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Tuning Single-Atom Dopants on Manganese Oxide for Selective Electrocatalytic Cyclooctene Epoxidation

Chung, Minju and Jin, Kyoungsuk and Zeng, Joy S. and Ton, Thu N. and Manthiram, Karthish (2022) Tuning Single-Atom Dopants on Manganese Oxide for Selective Electrocatalytic Cyclooctene Epoxidation. Journal of the American Chemical Society, 144 (38). pp. 17416-17422. ISSN 0002-7863. doi:10.1021/jacs.2c04711.

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Selective and efficient electrocatalysts are imperative for the successful deployment of electrochemistry toward synthetic applications. In this study, we used galvanic replacement reactions to synthesize iridium-decorated manganese oxide nanoparticles, which showed a cyclooctene epoxidation partial current density of 10.5 ± 2.8 mA/cm² and a Faradaic efficiency of 46 ± 4%. Results from operando X-ray absorption spectroscopy suggest that manganese leaching from the nanoparticles during galvanic replacement introduces lattice vacancies that make the nanoparticles more susceptible to metal oxidation and catalyst reconstruction under an applied anodic potential. This results in an increased presence of electrophilic oxygen atoms on the catalyst surface during reaction conditions, which may contribute to the enhanced electrocatalytic activity toward cyclooctene epoxidation.

Item Type:Article
Related URLs:
URLURL TypeDescription
Chung, Minju0000-0003-4359-7508
Jin, Kyoungsuk0000-0003-3009-6691
Zeng, Joy S.0000-0002-3443-3504
Ton, Thu N.0000-0003-0134-2435
Manthiram, Karthish0000-0001-9260-3391
Additional Information:This research was supported by the U.S. Department of Energy (DOE) Office of Science, Office of Basic Energy Sciences, Catalysis Science Program, under Award No. DE-SC0020999. This research used resources of the National Synchrotron Light Source II, a U.S. DOE Office of Science User Facility operated for the DOE Office of Science by Brookhaven National Laboratory under Contract No. DE-SC0012704. This research also used resources of the Advanced Light Source, which is a DOE Office of Science User Facility under Contract No. DE-AC02-05CH11231. The authors are grateful to Eli Stavitski, Denis Leshchev, Steven Ehrlich, Lu Ma, and Sirine Fakra for their help in operating XAS experiments. This work was performed in part at the Harvard University Center for Nanoscale Systems (CNS), a member of the National Nanotechnology Coordinated Infrastructure Network (NNCI), which is supported by the National Science Foundation under NSF Award No. ECCS-2025158. The authors appreciate Jules Gardner at CNS for taking HAADF-STEM images. M.C. gratefully acknowledges the support of the Kwanjeong Fellowship.
Funding AgencyGrant Number
Kwanjeong Educational FoundationUNSPECIFIED
Department of Energy (DOE)DE-SC0020999
Department of Energy (DOE)DE-SC0012704
Department of Energy (DOE)DE-AC02-05CH11231
Kwanjeong Educational FoundationUNSPECIFIED
Issue or Number:38
Record Number:CaltechAUTHORS:20221011-128968500.23
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Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:117361
Deposited By: Research Services Depository
Deposited On:12 Oct 2022 23:43
Last Modified:12 Oct 2022 23:43

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