CN118059883A - Hexagonal disk Fe2O3Catalyst for producing hydrogen by low-temperature water gas conversion loaded with single-atom Au and preparation method thereof - Google Patents
Hexagonal disk Fe2O3Catalyst for producing hydrogen by low-temperature water gas conversion loaded with single-atom Au and preparation method thereof Download PDFInfo
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- CN118059883A CN118059883A CN202410032818.5A CN202410032818A CN118059883A CN 118059883 A CN118059883 A CN 118059883A CN 202410032818 A CN202410032818 A CN 202410032818A CN 118059883 A CN118059883 A CN 118059883A
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- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 title claims abstract description 22
- 229910001868 water Inorganic materials 0.000 title claims abstract description 21
- 239000007789 gas Substances 0.000 title abstract description 11
- 238000002360 preparation method Methods 0.000 title abstract description 5
- 229910052739 hydrogen Inorganic materials 0.000 title description 17
- UFHFLCQGNIYNRP-UHFFFAOYSA-N Hydrogen Chemical compound [H][H] UFHFLCQGNIYNRP-UHFFFAOYSA-N 0.000 title description 16
- 239000001257 hydrogen Substances 0.000 title description 16
- 238000006243 chemical reaction Methods 0.000 title description 8
- 239000003054 catalyst Substances 0.000 claims abstract description 30
- 229910000859 α-Fe Inorganic materials 0.000 claims abstract description 21
- LFQSCWFLJHTTHZ-UHFFFAOYSA-N Ethanol Chemical compound CCO LFQSCWFLJHTTHZ-UHFFFAOYSA-N 0.000 claims abstract description 14
- 239000000203 mixture Substances 0.000 claims abstract description 7
- 238000001027 hydrothermal synthesis Methods 0.000 claims abstract description 5
- 238000001035 drying Methods 0.000 claims description 4
- VMHLLURERBWHNL-UHFFFAOYSA-M Sodium acetate Chemical compound [Na+].CC([O-])=O VMHLLURERBWHNL-UHFFFAOYSA-M 0.000 claims description 2
- IDGUHHHQCWSQLU-UHFFFAOYSA-N ethanol;hydrate Chemical compound O.CCO IDGUHHHQCWSQLU-UHFFFAOYSA-N 0.000 claims description 2
- 229910052751 metal Inorganic materials 0.000 claims description 2
- 239000002184 metal Substances 0.000 claims description 2
- 235000017281 sodium acetate Nutrition 0.000 claims description 2
- 239000001632 sodium acetate Substances 0.000 claims description 2
- 239000002904 solvent Substances 0.000 claims description 2
- 238000009210 therapy by ultrasound Methods 0.000 claims description 2
- 238000010438 heat treatment Methods 0.000 claims 3
- 239000002253 acid Substances 0.000 claims 1
- 238000004140 cleaning Methods 0.000 claims 1
- 238000002390 rotary evaporation Methods 0.000 claims 1
- 238000001308 synthesis method Methods 0.000 claims 1
- 230000003197 catalytic effect Effects 0.000 abstract description 5
- 230000003993 interaction Effects 0.000 abstract description 3
- 239000002243 precursor Substances 0.000 abstract description 3
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 abstract description 2
- 239000001301 oxygen Substances 0.000 abstract description 2
- 229910052760 oxygen Inorganic materials 0.000 abstract description 2
- 229910052737 gold Inorganic materials 0.000 description 8
- 239000000446 fuel Substances 0.000 description 6
- 238000004519 manufacturing process Methods 0.000 description 4
- 238000005406 washing Methods 0.000 description 4
- 229910003145 α-Fe2O3 Inorganic materials 0.000 description 4
- QGZKDVFQNNGYKY-UHFFFAOYSA-N Ammonia Chemical compound N QGZKDVFQNNGYKY-UHFFFAOYSA-N 0.000 description 2
- 230000009286 beneficial effect Effects 0.000 description 2
- 230000015572 biosynthetic process Effects 0.000 description 2
- 230000000052 comparative effect Effects 0.000 description 2
- 239000006185 dispersion Substances 0.000 description 2
- 230000000694 effects Effects 0.000 description 2
- 238000000034 method Methods 0.000 description 2
- 239000002105 nanoparticle Substances 0.000 description 2
- 239000002028 Biomass Substances 0.000 description 1
- 230000009471 action Effects 0.000 description 1
- 238000005054 agglomeration Methods 0.000 description 1
- 230000002776 aggregation Effects 0.000 description 1
