电催化剂
化学
催化作用
离解(化学)
过氧化氢
光化学
氧烷
吸附
X射线吸收精细结构
红外光谱学
选择性
价(化学)
吸收光谱法
光谱学
无机化学
物理化学
电化学
电极
有机化学
物理
量子力学
作者
Jinwen Hu,Wenzhe Shang,Cuncun Xin,Jingya Guo,Xusheng Cheng,Songlin Zhang,Suchan Song,Wei Liu,Feng Ju,Jungang Hou,Yantao Shi
标识
DOI:10.1002/ange.202304754
摘要
Abstract Understanding the nature of single‐atom catalytic sites and identifying their spectroscopic fingerprints are essential prerequisites for the rational design of target catalysts. Here, we apply correlated in situ X‐ray absorption and infrared spectroscopy to probe the edge‐site‐specific chemistry of Co−N−C electrocatalyst during the oxygen reduction reaction (ORR) operation. The unique edge‐hosted architecture affords single‐atom Co site remarkable structural flexibility with adapted dynamic oxo adsorption and valence state shuttling between Co (2−δ)+ and Co 2+ , in contrast to the rigid in‐plane embedded Co 1 −N x counterpart. Theoretical calculations demonstrate that the synergistic interplay of in situ reconstructed Co 1 −N 2 ‐oxo with peripheral oxygen groups gives a rise to the near‐optimal adsorption of *OOH intermediate and substantially increases the activation barrier for its dissociation, accounting for a robust acidic ORR activity and 2e − selectivity for H 2 O 2 production.
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