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Experimental Sabatier plot for predictive design of active and stable Pt-alloy oxygen reduction reaction catalysts

Huang, Jin and Sementa, Luca and Liu, Zeyan and Barcaro, Giovanni and Feng, Miao and Liu, Ershuai and Jiao, Li and Xu, Mingjie and Leshchev, Denis and Lee, Sung-Joon and Li, Mufan and Wan, Chengzhang and Zhu, Enbo and Liu, Yang and Peng, Bosi and Duan, Xiangfeng and Goddard, William A., III and Fortunelli, Alessandro and Jia, Qingying and Huang, Yu (2022) Experimental Sabatier plot for predictive design of active and stable Pt-alloy oxygen reduction reaction catalysts. Nature Catalysis, 5 (6). pp. 513-523. ISSN 2520-1158. doi:10.1038/s41929-022-00797-0.

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A critical technological roadblock to the widespread adoption of proton-exchange membrane fuel cells is the development of highly active and durable platinum-based catalysts for accelerating the sluggish oxygen reduction reaction, which has largely relied on anecdotal discoveries so far. While the oxygen binding energy ∆E₀ has been frequently used as a theoretical descriptor for predicting the activity, there is no known descriptor for predicting durability. Here we developed a binary experimental descriptor that captures both the strain and Pt transition metal coupling contributions through X-ray absorption spectroscopy and directly correlated the binary experimental descriptor with the calculated ∆EO of the catalyst surface. This leads to an experimentally validated Sabatier plot to predict both the catalytic activity and stability for a wide range of Pt-alloy oxygen reduction reaction catalysts. Based on the binary experimental descriptor, we further designed an oxygen reduction reaction catalyst wherein high activity and stability are simultaneously achieved.

Item Type:Article
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URLURL TypeDescription ReadCube access
Liu, Zeyan0000-0001-9237-7603
Barcaro, Giovanni0000-0002-5520-5914
Jiao, Li0000-0002-1063-9313
Lee, Sung-Joon0000-0003-2368-4647
Li, Mufan0000-0002-4575-4055
Duan, Xiangfeng0000-0002-4321-6288
Goddard, William A., III0000-0003-0097-5716
Fortunelli, Alessandro0000-0001-5337-4450
Jia, Qingying0000-0002-4005-8894
Huang, Yu0000-0003-1793-0741
Additional Information:© The Author(s), under exclusive licence to Springer Nature Limited 2022. Received 12 July 2021; Accepted 26 April 2022; Published 09 June 2022. Y.H., Q.J., W.A.G. and X.D. gratefully acknowledge the support of the Office of Naval Research (award N000141812155). The XAS data were collected at beamlines 6-BM, 7-BM and 8-ID of the National Synchrotron Light Source II, a US Department of Energy Office of Science User Facility operated for the Department of Energy Office of Science by Brookhaven National Laboratory under contract no. DE-SC0012704. We acknowledge the use of facilities and instrumentation at the University of California Irvine Materials Research Institute, supported in part by the National Science Foundation Materials Research Science and Engineering Center programme through the University of California Irvine Center for Complex and Active Materials (DMR-2011967). We also thank the Electron Imaging Center of Nanomachines at the California NanoSystems Institute (CNSI) for TEM support. A.F. and W.A.G. received support from the National Science Foundation (CBET-1805022 and CBET-2005250). A.F., G.B. and L.S. gratefully acknowledge the contribution of the International Research Network on Nanoalloys Centre national de la recherche scientifique (CNRS) and computational support from the CINECA supercomputing centre within the Italian SuperComputing Resource Allocation (ISCRA) programme. Data availability: The atomic coordinates of the DFT calculation data and simulated XANES data are available in the Supplementary Data. The data that support the findings of this study are available from the corresponding authors upon reasonable request. Source data are provided with this paper. Contributions: J.H., M.F., M.L., Y.L., C.W., S.-J.L., B.P. and Z.L. conducted the synthesis of electrocatalysts, structural characterization and electrochemical experiments. M.X. and J.H. conducted the TEM and EDX characterizations. Q.J., E.L., L.J. and D.L. conducted the XAS studies. A.F., L.S., G.B., Q.J., J.H. and W.A.G. performed the modelling and data analyses. The project was conceived by Y.H. and supervised by Y.H. (project design, syntheses and evaluation of the catalysts); Q.J. (XAS studies); and A.F. and W.A.G. (computational studies). J.H., Y.H., Q.J. and A.F. wrote the original draught. J.H., Y.H., Q.J., A.F., W.A.G. and Z.L. revised the manuscript. The authors declare no competing interests. Peer review information: Nature Catalysis thanks Janis Timoshenko and the other, anonymous, reviewer(s) for their contribution to the peer review of this work.
Funding AgencyGrant Number
Office of Naval Research (ONR)N000141812155
Department of Energy (DOE)DE-SC0012704
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Issue or Number:6
Record Number:CaltechAUTHORS:20220615-944206900
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Official Citation:Huang, J., Sementa, L., Liu, Z. et al. Experimental Sabatier plot for predictive design of active and stable Pt-alloy oxygen reduction reaction catalysts. Nat Catal 5, 513–523 (2022).
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:115169
Deposited By: Tony Diaz
Deposited On:17 Jun 2022 20:17
Last Modified:14 Aug 2022 23:49

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