- 229910021529 ammonia Inorganic materials 0.000 description 1
- 229910002091 carbon monoxide Inorganic materials 0.000 description 1
- 239000008367 deionised water Substances 0.000 description 1
- 229910021641 deionized water Inorganic materials 0.000 description 1
- 239000003792 electrolyte Substances 0.000 description 1
- 238000001704 evaporation Methods 0.000 description 1
- 230000002349 favourable effect Effects 0.000 description 1
- 239000012528 membrane Substances 0.000 description 1
- 238000002156 mixing Methods 0.000 description 1
- 238000012986 modification Methods 0.000 description 1
- 230000004048 modification Effects 0.000 description 1
- 239000002574 poison Substances 0.000 description 1
- 231100000614 poison Toxicity 0.000 description 1
- 238000000746 purification Methods 0.000 description 1
- 239000012495 reaction gas Substances 0.000 description 1
- 238000000629 steam reforming Methods 0.000 description 1
- 239000000126 substance Substances 0.000 description 1
Classifications
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J23/00—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00
- B01J23/70—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of the iron group metals or copper
- B01J23/89—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of the iron group metals or copper combined with noble metals
- B01J23/8906—Iron and noble metals
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J37/00—Processes, in general, for preparing catalysts; Processes, in general, for activation of catalysts
- B01J37/08—Heat treatment
- B01J37/10—Heat treatment in the presence of water, e.g. steam
-
- 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
- C01B3/12—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 carbon monoxide
- C01B3/16—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 carbon monoxide using catalysts
-
- 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
- C01B2203/02—Processes for making hydrogen or synthesis gas
- C01B2203/0283—Processes for making hydrogen or synthesis gas containing a CO-shift step, i.e. a water gas shift step
-
- 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
- C01B2203/10—Catalysts for performing the hydrogen forming reactions
- C01B2203/1041—Composition of the catalyst
- C01B2203/1047—Group VIII metal catalysts
-
- 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
- C01B2203/10—Catalysts for performing the hydrogen forming reactions
- C01B2203/1041—Composition of the catalyst
- C01B2203/1082—Composition of support materials
-
- 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
- Y02P20/00—Technologies relating to chemical industry
- Y02P20/50—Improvements relating to the production of bulk chemicals
- Y02P20/52—Improvements relating to the production of bulk chemicals using catalysts, e.g. selective catalysts
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- Chemical & Material Sciences (AREA)
- Chemical Kinetics & Catalysis (AREA)
- Organic Chemistry (AREA)
- Engineering & Computer Science (AREA)
- Materials Engineering (AREA)
- Health & Medical Sciences (AREA)
- General Health & Medical Sciences (AREA)
- Combustion & Propulsion (AREA)
- Inorganic Chemistry (AREA)
- Physics & Mathematics (AREA)
- Thermal Sciences (AREA)
- Catalysts (AREA)
Abstract
The invention discloses a hexagonal disk-shaped Fe 2O3 loaded single-atom Au catalyst, and a preparation method and application thereof. The catalyst synthesizes hexagonal disk-shaped alpha-Fe 2O3 by adopting a hydrothermal method, then loads an Au precursor on alpha-Fe 2O3 by adopting low-temperature roasting, then washes by adopting a mixture of water and ethanol, and finally generates Au monoatoms by adopting high-temperature roasting treatment. The catalyst is applied to water gas conversion reaction, shows high catalytic activity at 150 ℃, and the CO generation rate can reach 0.8mol/mol/s per mol Jin Meimiao. The excellent performance of the catalyst benefits from the interaction between the oxygen binding site on the surface of the hexagonal disk-shaped alpha-Fe 2O3 and the Au atoms, so that the Au atoms are highly dispersed and stable.
