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Enhanced O2 reduction on atomically thin Pt-based nanoshells by integrating surface facet, interfacial electronic, and substrate stabilization effects

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Abstract

To fully realize the commercial viability of Pt in fuel cells, the usage of scarce Pt must be reduced while the activity and durability in O2 reduction reaction (ORR) must be enhanced. Here we report a metallic stack design achieving these goals for ORR, based on atomically precise materials synthesis. Au@Pd@Pt nanostructures with atomically thin Pt shells and high-index surfaces form an excellent platform for integrating the effects of electronic structures, surface facets, and substrate stabilization to boost ORR performance. Au@Pd@Pt trisoctahedrons (TOH) achieve mass activity 6.1 times higher than that of commercial Pt/C and dramatically enhanced durability beyond 1.0 V vs. a reversible hydrogen electrode in oxidation potential. Meanwhile, Pt comprises only 3.2% of the nanostructures. To further improve the ORR activity and demonstrate the versatility of our strategy, we implement the same design in PtNi alloy electrocatalysts. The Au@Pd@PtNi TOHs exhibit mass activity 14.3 times higher than that of commercial Pt/C as well as excellent durability. This work demonstrates an alternative strategy for fabricating high-performance and low-cost catalysts, and highlights the importance of simultaneous surface and interfacial engineering with atomic precision in designing catalysts.

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Acknowledgements

This work was financially supported in part by the National Key R&D Program of China (No. 2017YFA- 0207301), the National Natural Science Foundation of China (NSFC) (Nos. 21471141, U1532135 and 21573212), CAS Key Research Program of Frontier Sciences (No. QYZDB-SSW-SLH018), CAS Interdisciplinary Innovation Team, Innovative Program of Development Foundation of Hefei Center for Physical Science and Technology (No. 2016FXCX003), Recruitment Program of Global Experts, CAS Hundred Talent Program, and Anhui Provincial Natural Science Foundation (Nos. 1608085QB24 and 1508085MB24). X.W. was supported by the MOST (No. 2016YFA0200602), the National Natural Science Foundation of China (NSFC) (Nos. 21421063, 51172223 and 21573204), Strategic Priority Research Program of CAS (No. XDB01020300), the National Key Basic Research Program (No. 2012CB922001), National Program for Support of Top-notch Young Professional, External Cooperation Program of BIC CAS (No. 211134KYSB20130017), and by USTCSCC, SCCAS, Tianjin, and Shanghai Supercomputer Centers. Depth-dependent XPS experiments were performed at the Photoemission Endstation at the BL10B beamline in the National Synchrotron Radiation Laboratory (NSRL) in Hefei, China.

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  1. Wei Ye and Zhongti Sun contributed equally to this work.

Authors and Affiliations

  1. Hefei National Laboratory for Physical Sciences at the Microscale, iChEM (Collaborative Innovation Center of Chemistry for Energy Materials), Synergetic Innovation of Quantum Information & Quantum Technology, School of Chemistry and Materials Science, CAS Center for Excellence in Nanoscience, and National Synchrotron Radiation Laboratory, University of Science and Technology of China, Hefei, 230026, China

    Wei Ye, Zhongti Sun, Chengming Wang, Mengshan Ye, Chenhao Ren, Ran Long, Xusheng Zheng, Junfa Zhu, Xiaojun Wu & Yujie Xiong

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  1. Wei Ye
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Correspondence to Chengming Wang, Xiaojun Wu or Yujie Xiong.

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Enhanced O2 reduction on atomically thin Pt-based nanoshells by integrating surface facet, interfacial electronic, and substrate stabilization effects

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Ye, W., Sun, Z., Wang, C. et al. Enhanced O2 reduction on atomically thin Pt-based nanoshells by integrating surface facet, interfacial electronic, and substrate stabilization effects. Nano Res. 11, 3313–3326 (2018). https://doi.org/10.1007/s12274-017-1891-x

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