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Moving beyond bimetallic-alloy to single-atom dimer atomic-interface for all-pH hydrogen evolution

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Title
Moving beyond bimetallic-alloy to single-atom dimer atomic-interface for all-pH hydrogen evolution
Author(s)
Ashwani Kumar; Viet Q. Bui; Jinsun Lee; Lingling Wang; Amol R. Jadhav; Xinghui Liu; Xiaodong Shao; Yang Liu; Jianmin Yu; Yosep Hwang; Huong T. D. Bui; Sara Ajmal; Kim, Min Gyu; Kim, Seong-Gon; Park, Gyeong-Su; Kawazoe, Yoshiyuki; Hyoyoung Lee
Publication Date
2021-11-19
Journal
Nature Communications, v.12, no.1
Publisher
Nature Research
Abstract
© 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.
URI
https://pr.ibs.re.kr/handle/8788114/10999
DOI
10.1038/s41467-021-27145-3
ISSN
2041-1723
Appears in Collections:
Center for Integrated Nanostructure Physics(나노구조물리 연구단) > 1. Journal Papers (저널논문)
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