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Shin, Tae Joo
UNIST Synchrotron Radiation Research Laboratory
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  • Synchrotron Radiation Application Researches

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

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Title
Reversible Ligand Exchange in Atomically Dispersed Catalysts for Modulating the Activity and Selectivity of the Oxygen Reduction Reaction
Author
Kim, Jae HyungShin, DongyupKim, JinjongLim, June SungPaidi, Vinod K.Shin, Tae JooJeong, Hu YoungLee, Kug-SeungKim, HyungjunJoo, Sang Hoon
Issue Date
2021-09
Publisher
WILEY-V C H VERLAG GMBH
Citation
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, v.60, no.37, pp.20528 - 20534
Abstract
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.
URI
https://scholarworks.unist.ac.kr/handle/201301/53539
URL
https://onlinelibrary.wiley.com/doi/10.1002/anie.202108439
DOI
10.1002/anie.202108439
ISSN
1433-7851
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