Moving beyond bimetallic-alloy to single-atom dimer atomic-interface for all-pH hydrogen evolution
© 2021. The Author(s)..
Single-atom-catalysts (SACs) afford a fascinating activity with respect to other nanomaterials for hydrogen evolution reaction (HER), yet the simplicity of single-atom center limits its further modification and utilization. Obtaining bimetallic single-atom-dimer (SAD) structures can reform the electronic structure of SACs with added atomic-level synergistic effect, further improving HER kinetics beyond SACs. However, the synthesis and identification of such SAD structure remains conceptually challenging. Herein, systematic first-principle screening reveals that the synergistic interaction at the NiCo-SAD atomic interface can upshift the d-band center, thereby, facilitate rapid water-dissociation and optimal proton adsorption, accelerating alkaline/acidic HER kinetics. Inspired by theoretical predictions, we develop a facile strategy to obtain NiCo-SAD on N-doped carbon (NiCo-SAD-NC) via in-situ trapping of metal ions followed by pyrolysis with precisely controlled N-moieties. X-ray absorption spectroscopy indicates the emergence of Ni-Co coordination at the atomic-level. The obtained NiCo-SAD-NC exhibits exceptional pH-universal HER-activity, demanding only 54.7 and 61 mV overpotentials at -10 mA cm-2 in acidic and alkaline media, respectively. This work provides a facile synthetic strategy for SAD catalysts and sheds light on the fundamentals of structure-activity relationships for future applications.
| Medienart: |
E-Artikel |
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| Erscheinungsjahr: |
2021 |
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| Erschienen: |
2021 |
| Enthalten in: |
Zur Gesamtaufnahme - volume:12 |
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| Enthalten in: |
Nature communications - 12(2021), 1 vom: 19. Nov., Seite 6766 |
| Sprache: |
Englisch |
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| Beteiligte Personen: |
Kumar, Ashwani [VerfasserIn] |
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| Anmerkungen: |
Date Revised 04.12.2021 published: Electronic Citation Status PubMed-not-MEDLINE |
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| doi: |
10.1038/s41467-021-27145-3 |
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| funding: |
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| Förderinstitution / Projekttitel: |
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NLM333369270 |
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| 520 | |a © 2021. The Author(s). | ||
| 520 | |a Single-atom-catalysts (SACs) afford a fascinating activity with respect to other nanomaterials for hydrogen evolution reaction (HER), yet the simplicity of single-atom center limits its further modification and utilization. Obtaining bimetallic single-atom-dimer (SAD) structures can reform the electronic structure of SACs with added atomic-level synergistic effect, further improving HER kinetics beyond SACs. However, the synthesis and identification of such SAD structure remains conceptually challenging. Herein, systematic first-principle screening reveals that the synergistic interaction at the NiCo-SAD atomic interface can upshift the d-band center, thereby, facilitate rapid water-dissociation and optimal proton adsorption, accelerating alkaline/acidic HER kinetics. Inspired by theoretical predictions, we develop a facile strategy to obtain NiCo-SAD on N-doped carbon (NiCo-SAD-NC) via in-situ trapping of metal ions followed by pyrolysis with precisely controlled N-moieties. X-ray absorption spectroscopy indicates the emergence of Ni-Co coordination at the atomic-level. The obtained NiCo-SAD-NC exhibits exceptional pH-universal HER-activity, demanding only 54.7 and 61 mV overpotentials at -10 mA cm-2 in acidic and alkaline media, respectively. This work provides a facile synthetic strategy for SAD catalysts and sheds light on the fundamentals of structure-activity relationships for future applications | ||
| 650 | 4 | |a Journal Article | |
| 700 | 1 | |a Bui, Viet Q |e verfasserin |4 aut | |
| 700 | 1 | |a Lee, Jinsun |e verfasserin |4 aut | |
| 700 | 1 | |a Wang, Lingling |e verfasserin |4 aut | |
| 700 | 1 | |a Jadhav, Amol R |e verfasserin |4 aut | |
| 700 | 1 | |a Liu, Xinghui |e verfasserin |4 aut | |
| 700 | 1 | |a Shao, Xiaodong |e verfasserin |4 aut | |
| 700 | 1 | |a Liu, Yang |e verfasserin |4 aut | |
| 700 | 1 | |a Yu, Jianmin |e verfasserin |4 aut | |
| 700 | 1 | |a Hwang, Yosep |e verfasserin |4 aut | |
| 700 | 1 | |a Bui, Huong T D |e verfasserin |4 aut | |
| 700 | 1 | |a Ajmal, Sara |e verfasserin |4 aut | |
| 700 | 1 | |a Kim, Min Gyu |e verfasserin |4 aut | |
| 700 | 1 | |a Kim, Seong-Gon |e verfasserin |4 aut | |
| 700 | 1 | |a Park, Gyeong-Su |e verfasserin |4 aut | |
| 700 | 1 | |a Kawazoe, Yoshiyuki |e verfasserin |4 aut | |
| 700 | 1 | |a Lee, Hyoyoung |e verfasserin |4 aut | |
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