Unveiling the Dynamic Migration and Aggregation Behaviors of Atomic Clusters on Defective Carbons for Efficient Catalyst Design

作者：Qilong Wu, Haiyuan Zou, Yun Han, Liyun Wu, Shuai Ma, Lachlan Smillie, Xiaozhi Su, Yongheng Chu, Hao Deng, Xin Mao, Fangfang Zhu, Dongdong Zhang, Fu‐Chen Liu, Shaohua Shen, Jiong‐Peng Zhao, Lele Duan, Aijun Du, Jun Chen, Xiangdong Yao · 发表于：Advanced Functional Materials · 年份：2025 · DOI：10.1002/adfm.202518284 · 被引用次数：4 · 研究领域：Catalytic Processes in Materials Science、Graphene research and applications、Catalysis and Oxidation Reactions

Abstract Carbon‐supported atomic clusters (CACs) have been demonstrated to have significant potential for heterogeneous catalysis; however, their synthesis remains a “black box” process due to the complexities associated with metal migration, aggregation, and carbon structural reconstruction behaviors. Herein, the general formation mechanism of metal clusters is uncovered in defective graphene oxide (DGO) during pyrolysis. First, multiple coordination modes of platinum (Pt) atoms on DGO provide opportunities for their temperature‐dependent release, where the highly thermally stable sites (Pt─C 2 on edge defect) serve as migration termini and nucleation centers. Notably, the size (from 1.5 to 0.99 nm) of Pt CACs can be precisely manipulated by increasing the defect densities of DGO. Moreover, the dynamic evolution process is monitored using multiple in situ technologies, revealing a more intense structural reconstitution of DGO compared to that of graphene oxide, which, in turn, limits the aggregation of metal clusters. Electrocatalytic results revealed a negative relationship between the size of Pt CACs and their hydrogen evolution performance, where the Pt CACs (size: 0.99 nm) exhibit a high mass activity in HER that is 32 times higher than that of the commercial 20% Pt/C catalyst. This work provides a paradigm for establishing the underlying architecture of CAC synthesis methodology.