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Title: Control of Architecture in Rhombic Dodecahedral Pt–Ni Nanoframe Electrocatalysts

Abstract

Platinum-based alloys are known to demonstrate advanced properties in electrochemical reactions that are relevant for proton exchange membrane fuel cells and electrolyzers. Further development of Pt alloy electrocatalysts relies on the design of architectures with highly active surfaces and optimized utilization of the expensive elpment, Pt. Here, we show that the three-dimensional Pt anisotropy of Pt-Ni rhombic dodecahedra can be tuned by controlling the ratio between Pt and Ni precursors such that either a completely hollow nanoframe or a new architecture, the excavated nanoframe, can be obtained. The excavated nanoframe showed similar to 10 times higher specific and similar to 6 times higher mass activity for the oxygen reduction reaction than Pt/C, and twice the mass activity of the hollow nanoframe. The high activity is attributed to enhanced Ni content in the near-surface region and the extended two-dimensional sheet structure within the nanoframe that minimizes the number of buried Pt sites.

Authors:
ORCiD logo [1];  [2]; ORCiD logo [3];  [4]; ORCiD logo [2]; ORCiD logo [2];  [2];  [5];  [5];  [4];  [4]; ORCiD logo [6]
  1. Department of Chemistry, University of California, Berkeley, Berkeley, California 94720, United States; Materials Science Division, Lawrence Berkeley National Laboratory, Berkeley, California 94720, United States
  2. Department of Chemistry, University of California, Berkeley, Berkeley, California 94720, United States
  3. Department of Materials Science and Engineering, University of California, Berkeley, Berkeley, California 94720, United States
  4. Materials Science Division, Argonne National Laboratory, Argonne, Illinois 60439, United States
  5. Center for Nanophase Materials Sciences, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37831, United States
  6. Department of Chemistry, University of California, Berkeley, Berkeley, California 94720, United States; Materials Science Division, Lawrence Berkeley National Laboratory, Berkeley, California 94720, United States; Department of Materials Science and Engineering, University of California, Berkeley, Berkeley, California 94720, United States; Kavli Energy NanoSciences Institute, Berkeley, California 94720, United States
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Energy Efficiency and Renewable Energy (EERE), Fuel Cell Technologies Office (EE-3F)
OSTI Identifier:
1395869
DOE Contract Number:
AC02-06CH11357
Resource Type:
Journal Article
Resource Relation:
Journal Name: Journal of the American Chemical Society; Journal Volume: 139; Journal Issue: 34
Country of Publication:
United States
Language:
English

Citation Formats

Becknell, Nigel, Son, Yoonkook, Kim, Dohyung, Li, Dongguo, Yu, Yi, Niu, Zhiqiang, Lei, Teng, Sneed, Brian T., More, Karren L., Markovic, Nenad M., Stamenkovic, Vojislav R., and Yang, Peidong. Control of Architecture in Rhombic Dodecahedral Pt–Ni Nanoframe Electrocatalysts. United States: N. p., 2017. Web. doi:10.1021/jacs.7b05584.
Becknell, Nigel, Son, Yoonkook, Kim, Dohyung, Li, Dongguo, Yu, Yi, Niu, Zhiqiang, Lei, Teng, Sneed, Brian T., More, Karren L., Markovic, Nenad M., Stamenkovic, Vojislav R., & Yang, Peidong. Control of Architecture in Rhombic Dodecahedral Pt–Ni Nanoframe Electrocatalysts. United States. doi:10.1021/jacs.7b05584.
Becknell, Nigel, Son, Yoonkook, Kim, Dohyung, Li, Dongguo, Yu, Yi, Niu, Zhiqiang, Lei, Teng, Sneed, Brian T., More, Karren L., Markovic, Nenad M., Stamenkovic, Vojislav R., and Yang, Peidong. 2017. "Control of Architecture in Rhombic Dodecahedral Pt–Ni Nanoframe Electrocatalysts". United States. doi:10.1021/jacs.7b05584.
@article{osti_1395869,
title = {Control of Architecture in Rhombic Dodecahedral Pt–Ni Nanoframe Electrocatalysts},
author = {Becknell, Nigel and Son, Yoonkook and Kim, Dohyung and Li, Dongguo and Yu, Yi and Niu, Zhiqiang and Lei, Teng and Sneed, Brian T. and More, Karren L. and Markovic, Nenad M. and Stamenkovic, Vojislav R. and Yang, Peidong},
abstractNote = {Platinum-based alloys are known to demonstrate advanced properties in electrochemical reactions that are relevant for proton exchange membrane fuel cells and electrolyzers. Further development of Pt alloy electrocatalysts relies on the design of architectures with highly active surfaces and optimized utilization of the expensive elpment, Pt. Here, we show that the three-dimensional Pt anisotropy of Pt-Ni rhombic dodecahedra can be tuned by controlling the ratio between Pt and Ni precursors such that either a completely hollow nanoframe or a new architecture, the excavated nanoframe, can be obtained. The excavated nanoframe showed similar to 10 times higher specific and similar to 6 times higher mass activity for the oxygen reduction reaction than Pt/C, and twice the mass activity of the hollow nanoframe. The high activity is attributed to enhanced Ni content in the near-surface region and the extended two-dimensional sheet structure within the nanoframe that minimizes the number of buried Pt sites.},
doi = {10.1021/jacs.7b05584},
journal = {Journal of the American Chemical Society},
number = 34,
volume = 139,
place = {United States},
year = 2017,
month = 8
}