Boosted hydrogen evolution kinetics of heteroatom-doped carbons with isolated Zn as an accelerant

• 成果类型: Article
• 署名作者: Li, Yang; Zuo, Shouwei; Wei, Fen; Chen, Cailing; Zhang, Guikai; Zhao, Xiaojuan; Wu, Zhipeng; Wang, Sibo; Zhou, Wei; Rueping, Magnus; Han, Yu; Zhang, Huabin
• 署名单位: King Abdullah University of Science & Technology; Fuzhou University; King Abdullah University of Science & Technology; Chinese Academy of Sciences; Institute of High Energy Physics, CAS; Tianjin University
• 刊物名称: PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
• ISSN/ISSBN: 0027-14955
• DOI: 10.1073/pnas.2315362121
• 发表日期: 2024-01-30
• 关键词: total-energy calculations; oxygen reduction

摘要

Carbon - based single - atom catalysts, a promising candidate in electrocatalysis, offer insights into electron- donating effects of metal center on adjacent atoms. Herein, we present a practical strategy to rationally design a model catalyst with a single zinc (Zn) atom coordinated with nitrogen and sulfur atoms in a multilevel carbon matrix. The Zn site exhibits an atomic interface configuration of ZnN4S1, where Zn's electron injection effect enables thermal- neutral hydrogen adsorption on neighboring atoms, pushing the activity boundaries of carbon electrocatalysts toward electrochemical hydrogen evolution to an unprecedented level. Experimental and theoretical analyses confirm the low- barrier Volmer-Tafel mechanism of proton reduction, while the multishell hollow structures facilitate the hydrogen evolution even at high current intensities. This work provides insights for understanding the actual active species during hydrogen evolution reaction and paves the way for designing high- performance electrocatalysts.