include "sour natural gas", acid gas from petroleum and natural gas recovery, sulfur-laden heavy oil and bitumen, and one or more of hard or soft coal and coke products.
- a system for producing hydrogen gas includes: a) an acid gas stream containing hydrogen sulfide; b)an air stream; c) a burner configured to burn the acid gas stream and air stream and produce a product stream having at least sulfur dioxide, water, and heat; d) a boiler unit operatively connected to the product stream of the burner and configured to capture heat from the burner, and generate at least a steam stream and an exhaust gas stream having at least SO 2 ; e) an SO 2 separation unit operatively connected to the exhaust gas stream of the boiler unit and configured to remove SO 2 from the exhaust gas stream and generate an SO 2 exit stream; and f) an electrolytic cell operatively connected to the SO 2 exit stream and configured to produce hydrogen gas (H 2 ).
- FIG. 1 presents a block diagram of one embodiment of the invention process for converting hydrogen sulfide and/or elemental sulfur into hydrogen and sulfuric acid.
- the invention described and claimed below comprises a combination of hydrogen sulfide (H 2 S), or elemental sulfur (S), combustion, electricity generation from recycled heat, and electrolytic processing of sulfurous acid (H 2 SO 3 ) to generate hydrogen and sulfuric acid with little CO 2 (or SO 2 ) being emitted.
- H 2 S hydrogen sulfide
- S elemental sulfur
- SO 3 sulfurous acid
- the required SO 2 can be generated from a number of one-pass processes.
- elemental sulfur can be captured from a Claus sulfur recovery process, wherein SO 2 is combined with H 2 S in a molar ratio of 1 :2 to generate approximately 3 moles of elemental sulfur and 2 moles of water. Since the Claus reaction does not typically go to completion, remaining H 2 S and SO 2 must be handled in a "tail gas treating unit" where the remaining gases are captured for further treatment, i.e., combusted in accordance with the invention. Alternatively, the tail gas could be combusted to convert all sulfur-containing compounds to SO 2 , while capturing the SO 2 in a special solvent, as described in WO-A-2006/016979. Another example is the combustion of sulfur-containing coal, or bitumen that generates SO 2 .
- Disulfide oils, mercaptans, etc. which can be separated from liquid hydrocarbons using caustic processes, may also be considered as combustible feed for this process.
- the ready availability of sulfur and/or hydrogen sulfide, plus oxygen, enables an efficient process for producing both sulfuric acid and hydrogen.
- the hydrogen gas can be cycled for use in hydrogenation processes or transported and/or packaged for sale and used for developing fuel processes using hydrogen.
- the sulfuric acid by-product is a commodity product that can be recycled or sold for further use, e.g., chemical process use, or it can be readily disposed of in saline aquifers generally available where sulfur-containing natural gas is recovered. Since the sulfuric acid is a liquid, it is amenable to downhole disposal, whereas solid elemental sulfur must be kept in stockpiles on the surface, or buried at some effort and expense. [0015] In one possible embodiment, relatively pure H 2 S is combusted in oxygen according to:
- the heat generated by these reactions can be used to produce steam, which then can be used to generate electricity for step (c) in the process.
- the SO 2 -containing stream is then quenched with water to generate a sulfurous acid solution:
- FIG. 1 An example heat and material balance for the process of FIG. 1 follows. This illustrative example starts with 1000 kg-mol/hr of acid gas containing 25% H 2 S, equating to 189 long tons/day (192x10 3 kg/day) of elemental sulfur. The case assumes that 2% of the H 2 S combusted is immediately converted to SO 3 , and must be purged out ahead of the separation unit.
- Heat is recovered in the waste heat boiler at 600°F (315.6°C), well above the dewpoint of the SO 3 /H 2 SO 4 present. Ninety-five percent heat recovery and 30% efficient conversion to electricity are assumed. Adequate heat is recovered to regenerate the scrubbing solvent, plus generate enough electricity for the electrolysis. Surplus heat can be used for additional steam or electricity.
- acid gas 1 containing hydrogen sulfide at 250.0 kgmols/hr, carbon dioxide at 705.0 kgmols/hr, water in the form of moisture in an amount of 45.0 kgmol/hr, air 2 containing oxygen in amount of 426.8 kgmols/hr, nitrogen in an amount at 1740.2 kgmols/hr, and water in the form of moisture in an amount of 33.0 kgmols/hr is introduced into a burner, or combustion chamber 20.
- stream 3 After combustion, stream 3 comprises the nitrogen and carbon dioxide in the same amounts as in the feed gas (unreacted), with sulfur dioxide at 245 kgmols/hr, with 5.0 kgmols/hr sulfur trioxide, 328.0 kgmols/hr water, and 49.3 kgmols/hr oxygen.
- This hot, gaseous stream 3 is passed to a boiler unit 21 (i.e., heat exchanger) where 863.3 kgmol/hr water, comprising at least in part condensed steam from the electrical generator 24, is introduced via stream 13 to provide water for the boiler.
- a separate water stream (not shown) can be used to source the boiler.
- water is condensed from the combusted stream 3 to provide the water reagent for reaction (6).
- Stream 4 will generally be maintained at temperatures above the SO 3 dewpoint, to avoid condensation of corrosive sulfuric acid, H 2 SO 4 .
- the operating temperature may be as high as 600°F.
- Stream 4 is then quenched by contact with liquid water in a device such as a DynaWave scrubber from MECS, Inc., to reduce the temperature to 100-150 F. Reactive SO 3 and H 2 SO 4 dissolve in the aqueous quench stream.
- a small amount of this stream is purged from the system as a weak solution Of H 2 SO 4 in purge stream 15.
- the balance of the stream is cooled, and recycled to the scrubbing device.
