US20150157979A1 - Methods and Systems for Synthesizing Iron-Based Materials and Sequestering Carbon Dioxide - Google Patents
Methods and Systems for Synthesizing Iron-Based Materials and Sequestering Carbon Dioxide Download PDFInfo
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- US20150157979A1 US20150157979A1 US14/621,438 US201514621438A US2015157979A1 US 20150157979 A1 US20150157979 A1 US 20150157979A1 US 201514621438 A US201514621438 A US 201514621438A US 2015157979 A1 US2015157979 A1 US 2015157979A1
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- CURLTUGMZLYLDI-UHFFFAOYSA-N Carbon dioxide Chemical compound O=C=O CURLTUGMZLYLDI-UHFFFAOYSA-N 0.000 title claims abstract description 91
- 238000000034 method Methods 0.000 title claims abstract description 56
- 229910002092 carbon dioxide Inorganic materials 0.000 title claims abstract description 53
- 239000001569 carbon dioxide Substances 0.000 title claims abstract description 36
- 239000000463 material Substances 0.000 title claims abstract description 16
- 230000014759 maintenance of location Effects 0.000 title claims abstract description 13
- 230000002194 synthesizing effect Effects 0.000 title 1
- XEEYBQQBJWHFJM-UHFFFAOYSA-N Iron Chemical compound [Fe] XEEYBQQBJWHFJM-UHFFFAOYSA-N 0.000 claims abstract description 130
- 229910052742 iron Inorganic materials 0.000 claims abstract description 62
- UQSXHKLRYXJYBZ-UHFFFAOYSA-N Iron oxide Chemical compound [Fe]=O UQSXHKLRYXJYBZ-UHFFFAOYSA-N 0.000 claims abstract description 48
- 239000000446 fuel Substances 0.000 claims abstract description 24
- 239000001257 hydrogen Substances 0.000 claims abstract description 22
- 229910052739 hydrogen Inorganic materials 0.000 claims abstract description 22
- UFHFLCQGNIYNRP-UHFFFAOYSA-N Hydrogen Chemical compound [H][H] UFHFLCQGNIYNRP-UHFFFAOYSA-N 0.000 claims abstract description 21
- 239000003054 catalyst Substances 0.000 claims abstract description 18
- JEIPFZHSYJVQDO-UHFFFAOYSA-N iron(III) oxide Inorganic materials O=[Fe]O[Fe]=O JEIPFZHSYJVQDO-UHFFFAOYSA-N 0.000 claims abstract description 16
- BVKZGUZCCUSVTD-UHFFFAOYSA-L Carbonate Chemical compound [O-]C([O-])=O BVKZGUZCCUSVTD-UHFFFAOYSA-L 0.000 claims abstract description 10
- 238000001556 precipitation Methods 0.000 claims abstract description 6
- 230000001590 oxidative effect Effects 0.000 claims abstract 4
- 229910052500 inorganic mineral Inorganic materials 0.000 claims description 48
- 239000011707 mineral Substances 0.000 claims description 48
- 239000002594 sorbent Substances 0.000 claims description 24
- 239000000126 substance Substances 0.000 claims description 24
- 235000013980 iron oxide Nutrition 0.000 claims description 22
- FYYHWMGAXLPEAU-UHFFFAOYSA-N Magnesium Chemical group [Mg] FYYHWMGAXLPEAU-UHFFFAOYSA-N 0.000 claims description 16
- 239000011777 magnesium Substances 0.000 claims description 16
- 229910052749 magnesium Inorganic materials 0.000 claims description 14
- OYPRJOBELJOOCE-UHFFFAOYSA-N Calcium Chemical group [Ca] OYPRJOBELJOOCE-UHFFFAOYSA-N 0.000 claims description 12
- 239000011575 calcium Substances 0.000 claims description 12
- 229910052791 calcium Inorganic materials 0.000 claims description 12
- KRKNYBCHXYNGOX-UHFFFAOYSA-N citric acid Chemical compound OC(=O)CC(O)(C(O)=O)CC(O)=O KRKNYBCHXYNGOX-UHFFFAOYSA-N 0.000 claims description 12
- 238000004519 manufacturing process Methods 0.000 claims description 11
- 238000006243 chemical reaction Methods 0.000 claims description 10
- QTBSBXVTEAMEQO-UHFFFAOYSA-N Acetic acid Chemical compound CC(O)=O QTBSBXVTEAMEQO-UHFFFAOYSA-N 0.000 claims description 9
- MUBZPKHOEPUJKR-UHFFFAOYSA-N Oxalic acid Chemical compound OC(=O)C(O)=O MUBZPKHOEPUJKR-UHFFFAOYSA-N 0.000 claims description 9
- 239000002028 Biomass Substances 0.000 claims description 8
- 239000002738 chelating agent Substances 0.000 claims description 8
- 239000002440 industrial waste Substances 0.000 claims description 8
- 230000003647 oxidation Effects 0.000 claims description 8
- 238000007254 oxidation reaction Methods 0.000 claims description 8
- 239000002699 waste material Substances 0.000 claims description 8
- CIWBSHSKHKDKBQ-JLAZNSOCSA-N Ascorbic acid Chemical compound OC[C@H](O)[C@H]1OC(=O)C(O)=C1O CIWBSHSKHKDKBQ-JLAZNSOCSA-N 0.000 claims description 6
- RGHNJXZEOKUKBD-SQOUGZDYSA-N D-gluconic acid Chemical compound OC[C@@H](O)[C@@H](O)[C@H](O)[C@@H](O)C(O)=O RGHNJXZEOKUKBD-SQOUGZDYSA-N 0.000 claims description 6
- NBIIXXVUZAFLBC-UHFFFAOYSA-N Phosphoric acid Chemical compound OP(O)(O)=O NBIIXXVUZAFLBC-UHFFFAOYSA-N 0.000 claims description 6
- VNWKTOKETHGBQD-UHFFFAOYSA-N methane Chemical compound C VNWKTOKETHGBQD-UHFFFAOYSA-N 0.000 claims description 6
