Selectively anchoring single atoms on specific sites of supports for improved oxygen evolution

  • 影响因子:14.919
  • DOI码:10.1038/s41467-022-30148-3
  • 发表刊物:Nat. Commun.
  • 关键字:catalysis, catalyst, chemical bonding, oxygen
  • 摘要:The homogeneity of single-atom catalysts is only to the first-order approximation when all isolated metal centers interact identically with the support. Since the realistic support with various topologies or defects offers diverse coordination environments, realizing real homogeneity requires precise control over the anchoring sites. In this work, we selectively anchor Ir single atoms onto the three-fold hollow sites (Ir1/TO–CoOOH) and oxygen vacancies (Ir1/VO–CoOOH) on defective CoOOH surface to investigate how the anchoring sites modulate catalytic performance. The oxygen evolution activities of Ir1/TO–CoOOH and Ir1/VO–CoOOH are improved relative to CoOOH through different mechanisms. For Ir1/TO–CoOOH, the strong electronic interaction between single-atom Ir and the support modifies the electronic structure of the active center for stronger electronic affinity to intermediates. For Ir1/VO–CoOOH, a hydrogen bonding is formed between the coordinated oxygen of single-atom Ir center and the oxygenated intermediates, which stabilizes the intermediates and lowers the energy barrier of the rate-determining step.
  • 合写作者:Ruyang Wang, Sunpei Hu, Hongliang Li, Ming Zuo
  • 第一作者:Zhirong Zhang, Chen Feng, Dongdi Wang
  • 通讯作者:Shiming Zhou,bYuan Kong, Jun Bao, Jie Zeng
  • 文献类型:SCI
  • 卷号:13
  • 期号:1
  • 页面范围:2473
  • 是否译文:
  • 发表时间:2022/05/05
  • 发布期刊链接:https://www.nature.com/articles/s41467-022-30148-3