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Single-atom tailoring of platinum nanocatalysts for high-performance multifunctional electrocatalysis

Li, Mufan and Duanmu, Kaining and Wan, Chengzhang and Cheng, Tao and Zhang, Liang and Dai, Sheng and Chen, Wenxin and Zhao, Zipeng and Li, Peng and Fei, Huilong and Zhu, Yuanming and Yu, Rong and Luo, Jun and Zang, Ketao and Lin, Zhaoyang and Ding, Mengning and Huang, Jin and Sun, Hongtao and Guo, Jinghua and Pan, Xiaoqing and Goddard, William A., III and Sautet, Philippe and Huang, Yu and Duan, Xiangfeng (2019) Single-atom tailoring of platinum nanocatalysts for high-performance multifunctional electrocatalysis. Nature Catalysis, 2 (6). pp. 495-503. ISSN 2520-1158.

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Platinum-based nanocatalysts play a crucial role in various electrocatalytic systems that are important for renewable, clean energy conversion, storage and utilization. However, the scarcity and high cost of Pt seriously limit the practical application of these catalysts. Decorating Pt catalysts with other transition metals offers an effective pathway to tailor their catalytic properties, but often at the sacrifice of the electrochemical active surface area (ECSA). Here we report a single-atom tailoring strategy to boost the activity of Pt nanocatalysts with minimal loss in surface active sites. By starting with PtNi alloy nanowires and using a partial electrochemical dealloying approach, we create single-nickel-atom-modified Pt nanowires with an optimum combination of specific activity and ECSA for the hydrogen evolution, methanol oxidation and ethanol oxidation reactions. The single-atom tailoring approach offers an effective strategy to optimize the activity of surface Pt atoms and enhance the mass activity for diverse reactions, opening a general pathway to the design of highly efficient and durable precious metal-based catalysts.

Item Type:Article
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URLURL TypeDescription ReadCube access InNature Catalysis : News & Views
Li, Mufan0000-0002-4575-4055
Cheng, Tao 0000-0003-4830-177X
Fei, Huilong0000-0002-4216-5810
Yu, Rong0000-0003-1687-3597
Luo, Jun0000-0001-5084-2087
Lin, Zhaoyang0000-0002-6474-7184
Guo, Jinghua0000-0002-8576-2172
Pan, Xiaoqing0000-0002-0965-8568
Goddard, William A., III0000-0003-0097-5716
Sautet, Philippe0000-0002-8444-3348
Duan, Xiangfeng0000-0002-4321-6288
Additional Information:© 2019 Springer Nature Publishing AG. Received 20 October 2018; Accepted 29 March 2019; Published 20 May 2019. Data availability: The data that support the findings of this study are available from the corresponding authors on reasonable request. Y.H. acknowledges support from the Office of Naval Research (grant no. N000141812155). X.D. acknowledges financial support from the National Science Foundation (grant no. 1800580). T.C. was supported by the Collaborative Innovation Center of Suzhou Nano Science & Technology, the Priority Academic Program Development of Jiangsu Higher Education Institutions (PAPD) and the 111 Project. W.A.G. was supported by the Joint Center for Artificial Photosynthesis, a DOE Energy Innovation Hub, supported through the Office of Science of the US Department of Energy under award no. DE‐SC0004993. This work used the Extreme Science and Engineering Discovery Environment (XSEDE) which is supported by National Science Foundation grant no. ACI‐1053575. J.L. acknowledges the National Key R&D Program of China (2017YFA0700104) and National Natural Science Foundation of China (51761165012). STEM experiments were conducted using the facilities in the Irvine Materials Research Institute (IMRI) at the University of California-Irvine. The authors thank S. Fakra for technical support for the EXAFS experiment. This research used resources of the Advanced Light Source, which is a DOE Office of Science User Facility under contract no. DEAC02-05CH11231. R.Y. acknowledges the National Natural Science Foundation of China (51525102, 51390475). Use of resources of the National Center for Electron Microscopy in Beijing is acknowledged. The calculations were performed on the Hoffman2 cluster at UCLA Institute for Digital Research and Education (IDRE) and the Extreme Science and Engineering Discovery Environment (XSEDE), which is supported by the National Science Foundation (grant no. ACI‐1053575). Author Contributions: X.D., Y.H. and P.S. supervised the project and designed the research. X.D., Y.H. and M.L. conceived the idea. M.L. and C.W. performed the synthesis, electrochemical tests and characterizations. K.D. and P.S. conceived and performed the DFT calculations. T.C. and W.G. performed the model simulations. L.Z. and W.C. performed XAS measurements and analysis. J.G. and W.C. provided expertise for XAS analysis. S.D. and X.P. performed the EELS and HAADF-STEM measurements. Z.Z., Y.Z., R.Y., J.L., K.Z. and Z.L. assisted with material characterizations. Z.Z., P.L., H.F., M.D., J.H. and H.S. assisted with catalytic measurements. M.L., K.D., C.W., P.S., Y.H. and X.D. co-wrote the paper. All authors discussed the results and commented on the manuscript. The authors declare no competing interests.
Funding AgencyGrant Number
Office of Naval Research (ONR)N000141812155
Suzhou Nano Science and TechnologyUNSPECIFIED
Priority Academic Program Development of Jiangsu Higher Education Institutions (PAPD)UNSPECIFIED
Joint Center for Artificial Photosynthesis (JCAP)UNSPECIFIED
Department of Energy (DOE)DE‐SC0004993
National Key R&D Program of China2017YFA0700104
National Natural Science Foundation of China51761165012
Department of Energy (DOE)DE-AC02-05CH11231
National Natural Science Foundation of China51525102
National Natural Science Foundation of China51390475
Subject Keywords:Electrocatalysis; Energy; Heterogeneous catalysis
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Issue or Number:6
Record Number:CaltechAUTHORS:20190327-094804466
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Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:94206
Deposited By: George Porter
Deposited On:04 Jun 2019 23:03
Last Modified:17 Jul 2019 16:11

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