- XNGIFLGASWRNHJ-UHFFFAOYSA-N phthalic acid Chemical compound OC(=O)C1=CC=CC=C1C(O)=O XNGIFLGASWRNHJ-UHFFFAOYSA-N 0.000 claims description 6
- 239000003245 coal Substances 0.000 claims description 5
- 239000010813 municipal solid waste Substances 0.000 claims description 4
- UGFAIRIUMAVXCW-UHFFFAOYSA-N Carbon monoxide Chemical compound [O+]#[C-] UGFAIRIUMAVXCW-UHFFFAOYSA-N 0.000 claims description 3
- RGHNJXZEOKUKBD-UHFFFAOYSA-N D-gluconic acid Natural products OCC(O)C(O)C(O)C(O)C(O)=O RGHNJXZEOKUKBD-UHFFFAOYSA-N 0.000 claims description 3
- 229910000147 aluminium phosphate Inorganic materials 0.000 claims description 3
- 239000011668 ascorbic acid Substances 0.000 claims description 3
- 229960005070 ascorbic acid Drugs 0.000 claims description 3
- 235000010323 ascorbic acid Nutrition 0.000 claims description 3
- 229910002091 carbon monoxide Inorganic materials 0.000 claims description 3
- 239000000174 gluconic acid Substances 0.000 claims description 3
- 235000012208 gluconic acid Nutrition 0.000 claims description 3
- NBZBKCUXIYYUSX-UHFFFAOYSA-N iminodiacetic acid Chemical compound OC(=O)CNCC(O)=O NBZBKCUXIYYUSX-UHFFFAOYSA-N 0.000 claims description 3
- 235000006408 oxalic acid Nutrition 0.000 claims description 3
- 239000002245 particle Substances 0.000 claims description 3
- 235000011007 phosphoric acid Nutrition 0.000 claims description 3
- 150000003839 salts Chemical class 0.000 claims description 3
- 229910000831 Steel Inorganic materials 0.000 claims description 2
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 claims description 2
- 238000000605 extraction Methods 0.000 claims description 2
- 239000007789 gas Substances 0.000 claims description 2
- VBMVTYDPPZVILR-UHFFFAOYSA-N iron(2+);oxygen(2-) Chemical class [O-2].[Fe+2] VBMVTYDPPZVILR-UHFFFAOYSA-N 0.000 claims description 2
- 239000001301 oxygen Substances 0.000 claims description 2
- 229910052760 oxygen Inorganic materials 0.000 claims description 2
- 239000004449 solid propellant Substances 0.000 claims description 2
- 239000010959 steel Substances 0.000 claims description 2
- 230000001172 regenerating effect Effects 0.000 claims 4
- 239000010881 fly ash Substances 0.000 claims 1
- 150000002431 hydrogen Chemical class 0.000 claims 1
- 239000002893 slag Substances 0.000 claims 1
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 description 13
- 229910052799 carbon Inorganic materials 0.000 description 13
- 238000005516 engineering process Methods 0.000 description 12
- 230000009919 sequestration Effects 0.000 description 11
- 239000001095 magnesium carbonate Substances 0.000 description 9
- 229910000021 magnesium carbonate Inorganic materials 0.000 description 9
- VYPSYNLAJGMNEJ-UHFFFAOYSA-N Silicium dioxide Chemical compound O=[Si]=O VYPSYNLAJGMNEJ-UHFFFAOYSA-N 0.000 description 8
- ZLNQQNXFFQJAID-UHFFFAOYSA-L magnesium carbonate Chemical compound [Mg+2].[O-]C([O-])=O ZLNQQNXFFQJAID-UHFFFAOYSA-L 0.000 description 7
- VTYYLEPIZMXCLO-UHFFFAOYSA-L Calcium carbonate Chemical compound [Ca+2].[O-]C([O-])=O VTYYLEPIZMXCLO-UHFFFAOYSA-L 0.000 description 4
- WYTGDNHDOZPMIW-RCBQFDQVSA-N alstonine Natural products C1=CC2=C3C=CC=CC3=NC2=C2N1C[C@H]1[C@H](C)OC=C(C(=O)OC)[C@H]1C2 WYTGDNHDOZPMIW-RCBQFDQVSA-N 0.000 description 4
- 239000000377 silicon dioxide Substances 0.000 description 4
- 238000003786 synthesis reaction Methods 0.000 description 4
- 230000008901 benefit Effects 0.000 description 3
- 230000015572 biosynthetic process Effects 0.000 description 3
- 238000004090 dissolution Methods 0.000 description 3
- -1 e.g. Substances 0.000 description 3
- 239000010450 olivine Substances 0.000 description 3
- 229910052609 olivine Inorganic materials 0.000 description 3
- 239000007787 solid Substances 0.000 description 3
- 239000012265 solid product Substances 0.000 description 3
- 229910000019 calcium carbonate Inorganic materials 0.000 description 2
- 239000003575 carbonaceous material Substances 0.000 description 2
- 230000005611 electricity Effects 0.000 description 2
- SZVJSHCCFOBDDC-UHFFFAOYSA-N ferrosoferric oxide Chemical compound O=[Fe]O[Fe]O[Fe]=O SZVJSHCCFOBDDC-UHFFFAOYSA-N 0.000 description 2
- 239000007788 liquid Substances 0.000 description 2
- 229910052751 metal Inorganic materials 0.000 description 2
- 239000002184 metal Substances 0.000 description 2
- 238000012545 processing Methods 0.000 description 2
- VHUUQVKOLVNVRT-UHFFFAOYSA-N Ammonium hydroxide Chemical compound [NH4+].[OH-] VHUUQVKOLVNVRT-UHFFFAOYSA-N 0.000 description 1
- 238000007792 addition Methods 0.000 description 1
- 238000013459 approach Methods 0.000 description 1
