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Title: Highly Crystalline Multimetallic Nanoframes with Three-Dimensional Electrocatalytic Surfaces

Control of structure at the atomic level can precisely and effectively tune catalytic properties of materials, enabling enhancement in both activity and durability. We synthesized a highly active and durable class of electrocatalysts by exploiting the structural evolution of platinum-nickel (Pt-Ni) bimetallic nanocrystals. The starting material, crystalline PtNi 3 polyhedra, transforms in solution by interior erosion into Pt 3Ni nanoframes with surfaces that offer three-dimensional molecular accessibility. The edges of the Pt-rich PtNi 3 polyhedra are maintained in the final Pt 3Ni nanoframes. Both the interior and exterior catalytic surfaces of this open-framework structure are composed of the nanosegregated Pt-skin structure, which exhibits enhanced oxygen reduction reaction (ORR) activity. The Pt 3Ni nanoframe catalysts achieved a factor of 36 enhancement in mass activity and a factor of 22 enhancement in specific activity, respectively, for this reaction (relative to state-of-the-art platinum-carbon catalysts) during prolonged exposure to reaction conditions.
Authors:
 [1] ;  [2] ;  [3] ;  [3] ;  [3] ;  [4] ;  [2] ;  [2] ;  [5] ;  [5] ;  [6] ;  [6] ;  [7] ;  [2] ;  [3] ;  [8] ;  [2]
  1. Univ. of California, Berkeley, CA (United States). Dept. of Chemistry; Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Materials Science Division; Tsinghua Univ., Beijing (China). Dept. of Chemistry
  2. Argonne National Lab. (ANL), Argonne, IL (United States). Materials Science Division
  3. Univ. of California, Berkeley, CA (United States). Dept. of Chemistry; Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Materials Science Division
  4. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Materials Science Division
  5. Univ. of Wisconsin, Madison, WI (United States). Dept. of Chemical and Biological Engineering
  6. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Divison of Materials Science and Technology
  7. Tsinghua Univ., Beijing (China). Dept. of Chemistry
  8. Univ. of California, Berkeley, CA (United States). Dept. of Chemistry; Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Materials Science Division; King Abdulaziz Univ., Jeddah (Saudi Arabia). Dept. of Chemistry; Univ. of California, Berkeley and Lawrence Berkeley National Lab. (LBNL), CA (United States). Kavli Energy NanoSciences Inst.
Publication Date:
Grant/Contract Number:
AC02-06CH11357; AC02-05CH11231; FG02-05ER15731
Type:
Accepted Manuscript
Journal Name:
Science
Additional Journal Information:
Journal Volume: 343; Journal Issue: 6177; Journal ID: ISSN 0036-8075
Publisher:
AAAS
Research Org:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); USDOE Office of Energy Efficiency and Renewable Energy (EERE), Fuel Cell Technologies Office (EE-3F)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE
OSTI Identifier:
1357584

Chen, Chen, Kang, Yijin, Huo, Ziyang, Zhu, Zhongwei, Huang, Wenyu, Xin, Huolin L., Snyder, Joshua D., Li, Dongguo, Herron, Jeffrey A., Mavrikakis, Manos, Chi, Miaofang, More, Karren L., Li, Yadong, Markovic, Nenad M., Somorjai, Gabor A., Yang, Peidong, and Stamenkovic, Vojislav R.. Highly Crystalline Multimetallic Nanoframes with Three-Dimensional Electrocatalytic Surfaces. United States: N. p., Web. doi:10.1126/science.1249061.
Chen, Chen, Kang, Yijin, Huo, Ziyang, Zhu, Zhongwei, Huang, Wenyu, Xin, Huolin L., Snyder, Joshua D., Li, Dongguo, Herron, Jeffrey A., Mavrikakis, Manos, Chi, Miaofang, More, Karren L., Li, Yadong, Markovic, Nenad M., Somorjai, Gabor A., Yang, Peidong, & Stamenkovic, Vojislav R.. Highly Crystalline Multimetallic Nanoframes with Three-Dimensional Electrocatalytic Surfaces. United States. doi:10.1126/science.1249061.
Chen, Chen, Kang, Yijin, Huo, Ziyang, Zhu, Zhongwei, Huang, Wenyu, Xin, Huolin L., Snyder, Joshua D., Li, Dongguo, Herron, Jeffrey A., Mavrikakis, Manos, Chi, Miaofang, More, Karren L., Li, Yadong, Markovic, Nenad M., Somorjai, Gabor A., Yang, Peidong, and Stamenkovic, Vojislav R.. 2014. "Highly Crystalline Multimetallic Nanoframes with Three-Dimensional Electrocatalytic Surfaces". United States. doi:10.1126/science.1249061. https://www.osti.gov/servlets/purl/1357584.
@article{osti_1357584,
title = {Highly Crystalline Multimetallic Nanoframes with Three-Dimensional Electrocatalytic Surfaces},
author = {Chen, Chen and Kang, Yijin and Huo, Ziyang and Zhu, Zhongwei and Huang, Wenyu and Xin, Huolin L. and Snyder, Joshua D. and Li, Dongguo and Herron, Jeffrey A. and Mavrikakis, Manos and Chi, Miaofang and More, Karren L. and Li, Yadong and Markovic, Nenad M. and Somorjai, Gabor A. and Yang, Peidong and Stamenkovic, Vojislav R.},
abstractNote = {Control of structure at the atomic level can precisely and effectively tune catalytic properties of materials, enabling enhancement in both activity and durability. We synthesized a highly active and durable class of electrocatalysts by exploiting the structural evolution of platinum-nickel (Pt-Ni) bimetallic nanocrystals. The starting material, crystalline PtNi3 polyhedra, transforms in solution by interior erosion into Pt3Ni nanoframes with surfaces that offer three-dimensional molecular accessibility. The edges of the Pt-rich PtNi3 polyhedra are maintained in the final Pt3Ni nanoframes. Both the interior and exterior catalytic surfaces of this open-framework structure are composed of the nanosegregated Pt-skin structure, which exhibits enhanced oxygen reduction reaction (ORR) activity. The Pt3Ni nanoframe catalysts achieved a factor of 36 enhancement in mass activity and a factor of 22 enhancement in specific activity, respectively, for this reaction (relative to state-of-the-art platinum-carbon catalysts) during prolonged exposure to reaction conditions.},
doi = {10.1126/science.1249061},
journal = {Science},
number = 6177,
volume = 343,
place = {United States},
year = {2014},
month = {2}
}