Reversible Ligand Exchange in Atomically Dispersed Catalysts for Modulating the Activity and Selectivity of the Oxygen Reduction Reaction

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Rational control of the coordination environment of atomically dispersed catalysts is pivotal to achieve desirable catalytic reactivity. We report the reversible control of coordination structure in atomically dispersed electrocatalysts via ligand exchange reactions to reversibly modulate their reactivity for oxygen reduction reaction (ORR). The CO-ligated atomically dispersed Rh catalyst exhibited ca. 30-fold higher ORR activity than the NHx-ligated catalyst, whereas the latter showed three times higher H2O2 selectivity than the former. Post-treatments of the catalysts with CO or NH3 allowed the reversible exchange of CO and NHx ligands, which reversibly tuned oxidation state of metal centers and their ORR activity and selectivity. DFT calculations revealed that more reduced oxidation state of CO-ligated Rh site could further stabilize the *OOH intermediate, facilitating the two- and four-electron pathway ORR. The reversible ligand exchange reactions were generalized to Ir- and Pt-based catalysts.
Publisher
WILEY-V C H VERLAG GMBH
Issue Date
2021-09
Language
English
Article Type
Article
Citation

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, v.60, no.37, pp.20528 - 20534

ISSN
1433-7851
DOI
10.1002/anie.202108439
URI
http://hdl.handle.net/10203/287618
Appears in Collection
CH-Journal Papers(저널논문)
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