- 229910001748 carbonate mineral Inorganic materials 0.000 description 1
- 150000004649 carbonic acid derivatives Chemical class 0.000 description 1
- 229910052681 coesite Inorganic materials 0.000 description 1
- 229910052906 cristobalite Inorganic materials 0.000 description 1
- 230000001627 detrimental effect Effects 0.000 description 1
- 238000010586 diagram Methods 0.000 description 1
- 230000000694 effects Effects 0.000 description 1
- 239000002803 fossil fuel Substances 0.000 description 1
- 239000005431 greenhouse gas Substances 0.000 description 1
- 230000010354 integration Effects 0.000 description 1
- FLTRNWIFKITPIO-UHFFFAOYSA-N iron;trihydrate Chemical compound O.O.O.[Fe] FLTRNWIFKITPIO-UHFFFAOYSA-N 0.000 description 1
- 238000002386 leaching Methods 0.000 description 1
- 229910044991 metal oxide Inorganic materials 0.000 description 1
- 150000004706 metal oxides Chemical class 0.000 description 1
- 229940031182 nanoparticles iron oxide Drugs 0.000 description 1
- 239000000047 product Substances 0.000 description 1
- 238000011084 recovery Methods 0.000 description 1
- 238000012827 research and development Methods 0.000 description 1
- 239000011435 rock Substances 0.000 description 1
- 230000000087 stabilizing effect Effects 0.000 description 1
- 229910052682 stishovite Inorganic materials 0.000 description 1
- 229910052905 tridymite Inorganic materials 0.000 description 1
- 238000010792 warming Methods 0.000 description 1
Images
Classifications
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- C—CHEMISTRY; METALLURGY
- C01—INORGANIC CHEMISTRY
- C01G—COMPOUNDS CONTAINING METALS NOT COVERED BY SUBCLASSES C01D OR C01F
- C01G49/00—Compounds of iron
- C01G49/02—Oxides; Hydroxides
- C01G49/06—Ferric oxide [Fe2O3]
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D53/00—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols
- B01D53/34—Chemical or biological purification of waste gases
- B01D53/46—Removing components of defined structure
- B01D53/62—Carbon oxides
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D53/00—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols
- B01D53/34—Chemical or biological purification of waste gases
- B01D53/74—General processes for purification of waste gases; Apparatus or devices specially adapted therefor
- B01D53/81—Solid phase processes
-
- C—CHEMISTRY; METALLURGY
- C01—INORGANIC CHEMISTRY
- C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
- C01B3/00—Hydrogen; Gaseous mixtures containing hydrogen; Separation of hydrogen from mixtures containing it; Purification of hydrogen
- C01B3/02—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen
- C01B3/06—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen by reaction of inorganic compounds containing electro-positively bound hydrogen, e.g. water, acids, bases, ammonia, with inorganic reducing agents
- C01B3/10—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen by reaction of inorganic compounds containing electro-positively bound hydrogen, e.g. water, acids, bases, ammonia, with inorganic reducing agents by reaction of water vapour with metals
- C01B3/105—Cyclic methods
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D2253/00—Adsorbents used in seperation treatment of gases and vapours
- B01D2253/10—Inorganic adsorbents
- B01D2253/112—Metals or metal compounds not provided for in B01D2253/104 or B01D2253/106
- B01D2253/1124—Metal oxides
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D2257/00—Components to be removed
- B01D2257/50—Carbon oxides
- B01D2257/504—Carbon dioxide
-
- C—CHEMISTRY; METALLURGY
- C01—INORGANIC CHEMISTRY
- C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
- C01B2203/00—Integrated processes for the production of hydrogen or synthesis gas
- C01B2203/80—Aspect of integrated processes for the production of hydrogen or synthesis gas not covered by groups C01B2203/02 - C01B2203/1695
- C01B2203/86—Carbon dioxide sequestration
-
- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
- Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
- Y02E60/30—Hydrogen technology
- Y02E60/36—Hydrogen production from non-carbon containing sources, e.g. by water electrolysis
-
- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02P—CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
- Y02P30/00—Technologies relating to oil refining and petrochemical industry
Definitions
- CCS carbon capture and storage
- chemical looping processes involve a sorbent, typically a metal, or more likely a low oxidation state metal oxide that can be oxidized in air. The oxide is reduced by carbonaceous fuels in a subsequent step.
