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Stabilizing Highly Active Ru Sites by Suppressing Lattice Oxygen Participation in Acidic Water Oxidation

Wen, Yunzhou and Chen, Peining and Wang, Lu and Li, Shangyu and Wang, Ziyun and Abed, Jehad and Mao, Xinnan and Min, Yimeng and Dinh, Cao Thang and De Luna, Phil and Huang, Rui and Zhang, Longsheng and Wang, Lie and Wang, Liping and Nielsen, Robert J. and Li, Huihui and Zhuang, Taotao and Ke, Changchun and Voznyy, Oleksandr and Hu, Yongfeng and Li, Youyong and Goddard, William A., III and Zhang, Bo and Peng, Huisheng and Sargent, Edward H. (2021) Stabilizing Highly Active Ru Sites by Suppressing Lattice Oxygen Participation in Acidic Water Oxidation. Journal of the American Chemical Society, 143 (17). pp. 6482-6490. ISSN 0002-7863. doi:10.1021/jacs.1c00384. https://resolver.caltech.edu/CaltechAUTHORS:20210503-115704310

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Abstract

In hydrogen production, the anodic oxygen evolution reaction (OER) limits the energy conversion efficiency and also impacts stability in proton-exchange membrane water electrolyzers. Widely used Ir-based catalysts suffer from insufficient activity, while more active Ru-based catalysts tend to dissolve under OER conditions. This has been associated with the participation of lattice oxygen (lattice oxygen oxidation mechanism (LOM)), which may lead to the collapse of the crystal structure and accelerate the leaching of active Ru species, leading to low operating stability. Here we develop Sr–Ru–Ir ternary oxide electrocatalysts that achieve high OER activity and stability in acidic electrolyte. The catalysts achieve an overpotential of 190 mV at 10 mA cm⁻² and the overpotential remains below 225 mV following 1,500 h of operation. X-ray absorption spectroscopy and ¹⁸O isotope-labeled online mass spectroscopy studies reveal that the participation of lattice oxygen during OER was suppressed by interactions in the Ru–O–Ir local structure, offering a picture of how stability was improved. The electronic structure of active Ru sites was modulated by Sr and Ir, optimizing the binding energetics of OER oxo-intermediates.


Item Type:Article
Related URLs:
URLURL TypeDescription
https://doi.org/10.1021/jacs.1c00384DOIArticle
ORCID:
AuthorORCID
Wang, Lu0000-0003-0552-1385
Wang, Ziyun0000-0002-2817-8367
Dinh, Cao Thang0000-0001-9641-9815
De Luna, Phil0000-0002-7729-8816
Nielsen, Robert J.0000-0002-7962-0186
Li, Huihui0000-0002-3823-1010
Voznyy, Oleksandr0000-0002-8656-5074
Li, Youyong0000-0002-5248-2756
Goddard, William A., III0000-0003-0097-5716
Zhang, Bo0000-0002-7853-979X
Peng, Huisheng0000-0003-3746-8494
Sargent, Edward H.0000-0003-0396-6495
Additional Information:© 2021 American Chemical Society. Received: January 12, 2021. This work was supported by MOST (2016YFA0203302), NSFC (21634003, 51573027, 21875042, 21805044, and 21771170), STCSM (16JC1400702, 18QA140080, and 19QA140080), SHMEC (2017-01-07-00-07-E00062), and Yanchang Petroleum Group. This work was also supported by the Program for Eastern Scholars at Shanghai Institutions. This work was supported by the Ontario Research Fund - Research Excellence Program, NSERC, and the CIFAR Bio-Inspired Solar Energy program. The ex situ XAFS was carried out at the BL14W1 beamline, Shanghai Synchrotron Radiation Facility (SSRF). The in situ Ru K-edge and Ir L₃-edge XAFS was measured at the 1W1B beamline, Beijing Synchrotron Radiation Facility (BSRF). The in situ Ru L₃-edge measurements were carried out at the soft X-ray microcharacterization beamline (SXRMB) in Canadian Light Source (CLS). The STEM imaging part of this research was completed at the Analytical and Testing Center, Northwestern Polytechnical University. The Caltech studies were supported by the Joint Center for Artificial Photosynthesis, a DOE Energy Innovation Hub, supported through the Office of Science of the U.S. Department of Energy under Award DE-SC0004993, by NSF (CBET-1805022), and by DOE AMO. Author Contributions: Y.W., P.C., L.W., and S.L. contributed equally to this work. The authors declare no competing financial interest.
Group:JCAP
Funders:
Funding AgencyGrant Number
Ministry of Science and Technology (Taipei)2016YFA0203302
National Natural Science Foundation of China21634003
National Natural Science Foundation of China51573027
National Natural Science Foundation of China21875042
National Natural Science Foundation of China21805044
National Natural Science Foundation of China21771170
Shanghai Science and Technology Committee (STCSM)16JC1400702
Shanghai Science and Technology Committee (STCSM)18QA140080
Shanghai Science and Technology Committee (STCSM)19QA140080
Shanghai Municipal Education2017-01-07-00-07-E00062
Yanchang Petroleum GroupUNSPECIFIED
Shanghai InstitutionsUNSPECIFIED
Ontario Research Fund-Research ExcellenceUNSPECIFIED
Natural Sciences and Engineering Research Council of Canada (NSERC)UNSPECIFIED
Canadian Institute for Advanced Research (CIFAR)UNSPECIFIED
Joint Center for Artificial Photosynthesis (JCAP)UNSPECIFIED
Department of Energy (DOE)DE-SC0004993
NSFCBET-1805022
Subject Keywords:Oxides, Radiology, Electrocatalysts, Catalysts, Transition metals
Other Numbering System:
Other Numbering System NameOther Numbering System ID
WAG1422
Issue or Number:17
DOI:10.1021/jacs.1c00384
Record Number:CaltechAUTHORS:20210503-115704310
Persistent URL:https://resolver.caltech.edu/CaltechAUTHORS:20210503-115704310
Official Citation:Stabilizing Highly Active Ru Sites by Suppressing Lattice Oxygen Participation in Acidic Water Oxidation. Yunzhou Wen, Peining Chen, Lu Wang, Shangyu Li, Ziyun Wang, Jehad Abed, Xinnan Mao, Yimeng Min, Cao Thang Dinh, Phil De Luna, Rui Huang, Longsheng Zhang, Lie Wang, Liping Wang, Robert J. Nielsen, Huihui Li, Taotao Zhuang, Changchun Ke, Oleksandr Voznyy, Yongfeng Hu, Youyong Li, William A. Goddard III, Bo Zhang, Huisheng Peng, and Edward H. Sargent. Journal of the American Chemical Society 2021 143 (17), 6482-6490; DOI: 10.1021/jacs.1c00384
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:108933
Collection:CaltechAUTHORS
Deposited By: George Porter
Deposited On:05 May 2021 17:47
Last Modified:06 Jun 2021 02:52

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