Enhanced mass transfer and optimized electronic structure on Pd–Ag nanoparticles embedded in mesoporous carbon for superior electro-oxidation
Abstract The development of economically viable anode catalysts for the alcohol oxidation reaction (AOR) has been a long-standing challenge in direct alcohol fuel cells (DAFCs). A series of Pd–Ag nanoparticles embedded in mesoporous carbon were fabricated in this study using a green approach that did not require the use of a surfactant, which exhibited better catalytic properties for AOR. Experiments and DFT calculations reveal that the d-band center of Pd is influenced by both strain and ligand effects, with the ligand effect predominating. The electrochemical studies demonstrated that the composite-optimized Pd–Ag alloy at a Pd/Ag molar ratio of 1:1 was the highest in terms of ethanol oxidation (EOR) and ethylene glycol oxidation (EGOR) catalytic activity. The mass activities of $ Pd_{1} $$ Ag_{1} $/MC for EOR and EGOR were 7921 mA $ mg^{−1} $ and 11,520 mA $ mg^{−1} $, respectively, which were 3.77 and 5.3 fold greater than Pd/C. The impressive performance of $ Pd_{1} $$ Ag_{1} $/MC catalyst could be attributed to the vital roles of the unique mesoporous structure of carbon sphere with abundant self-doping defect and the boosting effect of Ag (benefit from optimized d-band electronic structure and bi-functional mechanism). The present simple method of synthesizing low-cost, easy-to-use, and high-performance catalysts contributes to the exploration of the large-scale practical applications of direct alkaline alcohol fuel cells..
| Medienart: |
Artikel |
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| Erscheinungsjahr: |
2023 |
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| Erschienen: |
2023 |
| Enthalten in: |
Zur Gesamtaufnahme - volume:27 |
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| Enthalten in: |
Journal of solid state electrochemistry - 27(2023), 10 vom: 28. Juni, Seite 2737-2750 |
| Sprache: |
Englisch |
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| Beteiligte Personen: |
Chen, DePing [VerfasserIn] |
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| Links: |
Volltext [lizenzpflichtig] |
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| Themen: |
D-band center |
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| Anmerkungen: |
© The Author(s), under exclusive licence to Springer-Verlag GmbH Germany, part of Springer Nature 2023. Springer Nature or its licensor (e.g. a society or other partner) holds exclusive rights to this article under a publishing agreement with the author(s) or other rightsholder(s); author self-archiving of the accepted manuscript version of this article is solely governed by the terms of such publishing agreement and applicable law. |
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| doi: |
10.1007/s10008-023-05561-3 |
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| funding: |
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| Förderinstitution / Projekttitel: |
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| 520 | |a Abstract The development of economically viable anode catalysts for the alcohol oxidation reaction (AOR) has been a long-standing challenge in direct alcohol fuel cells (DAFCs). A series of Pd–Ag nanoparticles embedded in mesoporous carbon were fabricated in this study using a green approach that did not require the use of a surfactant, which exhibited better catalytic properties for AOR. Experiments and DFT calculations reveal that the d-band center of Pd is influenced by both strain and ligand effects, with the ligand effect predominating. The electrochemical studies demonstrated that the composite-optimized Pd–Ag alloy at a Pd/Ag molar ratio of 1:1 was the highest in terms of ethanol oxidation (EOR) and ethylene glycol oxidation (EGOR) catalytic activity. The mass activities of $ Pd_{1} $$ Ag_{1} $/MC for EOR and EGOR were 7921 mA $ mg^{−1} $ and 11,520 mA $ mg^{−1} $, respectively, which were 3.77 and 5.3 fold greater than Pd/C. The impressive performance of $ Pd_{1} $$ Ag_{1} $/MC catalyst could be attributed to the vital roles of the unique mesoporous structure of carbon sphere with abundant self-doping defect and the boosting effect of Ag (benefit from optimized d-band electronic structure and bi-functional mechanism). The present simple method of synthesizing low-cost, easy-to-use, and high-performance catalysts contributes to the exploration of the large-scale practical applications of direct alkaline alcohol fuel cells. | ||
| 650 | 4 | |a Pd–Ag alloy | |
| 650 | 4 | |a D-band center | |
| 650 | 4 | |a Ligand effect | |
| 650 | 4 | |a Strain effect | |
| 650 | 4 | |a Mesoporous carbon | |
| 650 | 4 | |a Electro-oxidation | |
| 700 | 1 | |a Li, Mengjue |4 aut | |
| 700 | 1 | |a Chen, Ying |4 aut | |
| 700 | 1 | |a Shao, Zhenyi |4 aut | |
| 700 | 1 | |a Wei, Yanhong |4 aut | |
| 700 | 1 | |a Xian, Yong |4 aut | |
| 700 | 1 | |a Liu, Xi Chuan |4 aut | |
| 700 | 1 | |a Ying, XianJun |4 aut | |
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