- a variation of this approach oxidizes the metal not in air but in a chemical reaction with steam to produce a pure stream of H 2 .
- the chemical looping processes also allow the inherent generation of the sequestration-ready CO 2 stream at higher pressures.
- CO 2 can be stored via geological sequestration, ocean disposal, mineral carbonation, and biological fixation.
- the mineral sequestration scheme is particularly attractive, since this process converts CO 2 into thermodynamically stable carbonates via the reaction of CO 2 with widely available non-carbonate minerals, such as serpentine and olivine. Therefore, the mineral sequestration process eliminates the risk of accidental CO 2 releases.
- the reaction underlining mineral carbonation mimics natural chemical transformations of CO 2 , such as the weathering of rocks.
- the main challenges of this storage method have been the slow dissolution kinetics and large energy requirement associated with the mineral processing.
- the previously developed pH swing carbon mineral sequestration immobilizes the gaseous CO 2 into a thermodynamically stable solid, MgCO 3 , using Mg-bearing minerals such as serpentine.
- This mineral carbonation technology is particularly promising since it generates value-added solid products: high surface area silica, iron oxide, and magnesium carbonate, while providing a safe and permanent storage option for CO 2 .
- By carefully controlling the pH of the system these solids products can be produced with high purity.
- the disclosed subject matter focuses on the synthesis of iron oxide particles as a chemical looping sorbent in order to achieve the integration between carbon capture and storage technologies.
- the synthesized iron-based chemical looping sorbent has been found to be as effective as commercially available iron oxide nanoparticles at converting syngas/carbonaceous fuel into high purity H 2 , while producing a sequestration-ready CO 2 stream.
- the disclosed subject matter utilizes the iron component of magnesium-bearing minerals, e.g., olivine and serpentine, during carbon mineral sequestration. These minerals often contain 5-10 percent by weight of iron, and the recovery and utilization of iron during the mineral processing increases the economic feasibility of carbon mineral sequestration technology.
- iron-based materials the disclosed subject matter focuses on the synthesis of iron-based chemical looping sorbents, which can be used for carbon dioxide capture and hydrogen production, as well as the syntheses of iron-based catalysts to be used in the production of synthetic liquid fuels and hydrogen from carbonaceous materials including coal, biomass, and municipal solid wastes.
- FIG. 1 is a chart of a method according to some embodiments of the disclosed subject matter.
- FIG. 2 is a schematic diagram of a system according to some embodiments of the disclosed subject matter.
- Some embodiments of the disclosed subject matter include methods and systems for sequestering carbon dioxide and generating hydrogen.
- Methods and systems according to the disclosed subject matter include combining pH swing carbon sequestration processes with chemical looping processes. pH swing processes are employed, which can sequestrate CO 2 while generating solid products: high surface area silica; iron oxide; and magnesium carbonate. Iron-based chemical looping sorbents are synthesized during the pH swing carbon mineral sequestration process. Thus, two CCS technologies are integrated. Processes including carbon mineral sequestration are used to generate a supply of Fe 2 O 3 , which is used by chemical looping processes for H 2 production. The CO 2 produced during chemical looping processes is then sequestered via mineral carbonation.
- pH swing processes are used to both consume a first source of carbon dioxide to produce carbonated minerals and thus sequester the carbon dioxide and also generate iron-based chemical looping sorbents from minerals, respectively:
- the iron-based chemical looping sorbents are then reduced via oxidation with a carbonaceous fuel to generate a second source of carbon dioxide for consumption in the pH swing processes.
- the iron-based chemical looping sorbents are regenerated via oxidation with steam to generate hydrogen:
- some embodiments include a method 100 of sequestering carbon dioxide and generating hydrogen.
- an iron-based material such as a magnesium or calcium-bearing mineral or other carbonate-forming element or industrial wastes containing iron and a carbonate-forming element such as calcium or magnesium is dissolved to form a solution including a carbonate-forming element, e.g., magnesium and/or calcium, and iron.
- a carbonate-forming element e.g., magnesium and/or calcium
- Magnesium-bearing minerals e.g. olivine and serpentine, often contain 510 percent by weight of iron.
- a chelating agent that targets magnesium, calcium, and iron is added to the solution before increasing a pH of the solution.
- the chelating agent is selected so as to be effective at leaching out iron content from the solution while allowing fast precipitation of iron oxide during the pH swing processes.
- Examples of chelating agents include acetic acid, citric acid, iminodiacetic acid, oxalic acid, phosphoric acid, gluconic acid, ascorbic acid, phthalic acid, a salt thereof, and a combination thereof. Citric acid has been found to provide higher dissolution as compared other chelating agents.
- a pH of the solution is increased to cause precipitation of iron oxide from the solution thereby generating a first source of Fe 2 O 3 .
- precipitation of iron oxide is conducted in the presence of support materials such as commercially available Fe 2 O 3 particles.
- the support materials can be commercially available materials or high surface area silica produced during dissolution of minerals and/or wastes during method 100 .
- the carbonate-forming element, e.g., magnesium or calcium, in the solution is reacted with a first source of carbon dioxide to produce a carbonate, e.g., magnesium or calcium carbonate, thereby sequestering the carbon dioxide.
- the first source of carbon dioxide is anthropogenic produced, e.g., emissions from coal-burning power plants and other man-made sources of carbon dioxide.
- the first source of Fe 2 O 3 is oxidized with a carbonaceous fuel thereby generating a second source of carbon dioxide and iron.
