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In Situ Identifying the Dynamic Structure behind Activity of Atomically Dispersed Platinum Catalyst toward Hydrogen Evolution Reaction
Author(s) -
Wang Jiali,
Tan HuiYing,
Kuo TsungRong,
Lin ShengChih,
Hsu ChiaShuo,
Zhu Yanping,
Chu YouChiuan,
Chen Tai Lung,
Lee JyhFu,
Chen Hao Ming
Publication year - 2021
Publication title -
small
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 3.785
H-Index - 236
eISSN - 1613-6829
pISSN - 1613-6810
DOI - 10.1002/smll.202005713
Subject(s) - tafel equation , catalysis , platinum , cyclic voltammetry , materials science , x ray photoelectron spectroscopy , electrochemistry , transition metal , chemical engineering , chemistry , electrode , organic chemistry , engineering
Single‐atom catalysts (SAs) with the maximum atom utilization and breakthrough activities toward hydrogen evolution reaction (HER) have attracted considerable research interests. Uncovering the nature of single‐atom metal centers under operating electrochemical condition is highly significant for improving their catalytic performance, yet is poorly understood in most studies. Herein, Pt single atoms anchoring on the nitrogen–carbon substrate (Pt SA /N–C) as a model system are utilized to investigate the dynamic structure of Pt single‐atom centers during the HER process. Via in situ/operando synchrotron X‐ray absorption spectroscopy and X‐ray photoelectron spectroscopy, an intriguing structural reconstruction at atomic level is identified in the Pt SA /N–C when it is subjected to the repetitive linear sweep voltammetry and cyclic voltammetry scanning. It demonstrates that the PtN bonding tends to be weakened under cathodic potentials, which induces some Pt single atoms to dynamically aggregate into forming small clusters during the HER reaction. More importantly, experimental evidence and/or indicator is offered to correlate the observed Tafel slope with the dynamic structure of Pt catalysts. This work provides an evident understanding of SAs under electrocatalytic process and offers informative insights into constructing efficient catalysts at atomic level for electrochemical water‐splitting system.