CaltechAUTHORS
Published June 2019 | Version Supplemental Material
Journal Article Open

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

Creators

  • 1. ROR icon University of California, Los Angeles
  • 2. ROR icon California Institute of Technology
  • 3. ROR icon Soochow University
  • 4. ROR icon Lawrence Berkeley National Laboratory
  • 5. ROR icon University of California, Irvine
  • 6. ROR icon Tsinghua University
  • 7. ROR icon Tianjin University of Technology

Abstract

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.

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.

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Additional details

Identifiers

Eprint ID
94206
Resolver ID
CaltechAUTHORS:20190327-094804466

Related works

Describes
10.1038/s41929-019-0302-y (DOI)

Funding

Office of Naval Research (ONR)
N000141812155
NSF
CHE-1800580
Suzhou Nano Science and Technology
Priority Academic Program Development of Jiangsu Higher Education Institutions (PAPD)
111 Project
Joint Center for Artificial Photosynthesis (JCAP)
Department of Energy (DOE)
DE‐SC0004993
NSF
ACI‐1053575
National Key R&D Program of China
2017YFA0700104
National Natural Science Foundation of China
51761165012
Department of Energy (DOE)
DE-AC02-05CH11231
National Natural Science Foundation of China
51525102
National Natural Science Foundation of China
51390475
NSF
ACI‐1053575

Dates

Created
2019-06-04
Created from EPrint's datestamp field
Updated
2021-11-16
Created from EPrint's last_modified field

Caltech Custom Metadata

Caltech groups
JCAP
Other Numbering System Name
WAG
Other Numbering System Identifier
1339