- the second source of carbon dioxide can then be utilized in step 108 to produce magnesium carbonate thereby sequestering the carbon dioxide.
- the carbonaceous fuel includes gaseous fuels such as synthetic gas (carbon monoxide and hydrogen) and methane.
- the carbonaceous fuel includes solid fuels including coal, biomass, and municipal solid wastes.
- the iron is oxidized with steam thereby generating hydrogen and an iron oxide.
- the iron oxide is fully oxidized with oxygen thereby generating a second source of Fe 2 O 3 , which can be reacted with the carbonaceous fuel in 110 to generate additional carbon dioxide and iron.
- iron-based catalysts e.g., iron oxide
- the produced iron oxide can also be used as catalysts for various industrial processes such as Fischer-Tropsch, water-gas-shift, and biomass conversion processes. These catalysts are currently produced using pure systems but can be produced utilizing methods and systems according to the disclosed subject matter from the waste stream of the carbon mineral sequestration process.
- System 200 includes a mineral and waste carbonation module 202 and a chemical looping module 204 .
- Mineral carbonation module 202 produces iron-based chemical looping sorbents 206 from minerals and industrial wastes 208 using pH swing processes.
- Iron-based chemical looping sorbents 206 include iron oxides such as Fe 2 O 3 or similar.
- Minerals and industrial wastes 208 are carbonate-forming minerals and wastes including carbonate-forming minerals, e.g., magnesium and calcium-bearing minerals that include iron 210 .
- the pH swing processes also consume a first source of carbon dioxide 212 to produce carbonated minerals 214 such as magnesium or calcium carbonate or similar.
- the pH swing processes include the use of a chelating agent 216 to facilitate the extraction of iron 210 from minerals or industrial wastes 208 .
- chemical looping module 204 includes a fuel reactor 218 and a hydrogen production reactor 220 .
- fuel reactor 218 chemical looping processes are utilized to reduce the iron-based chemical looping sorbents 206 via oxidation with a carbonaceous fuel 222 to generate a second source of carbon dioxide 224 for consumption by the pH swing processes in mineral carbonation module 202 and iron 226 (Fe, FeO).
- iron-based chemical looping sorbents 206 are regenerated by reducing iron 226 via oxidation with steam 228 to generate hydrogen 230 .
- system 200 includes a module for producing iron-based catalysts, e.g., iron oxide.
- the iron-based catalysts can be used for various industrial processes including Fischer-Tropsch synthesis, water-gas-shift reactions, and biomass conversion.
- Methods and systems according to the disclosed subject matter offer benefits and advantages over known technologies.
- Technology according to the disclosed subject matter can be used for carbon dioxide capture and mineral sequestration, while also being used for hydrogen production.
- Synthesized iron-based catalysts can be used in the production of synthetic liquid fuels and/or hydrogen from carbonaceous materials including coal, biomass, and municipal solid wastes. Synthesized iron oxide can also directly be used in the steel industry once it is recovered.
- Technology ties carbon storage technology with carbon capture technology as well as other sustainable energy conversion systems to improve the overall life cycle of carbon management technologies.
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- Engineering & Computer Science (AREA)
- Chemical Kinetics & Catalysis (AREA)
- Health & Medical Sciences (AREA)
- Inorganic Chemistry (AREA)
- Environmental & Geological Engineering (AREA)
- General Chemical & Material Sciences (AREA)
- Analytical Chemistry (AREA)
- Oil, Petroleum & Natural Gas (AREA)
- Biomedical Technology (AREA)
- General Health & Medical Sciences (AREA)
- Combustion & Propulsion (AREA)
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Abstract
Methods and systems for sequestering carbon dioxide and generating hydrogen are disclosed. In some embodiments, the methods include the following: dissolving an iron based material that includes a carbonate-forming element into a solution including the carbonate-forming element and iron; increasing a pH of the solution to cause precipitation of iron oxide from the solution thereby generating a first source of Fe2O3; reacting the carbonate-forming element in the solution with a first source of carbon dioxide to produce a carbonate thereby sequestering the carbon dioxide; oxidizing the first source of Fe2O3 with a carbonaceous fuel thereby generating a second source of carbon dioxide and iron; and oxidizing the iron with steam thereby generating hydrogen and an iron oxide. Some embodiments include producing iron-based catalysts.
Description
- This application is a continuation of copending U.S. patent application Ser. No. 13/319,831, filed Nov. 10, 2011, which is a national stage patent application of PCT/US2010/034921, filed May 14, 2010, which claims the benefit of U.S. Provisional Application No. 61/178,272, filed May 14, 2009, all of which are incorporated by reference as if disclosed herein in their entireties.
- Since the industrial revolution, the amount of CO2 in the atmosphere has risen from 280 ppm in 1800 to 370 ppm in 2000, mainly due to the consumption of fossil fuels. More than half of the energy used in the United States comes from the use of coal, and it is mostly used to generate electricity. Unfortunately, CO2 is one of the greenhouse gases considered to be responsible for global warming. Moreover, the increased atmospheric CO2 concentration will acidify the ocean and will change the chemistry of the surface ocean, leading to a potentially detrimental impact on the ecosystem. In order to meet the ever-increasing global energy demands, while stabilizing the atmospheric CO2 level, current carbon emissions should be significantly reduced.
