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Selectively anchoring single atoms on specific sites of supports for improved oxygen evolution
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Selectively anchoring single atoms on specific sites of supports for improved oxygen evolution
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Journal Article
Selectively anchoring single atoms on specific sites of supports for improved oxygen evolution
2022
Overview
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 (Ir
1
/T
O
–CoOOH) and oxygen vacancies (Ir
1
/V
O
–CoOOH) on defective CoOOH surface to investigate how the anchoring sites modulate catalytic performance. The oxygen evolution activities of Ir
1
/T
O
–CoOOH and Ir
1
/V
O
–CoOOH are improved relative to CoOOH through different mechanisms. For Ir
1
/T
O
–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 Ir
1
/V
O
–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.
While single-atom catalysts offer well-defined structures, the homogeneity of the active sites is determined by localized coordination environments. Here, authors anchor Ir single atoms onto different sites on CoOOH and show how their distinct coordinations activate oxygen-evolving electrocatalysis