- the cooled, H 2 SO 4 -free gas stream is then provided for separation where SO 2 is preferentially removed by absorbing it into an SO 2 - selective solvent in a gas-liquid contacting device 22a.
- SO 2 is preferentially removed by absorbing it into an SO 2 - selective solvent in a gas-liquid contacting device 22a.
- Cansolv Technologies, Inc. markets a diamine solvent that is selective for SO 2 over CO 2 and other combustion gases. Gases not absorbed into the solution (including trace SO 2 ) are vented through stream 5.
- the rich solution is then regenerated in a separate vessel, generally requiring steam (12) to heat the solvent to 250-300°F.
- the exit stream 6, cooled to 100-150°F, comprises 240.6 kgmols/hr SO 2 and flows from the regeneration unit 22b at 17-25 psia to the electrolytic cell 23 at near-atmospheric pressure.
- a portion of the steam (1,992.2 kgmols/hr) from the boiler unit 21 in exit stream 10 is diverted in stream 12 to the regeneration unit 22b to provide heat.
- stream 11 to the electricity generator comprises 862.3 kgmols/hr steam.
- Excess steam in an amount of 261.8 kgmols/hr water is removed from stream 12 via stream 16 prior to provision to the regeneration unit 22b.
- a separate stream 15 takes off 5.0 kgmols/hr H 2 SO 4 , 3.4 kgmols/hr SO 2 (as H 2 SO 3 ), and 25.0 kgmols/hr water from the scrubbing unit 22a. Unreacted and by-product gases are vented from the separation unit and removed in stream 5, this stream thus comprising all of the CO 2 , residual O 2 , and N 2 , plus 1.0 kgmol/hr SO 2 , and 328.0 kgmols/hr water vapor.
- Separate stream 14 returns 1,992.2 kgmols/hr water from the regenerator unit 22b as condensate to the boiler unit 21.
Landscapes
- Chemical & Material Sciences (AREA)
- Organic Chemistry (AREA)
- Inorganic Chemistry (AREA)
- Engineering & Computer Science (AREA)
- Chemical Kinetics & Catalysis (AREA)
- Electrochemistry (AREA)
- Materials Engineering (AREA)
- Metallurgy (AREA)
- Electrolytic Production Of Non-Metals, Compounds, Apparatuses Therefor (AREA)
Abstract
Description
Claims
Applications Claiming Priority (2)
Application Number | Priority Date | Filing Date | Title |
---|---|---|---|
US96163907P | 2007-07-23 | 2007-07-23 | |
PCT/US2008/007524 WO2009014584A1 (en) | 2007-07-23 | 2008-06-17 | Production of hydrogen gas from sulfur-containing compounds |
Publications (2)
Publication Number | Publication Date |
---|---|
EP2167423A1 true EP2167423A1 (en) | 2010-03-31 |
EP2167423A4 EP2167423A4 (en) | 2011-11-09 |
Family
ID=38910941
Family Applications (1)
Application Number | Title | Priority Date | Filing Date |
---|---|---|---|
EP08768528A Withdrawn EP2167423A4 (en) | 2007-07-23 | 2008-06-17 | Production of hydrogen gas from sulfur-containing compounds |
Country Status (5)
Country | Link |
---|---|
US (1) | US20100230296A1 (en) |
EP (1) | EP2167423A4 (en) |
AU (1) | AU2008279815A1 (en) |
CA (1) | CA2689461A1 (en) |
WO (1) | WO2009014584A1 (en) |
Families Citing this family (8)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
DE102011002320B3 (en) | 2011-04-28 | 2012-06-21 | Knauf Gips Kg | Method and device for generating electricity from hydrogen sulfide-containing exhaust gases |
WO2013098329A1 (en) * | 2011-12-27 | 2013-07-04 | Shell Internationale Research Maatschappij B.V. | Method for producing sulphuric acid |
US9644840B2 (en) * | 2012-09-20 | 2017-05-09 | General Electric Technology Gmbh | Method and device for cleaning an industrial waste gas comprising CO2 |
US10066834B2 (en) | 2013-01-30 | 2018-09-04 | Bogdan Wojak | Sulphur-assisted carbon capture and storage (CCS) processes and systems |
US20180119293A1 (en) * | 2016-10-30 | 2018-05-03 | Tolulope Israel Mayomi | Salt cycle for hydrogen production |
CN109539280B (en) * | 2019-01-09 | 2024-02-09 | 大连昊通节能环保工程技术有限公司 | Ammonia desulfurization waste liquid heat accumulating type incineration SO preparation 2 Process gas technology and system |
CN113277639A (en) * | 2021-03-31 | 2021-08-20 | 李晟贤 | Test gas sewage treatment method |
WO2023187781A1 (en) * | 2022-03-31 | 2023-10-05 | Hys Energy Ltd | Hydrogen production by electrochemical decomposition of saline water using sulfur dioxide or bisulfite as an anode depolarizer |
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2008
- 2008-06-17 AU AU2008279815A patent/AU2008279815A1/en not_active Abandoned
- 2008-06-17 US US12/599,857 patent/US20100230296A1/en not_active Abandoned
- 2008-06-17 EP EP08768528A patent/EP2167423A4/en not_active Withdrawn
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- 2008-06-17 CA CA002689461A patent/CA2689461A1/en not_active Abandoned
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See also references of WO2009014584A1 * |
Also Published As
Publication number | Publication date |
---|---|
CA2689461A1 (en) | 2009-01-29 |
EP2167423A4 (en) | 2011-11-09 |
WO2009014584A1 (en) | 2009-01-29 |
AU2008279815A1 (en) | 2009-01-29 |
US20100230296A1 (en) | 2010-09-16 |
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