- There have been significant research and development activities in the area of carbon capture and storage (CCS), including a number of integrated technologies (e.g., chemical looping processes) to combine CO2 capture with electricity/chemical/fuel production. Chemical looping processes involve a sorbent, typically a metal, or more likely a low oxidation state metal oxide that can be oxidized in air. The oxide is reduced by carbonaceous fuels in a subsequent step. A variation of this approach oxidizes the metal not in air but in a chemical reaction with steam to produce a pure stream of H2. The chemical looping processes also allow the inherent generation of the sequestration-ready CO2 stream at higher pressures.
- Once captured, CO2 can be stored via geological sequestration, ocean disposal, mineral carbonation, and biological fixation. The mineral sequestration scheme is particularly attractive, since this process converts CO2 into thermodynamically stable carbonates via the reaction of CO2 with widely available non-carbonate minerals, such as serpentine and olivine. Therefore, the mineral sequestration process eliminates the risk of accidental CO2 releases. The reaction underlining mineral carbonation mimics natural chemical transformations of CO2, such as the weathering of rocks. The main challenges of this storage method have been the slow dissolution kinetics and large energy requirement associated with the mineral processing.
- The previously developed pH swing carbon mineral sequestration immobilizes the gaseous CO2 into a thermodynamically stable solid, MgCO3, using Mg-bearing minerals such as serpentine. This mineral carbonation technology is particularly promising since it generates value-added solid products: high surface area silica, iron oxide, and magnesium carbonate, while providing a safe and permanent storage option for CO2. By carefully controlling the pH of the system, these solids products can be produced with high purity. The disclosed subject matter focuses on the synthesis of iron oxide particles as a chemical looping sorbent in order to achieve the integration between carbon capture and storage technologies. The synthesized iron-based chemical looping sorbent has been found to be as effective as commercially available iron oxide nanoparticles at converting syngas/carbonaceous fuel into high purity H2, while producing a sequestration-ready CO2 stream.
- The disclosed subject matter utilizes the iron component of magnesium-bearing minerals, e.g., olivine and serpentine, during carbon mineral sequestration. These minerals often contain 5-10 percent by weight of iron, and the recovery and utilization of iron during the mineral processing increases the economic feasibility of carbon mineral sequestration technology. Among many applications of iron-based materials, the disclosed subject matter focuses on the synthesis of iron-based chemical looping sorbents, which can be used for carbon dioxide capture and hydrogen production, as well as the syntheses of iron-based catalysts to be used in the production of synthetic liquid fuels and hydrogen from carbonaceous materials including coal, biomass, and municipal solid wastes.
- The drawings show embodiments of the disclosed subject matter for the purpose of illustrating the invention. However, it should be understood that the present application is not limited to the precise arrangements and instrumentalities shown in the drawings, wherein:
-
FIG. 1 is a chart of a method according to some embodiments of the disclosed subject matter; and -
FIG. 2 is a schematic diagram of a system according to some embodiments of the disclosed subject matter. - Some embodiments of the disclosed subject matter include methods and systems for sequestering carbon dioxide and generating hydrogen. Methods and systems according to the disclosed subject matter include combining pH swing carbon sequestration processes with chemical looping processes. pH swing processes are employed, which can sequestrate CO2 while generating solid products: high surface area silica; iron oxide; and magnesium carbonate. Iron-based chemical looping sorbents are synthesized during the pH swing carbon mineral sequestration process. Thus, two CCS technologies are integrated. Processes including carbon mineral sequestration are used to generate a supply of Fe2O3, which is used by chemical looping processes for H2 production. The CO2 produced during chemical looping processes is then sequestered via mineral carbonation.
- As shown in equations [1] and [2], pH swing processes are used to both consume a first source of carbon dioxide to produce carbonated minerals and thus sequester the carbon dioxide and also generate iron-based chemical looping sorbents from minerals, respectively:
-
1/3(Mg,Fe)3Si2O5(OH)4+CO2=MgCO3+Fe+2/3SiO2+2/3H2O; [1] -
and -
Fe+NH4OH→Fe(OH)3 (and ultimately Fe2O3) [2] - As shown in equations [3] and [4], the iron-based chemical looping sorbents are then reduced via oxidation with a carbonaceous fuel to generate a second source of carbon dioxide for consumption in the pH swing processes. Finally, as shown in equations [5] and [6], the iron-based chemical looping sorbents are regenerated via oxidation with steam to generate hydrogen:
-
3CO+Fe2O3→3CO2+2Fe; [3] -
3H2+Fe2O3→3H20+2Fe; [4] -
3Fe4H2O→Fe3O4+4H2; [5] -
and -
4Fe3O4+O2→6Fe2O (ultimately to Fe2O3). [6] - Referring now to
FIG. 1 , some embodiments include amethod 100 of sequestering carbon dioxide and generating hydrogen. At 102, an iron-based material such as a magnesium or calcium-bearing mineral or other carbonate-forming element or industrial wastes containing iron and a carbonate-forming element such as calcium or magnesium is dissolved to form a solution including a carbonate-forming element, e.g., magnesium and/or calcium, and iron. Magnesium-bearing minerals, e.g. olivine and serpentine, often contain 510 percent by weight of iron. - At 104, a chelating agent that targets magnesium, calcium, and iron is added to the solution before increasing a pH of the solution. The chelating agent is selected so as to be effective at leaching out iron content from the solution while allowing fast precipitation of iron oxide during the pH swing processes. Examples of chelating agents include acetic acid, citric acid, iminodiacetic acid, oxalic acid, phosphoric acid, gluconic acid, ascorbic acid, phthalic acid, a salt thereof, and a combination thereof. Citric acid has been found to provide higher dissolution as compared other chelating agents.
