Unconventional Bilateral Compressive Strained Ni-Ir Interface Synergistically Accelerates Alkaline Hydrogen Oxidation
The alkaline hydrogen oxidation reaction (HOR) involves the coupling of adsorbed hydrogen (Had) and hydroxyl (OHad) species and is thus orders of magnitude slower than that in acid media. According to the Sabatier principle, developing electrocatalysts with appropriate binding energy for both intermediates is vital to accelerating the HOR though it is still challenging. Herein, we propose an unconventional bilateral compressive strained Ni-Ir interface (Ni-Ir(BCS)) as efficient synergistic HOR sites. Density functional theory (DFT) simulations reveal that the bilateral compressive strain effect leads to the appropriate adsorption for both Had and OHad, enabling their coupling thermodynamically spontaneous and kinetically preferential. Such Ni-Ir(BCS) is experimentally achieved by embedding sub-nanometer Ir clusters in graphene-loaded high-density Ni nanocrystals (Ni-Ir(BCS)/G). As predicted, it exhibits a HOR mass activity of 7.95 and 2.88 times those of commercial Ir/C and Pt/C together with much enhanced CO tolerance, respectively, ranking among the most active state-of-the-art HOR catalysts. These results provide new insights into the rational design of advanced electrocatalysts involving coordinated adsorption and activation of multiple reactants.
| Medienart: |
E-Artikel |
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| Erscheinungsjahr: |
2023 |
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| Erschienen: |
2023 |
| Enthalten in: |
Zur Gesamtaufnahme - volume:145 |
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| Enthalten in: |
Journal of the American Chemical Society - 145(2023), 25 vom: 28. Juni, Seite 13805-13815 |
| Sprache: |
Englisch |
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| Beteiligte Personen: |
Tang, Tang [VerfasserIn] |
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| Links: |
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| Themen: |
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| Anmerkungen: |
Date Completed 28.06.2023 Date Revised 28.06.2023 published: Print-Electronic Citation Status PubMed-not-MEDLINE |
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| doi: |
10.1021/jacs.3c02487 |
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| funding: |
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| Förderinstitution / Projekttitel: |
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| PPN (Katalog-ID): |
NLM358191297 |
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| 245 | 1 | 0 | |a Unconventional Bilateral Compressive Strained Ni-Ir Interface Synergistically Accelerates Alkaline Hydrogen Oxidation |
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| 500 | |a Date Completed 28.06.2023 | ||
| 500 | |a Date Revised 28.06.2023 | ||
| 500 | |a published: Print-Electronic | ||
| 500 | |a Citation Status PubMed-not-MEDLINE | ||
| 520 | |a The alkaline hydrogen oxidation reaction (HOR) involves the coupling of adsorbed hydrogen (Had) and hydroxyl (OHad) species and is thus orders of magnitude slower than that in acid media. According to the Sabatier principle, developing electrocatalysts with appropriate binding energy for both intermediates is vital to accelerating the HOR though it is still challenging. Herein, we propose an unconventional bilateral compressive strained Ni-Ir interface (Ni-Ir(BCS)) as efficient synergistic HOR sites. Density functional theory (DFT) simulations reveal that the bilateral compressive strain effect leads to the appropriate adsorption for both Had and OHad, enabling their coupling thermodynamically spontaneous and kinetically preferential. Such Ni-Ir(BCS) is experimentally achieved by embedding sub-nanometer Ir clusters in graphene-loaded high-density Ni nanocrystals (Ni-Ir(BCS)/G). As predicted, it exhibits a HOR mass activity of 7.95 and 2.88 times those of commercial Ir/C and Pt/C together with much enhanced CO tolerance, respectively, ranking among the most active state-of-the-art HOR catalysts. These results provide new insights into the rational design of advanced electrocatalysts involving coordinated adsorption and activation of multiple reactants | ||
| 650 | 4 | |a Journal Article | |
| 700 | 1 | |a Liu, XiaoZhi |e verfasserin |4 aut | |
| 700 | 1 | |a Luo, Xuan |e verfasserin |4 aut | |
| 700 | 1 | |a Xue, Zhuangzhuang |e verfasserin |4 aut | |
| 700 | 1 | |a Pan, Hai-Rui |e verfasserin |4 aut | |
| 700 | 1 | |a Fu, Jiaju |e verfasserin |4 aut | |
| 700 | 1 | |a Yao, Ze-Cheng |e verfasserin |4 aut | |
| 700 | 1 | |a Jiang, Zhe |e verfasserin |4 aut | |
| 700 | 1 | |a Lyu, Zhen-Hua |e verfasserin |4 aut | |
| 700 | 1 | |a Zheng, Lirong |e verfasserin |4 aut | |
| 700 | 1 | |a Su, Dong |e verfasserin |4 aut | |
| 700 | 1 | |a Zhang, Jia-Nan |e verfasserin |4 aut | |
| 700 | 1 | |a Zhang, Liang |e verfasserin |4 aut | |
| 700 | 1 | |a Hu, Jin-Song |e verfasserin |4 aut | |
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| 856 | 4 | 0 | |u http://dx.doi.org/10.1021/jacs.3c02487 |3 Volltext |
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