Description
Technical Field
The invention relates to a hexagonal disk-shaped Fe 2O3 loaded single-atom Au catalyst, and a preparation method and application thereof. The catalyst consists of hexagonal disk alpha-Fe 2O3 and Au monoatoms, has high catalytic activity and stability, and can be used for water gas conversion reaction.
Background
The water gas shift reaction (co+h 2O→CO2+H2) is an important reaction for extracting hydrogen from water, and is an important reaction for fossil energy and biomass hydrogen production and hydrogen purification processes. The combination of the catalyst and steam reforming reaction is the main industrial technology of low-cost hydrogen production at present, and is widely applied to the production process of synthetic ammonia, oil products and chemicals.
With the development of hydrogen energy economy, hydrogen fuel cells are becoming an important new energy application platform. The hydrogen fuel cell takes hydrogen as fuel, and under the action of an electrolyte membrane, the hydrogen reacts with oxygen to generate electric energy and water. However, small amounts of CO in hydrogen fuel can poison fuel cell catalysts, reducing the activity and life of the catalyst. Therefore, it is necessary to purify the hydrogen fuel to remove CO therefrom.
The water gas shift reaction is a low temperature favorable reaction and has higher catalytic activity at low temperature. Therefore, the development of water gas shift catalysts with both high catalytic activity and stability in the low temperature region (< 200 ℃) is of great importance for hydrogen economy.
Disclosure of Invention
The invention discloses a hexagonal disk-shaped Fe 2O3 loaded single-atom Au catalyst, and a preparation method and application thereof. The catalyst synthesizes hexagonal disk-shaped alpha-Fe 2O3 by adopting a hydrothermal method, then loads an Au precursor on alpha-Fe 2O3 by adopting low-temperature roasting, then washes by adopting a mixture of water and ethanol, and finally generates Au monoatoms by adopting high-temperature roasting treatment. The invention aims to provide a catalyst of hexagonal disk-shaped Fe 2O3 loaded with single-atom Au, which realizes high dispersion and stability of the single-atom Au by improving the interaction between alpha-Fe 2O3 and the Au and shows excellent catalytic activity under the condition of water gas conversion reaction.
The technical scheme of the invention comprises the following steps:
1) Preparing hexagonal disk-shaped alpha-Fe 2O3;
2) Mixing HAuCl 4 with alpha-Fe 2O3, and then drying and roasting at low temperature to obtain alpha-Fe 2O3 loaded by Au precursor;
3) Washing with water and ethanol mixture, and roasting at high temperature to obtain Au monoatoms.
The beneficial effects of the invention include:
1) The hexagonal disk shape of the alpha-Fe 2O3 is beneficial to the high dispersion of Au monoatoms;
2) The alpha-Fe 2O3 has stronger interaction with the Au, so that the agglomeration growth of the Au is inhibited, and the stability of the Au monoatomic is enhanced;
3) In the preferred catalyst of the present invention, the CO formation rate per mole of metal reaches 0.8mol/mol/s at 150℃and shows excellent low temperature activity.
Description of the attached tables
Table 1 shows the results of a comparison of the hydrogen-producing performance of the 2wt% Au 1/α-Fe2O3 catalyst prepared in example 1 of the present invention with the 2wt% Au NP/a-Fe 2O3 catalyst prepared in comparative example 1 under water gas shift conditions.
Detailed Description
The technical scheme of the invention is further illustrated and described below by the detailed description in combination with the attached tables.
Example 1:
The procedure for preparing the 2wt% Au 1/α-Fe2O3 monoatomic catalyst was as follows:
1) 13.12g FeCl 3·6H2 O was dissolved in 480mL ethanol, 33.4mL water and 38.4g sodium acetate were added and mixed well;
2) After hydrothermal reaction for 12 hours at 180 ℃, centrifugally collecting hexagonal disk-shaped alpha-Fe 2O3, and washing and drying;
3) 100mg of alpha-Fe 2O3 and 45.5mg of HAuCl 4 are dissolved in 20mL of ethanol and subjected to ultrasonic treatment for 10 minutes;
4) Rotary evaporating to remove solvent, drying at 80deg.C, roasting at 300deg.C, and washing with water-ethanol mixture;
5) Roasting for 2 hours at 350 ℃ to obtain the Au single-atom loaded alpha-Fe 2O3.