- At 106, a pH of the solution is increased to cause precipitation of iron oxide from the solution thereby generating a first source of Fe2O3. In some embodiments, precipitation of iron oxide is conducted in the presence of support materials such as commercially available Fe2O3 particles. The support materials can be commercially available materials or high surface area silica produced during dissolution of minerals and/or wastes during
method 100. - At 108, the carbonate-forming element, e.g., magnesium or calcium, in the solution is reacted with a first source of carbon dioxide to produce a carbonate, e.g., magnesium or calcium carbonate, thereby sequestering the carbon dioxide. In some embodiments, the first source of carbon dioxide is anthropogenic produced, e.g., emissions from coal-burning power plants and other man-made sources of carbon dioxide.
- At 110, the first source of Fe2O3 is oxidized with a carbonaceous fuel thereby generating a second source of carbon dioxide and iron. The second source of carbon dioxide can then be utilized in
step 108 to produce magnesium carbonate thereby sequestering the carbon dioxide. In some embodiments, the carbonaceous fuel includes gaseous fuels such as synthetic gas (carbon monoxide and hydrogen) and methane. In some embodiments, the carbonaceous fuel includes solid fuels including coal, biomass, and municipal solid wastes. - At 112, the iron is oxidized with steam thereby generating hydrogen and an iron oxide. At 114, the iron oxide is fully oxidized with oxygen thereby generating a second source of Fe2O3, which can be reacted with the carbonaceous fuel in 110 to generate additional carbon dioxide and iron.
- Although not illustrated in
FIG. 1 , in some embodiments, iron-based catalysts, e.g., iron oxide, are produced. The produced iron oxide can also be used as catalysts for various industrial processes such as Fischer-Tropsch, water-gas-shift, and biomass conversion processes. These catalysts are currently produced using pure systems but can be produced utilizing methods and systems according to the disclosed subject matter from the waste stream of the carbon mineral sequestration process. - Referring now to
FIG. 2 , some embodiments of the disclosed subject matter include asystem 200 for sequestering carbon dioxide and generating hydrogen.System 200 includes a mineral andwaste carbonation module 202 and achemical looping module 204. -
Mineral carbonation module 202 produces iron-basedchemical looping sorbents 206 from minerals andindustrial wastes 208 using pH swing processes. Iron-basedchemical looping sorbents 206 include iron oxides such as Fe2O3 or similar. Minerals andindustrial wastes 208 are carbonate-forming minerals and wastes including carbonate-forming minerals, e.g., magnesium and calcium-bearing minerals that includeiron 210. The pH swing processes also consume a first source ofcarbon dioxide 212 to producecarbonated minerals 214 such as magnesium or calcium carbonate or similar. In some embodiments, the pH swing processes include the use of achelating agent 216 to facilitate the extraction ofiron 210 from minerals orindustrial wastes 208. - In some embodiments,
chemical looping module 204 includes afuel reactor 218 and ahydrogen production reactor 220. Infuel reactor 218, chemical looping processes are utilized to reduce the iron-basedchemical looping sorbents 206 via oxidation with acarbonaceous fuel 222 to generate a second source ofcarbon dioxide 224 for consumption by the pH swing processes inmineral carbonation module 202 and iron 226 (Fe, FeO). Inhydrogen production reactor 220, iron-basedchemical looping sorbents 206 are regenerated by reducingiron 226 via oxidation withsteam 228 to generatehydrogen 230. - In some embodiments,
system 200 includes a module for producing iron-based catalysts, e.g., iron oxide. The iron-based catalysts can be used for various industrial processes including Fischer-Tropsch synthesis, water-gas-shift reactions, and biomass conversion. - Methods and systems according to the disclosed subject matter offer benefits and advantages over known technologies. Technology according to the disclosed subject matter can be used for carbon dioxide capture and mineral sequestration, while also being used for hydrogen production.
- Synthesized iron-based catalysts can be used in the production of synthetic liquid fuels and/or hydrogen from carbonaceous materials including coal, biomass, and municipal solid wastes. Synthesized iron oxide can also directly be used in the steel industry once it is recovered.
- Technology according to the disclosed subject matter ties carbon storage technology with carbon capture technology as well as other sustainable energy conversion systems to improve the overall life cycle of carbon management technologies.
- By controlling the pH of the system, technology according to the disclosed subject matter can be used to generate solid products from the mineral carbonation process: SiO2-rich solids; iron oxide; and MgCO3*3H2O. The iron oxide and MgCO3 produced would be highly pure.
- Although the disclosed subject matter has been described and illustrated with respect to embodiments thereof, it should be understood by those skilled in the art that features of the disclosed embodiments can be combined, rearranged, etc., to produce additional embodiments within the scope of the invention, and that various other changes, omissions, and additions may be made therein and thereto, without parting from the spirit and scope of the present invention.
Claims (24)
1. A method of sequestering carbon dioxide, said method comprising:
producing iron-based sorbents and a carbonate forming material from minerals comprising iron;
consuming a first source of carbon dioxide to produce carbonated minerals from the carbonate forming material;
reducing the iron-based sorbents with a carbonaceous fuel to generate a second source of carbon dioxide; and
regenerating said iron-based sorbents that have been reduced via oxidation with steam.
