期刊
NATURE COMMUNICATIONS
卷 12, 期 1, 页码 -出版社
NATURE PORTFOLIO
DOI: 10.1038/s41467-021-27145-3
关键词
-
资金
- Institute for Basic Science [IBS-R011-D1]
- National Research Foundation of Korea (NRF) - Ministry of Science, ICT & Future Planning (MSIP) [NRF-2019R1A2C2090249]
The study successfully prepared nickel-cobalt single-atom dimers as high-performance pH-universal H-2 evolution electrocatalysts, demonstrating improved HER kinetics under alkaline/acidic conditions through rational structural design and preparation methods.
While single, dispersed atoms enable efficient atomic utilization, controllably preparing single-atom dimers remains challenging. Here, authors prepare nickel-cobalt single-atom dimers as high-performance pH-universal H-2 evolution electrocatalysts. 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.
作者
我是这篇论文的作者
点击您的名字以认领此论文并将其添加到您的个人资料中。
推荐
暂无数据