Comparative example 1:
the procedure for preparing 2wt% Au NP/α -Fe 2O3 nanoparticle catalyst was as follows:
1) Repeating steps 1) and 2) of example 1);
2) In step 3) of example 1, 45.5mg of HAuCl 4 was directly dissolved in 20mL of water, and then reduced by addition of NaBH 4 solution (NaBH 4: au=5:1);
3) Washing with deionized water, and roasting at 350 ℃ for 2 hours to obtain the Au nanoparticle-loaded alpha-Fe 2O3.
Taking 0.1g of catalyst, and carrying out water gas conversion reaction at 150 ℃ and a flow rate of 150mL/min, wherein the composition of reaction gas is as follows: 11% CO/20% H 2/15％H2O/7％CO2/rest He. The results show that the 2wt% Au 1/α-Fe2O3 monoatomic catalyst prepared in example 1 had a water gas conversion of 0.8mol/mol/s at 150℃which is 7 times higher than the CO formation rate (0.1 mol/mol/s) of the 2wt% Au NP/alpha-Fe 2O3 catalyst.
Table 1.2 wt% Au 1/α-Fe2O3 catalyst vs. 2wt% Au NP/alpha-Fe 2O3 catalyst in terms of hydrogen making performance.
The foregoing description is only of the preferred embodiments of the present invention and is not intended to limit the scope of the invention. Equivalent changes and modifications are intended to be covered by this invention, as equivalents will fall within the scope of the invention.
Claims (4)
1. A hexagonal disk-shaped Fe 2O3 loaded single-atom Au catalyst is characterized in that: the catalyst contains Au metal active components which are loaded on hexagonal disk alpha-Fe 2O3 in a monoatomic mode in a highly dispersed mode. The hexagonal disk-shaped Fe 2O3 is synthesized by a hydrothermal method, and the Au loading amount is 0.1-5wt%.
2. The hexagonal disk shaped Fe 2O3 supported single atom Au catalyst according to claim 1, characterized in that: the synthesis method of the hexagonal disk-shaped alpha-Fe 2O3 comprises the following steps: feCl 3·6H2 O is dissolved in ethanol and water, sodium acetate is added, and the mixture is subjected to hydrothermal reaction at 150-240 ℃ for 4-24 hours to obtain the product.
3. The hexagonal disk shaped Fe 2O3 supported single atom Au catalyst according to claim 1, characterized in that: dispersing chloroauric acid and alpha-Fe 2O3 in ethanol, performing ultrasonic treatment for several minutes, performing rotary evaporation on the solvent, performing low-temperature drying, heating to 200-300 ℃ (heating rate of 5 ℃/min), cleaning by a water-ethanol mixture, heating to 300-500 ℃ in air at a rate of 1-5 ℃/min, and maintaining for 1-5 hours to generate Au monoatoms.
4. A hexagonal disk shaped Fe 2O3 supported single atom Au catalyst as claimed in any one of claims 1 to 3 characterised in that: is used for water gas conversion reaction and used as a catalyst.
Priority Applications (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| CN202410032818.5A CN118059883A (en) | 2024-01-09 | 2024-01-09 | Hexagonal disk Fe2O3Catalyst for producing hydrogen by low-temperature water gas conversion loaded with single-atom Au and preparation method thereof |
Applications Claiming Priority (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| CN202410032818.5A CN118059883A (en) | 2024-01-09 | 2024-01-09 | Hexagonal disk Fe2O3Catalyst for producing hydrogen by low-temperature water gas conversion loaded with single-atom Au and preparation method thereof |
Publications (1)
| Publication Number | Publication Date |
|---|---|
| CN118059883A true CN118059883A (en) | 2024-05-24 |
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| Application Number | Title | Priority Date | Filing Date |
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| CN202410032818.5A Pending CN118059883A (en) | 2024-01-09 | 2024-01-09 | Hexagonal disk Fe2O3Catalyst for producing hydrogen by low-temperature water gas conversion loaded with single-atom Au and preparation method thereof |
Country Status (1)
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| CN (1) | CN118059883A (en) |
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- 2024-01-09 CN CN202410032818.5A patent/CN118059883A/en active Pending
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