2. The method according to claim 1 , wherein the minerals comprising iron include calcium-bearing minerals, magnesium-bearing minerals, and industrial wastes.
3. The method according to claim 1 , further comprising producing iron-based catalysts including Fischer Tropsch catalysts, water-gas-shift catalysts, and biomass conversion catalysts.
4. The method according to claim 3 , wherein said iron-based catalysts and iron-based sorbents include iron oxides such as Fe2O3.
5. The method of according to claim 1 , further comprising isolating the iron-based sorbents from the carbonate forming material via a pH swing process.
6. The method according to claim 1 , further comprising the step of consuming the second source of carbon dioxide using the carbonate forming material.
7. The method according to claim 1 , wherein the step of regenerating said iron-based sorbents further includes the step of generating hydrogen.
8. A method of sequestering carbon dioxide and generating hydrogen, said method comprising:
dissolving a material that includes a carbonate-forming element and iron with a chelating agent into a solution;
increasing a pH of said solution to cause precipitation of a first source of iron oxide from said solution;
reacting said carbonate-forming element with a first source of carbon dioxide;
reducing said first source of iron oxide with a carbonaceous fuel thereby generating a second source of carbon dioxide and reduced iron; and
oxidizing said reduced iron with steam thereby generating hydrogen and a second source of iron oxide.
9. The method according to claim 8 , further comprising:
producing iron-based catalysts including Fischer Tropsch catalysts, water-gas-shift catalysts, and biomass conversion catalysts.
10. The method according to claim 8 , wherein said material is selected from the group consisting of: calcium-bearing minerals, magnesium-bearing minerals, and industrial wastes containing iron and carbonate-forming elements including magnesium and calcium.
11. The method according to claim 8 , wherein said carbonate forming element is selected from the group consisting of: magnesium, calcium, and a combination thereof.
12. The method according to claim 8 , further comprising:
oxidizing said second source of iron oxide with oxygen thereby generating a source of fully oxidized Fe2O3.
13. The method according to claim 10 , wherein the chelating agents are added to said solution before increasing a pH of said solution to dissolve said minerals or said wastes and target Ma, Ca and Fe and include acetic acid, citric acid, iminodiacetic acid, oxalic acid, phosphoric acid, gluconic acid, ascorbic acid, phthalic acid, a salt thereof, and a combination thereof.
14. The method according to claim 8 , further comprising:
reacting said carbonate-forming element in said solution with said second source of carbon dioxide to produce a carbonate thereby sequestering said carbon dioxide.
15. The method according to claim 8 , further comprising:
reacting said second source of iron oxide with said carbonaceous fuel.
16. The method according to claim 8 , wherein said carbonaceous fuel includes gaseous fuels including carbon monoxide and hydrogen and methane.
17. The method according to claim 8 , wherein precipitation of the first source of iron oxide is conducted in the presence of support materials such as provided Fe2O3 particles.
18. A system for sequestering carbon dioxide, said system comprising:
a mineral and waste carbonation module for producing iron-based sorbents and carbonate forming material from at least one of minerals and industrial wastes using pH swing processes and sequestering carbon dioxide using the carbonate forming material; and
a chemical looping module, said chemical looping module configured to reduce said iron-based sorbents and generate carbon dioxide for consumption in the mineral and waste carbonation module and regenerating said iron-based sorbents that have been reduced via oxidation with steam.
19. The system according to claim 18 , wherein minerals include magnesium and calcium-bearing minerals including iron and industrial wastes include magnesium and calcium-bearing wastes including steel slag and fly ash containing iron.
20. The system according to claim 18 , wherein said iron-based sorbents include Fe2O3.
21. The system according to claim 18 , wherein said pH swing processes include the use of at least one of acetic acid, citric acid, iminodiacetic acid, oxalic acid, phosphoric acid, gluconic acid, ascorbic acid, phthalic acid, a salt thereof, and a combination thereof as a chelating agent to facilitate the extraction of iron from said minerals.
22. The system according to claim 18 , wherein said chemical looping module further comprises:
a fuel reactor for reducing said iron-based sorbents via a carbonaceous fuel to generate carbon dioxide; and
a hydrogen production reactor for regenerating said iron-based sorbents that have been reduced via oxidation with steam to generate hydrogen.
23. The system according to claim 18 , further comprising a module for producing iron-based catalysts.
24. The system according to claim 22 , wherein said carbonaceous fuel includes gaseous fuels including synthetic gas (carbon monoxide and hydrogen) and methane, and solid fuels including coal, biomass, and municipal solid wastes.
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US11305261B2 (en) * | 2018-05-29 | 2022-04-19 | Sekisui Chemical Co., Ltd. | Catalyst, carbon dioxide reducing method, and apparatus for reducing carbon dioxide |
WO2022259022A1 (en) * | 2021-06-09 | 2022-12-15 | Cyprus University Of Technology | System and method for carbon capture and utilization |
WO2023007466A1 (en) * | 2021-07-30 | 2023-02-02 | Ohio State Innovation Foundation | Systems and methods for generating hydrogen and magnetite from rock |
US11896930B2 (en) | 2021-10-18 | 2024-02-13 | Project Vesta, PBC | Carbon-removing sand and method and process for design, manufacture, and utilization of the same |
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US9089837B2 (en) * | 2013-09-30 | 2015-07-28 | Institute Of Nuclear Energy Research, Atomic Energy Council | Method of fabricating a high-temperature CO2 capture agent |
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