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Title: Hard-Magnet L1 0-CoPt Nanoparticles Advance Fuel Cell Catalysis

Stabilizing transition metals (M) in MPt alloy under acidic conditions is challenging, yet crucial to boost Pt catalysis toward oxygen reduction reaction (ORR). We synthesized ~9 nm hard-magnet core/shell L1 0-CoPt/Pt nanoparticles with 2–3 atomic layers of strained Pt shell for ORR. At 60°C in acid, the hard-magnet L1 0-CoPt better stabilizes Co (5% loss after 24 hr) than soft-magnet A1-CoPt (34% loss in 7 hr). L1 0-CoPt/Pt achieves mass activities (MA) of 0.56 A/mg Pt initially and 0.45 A/mg Pt after 30,000 voltage cycles in the membrane electrode assembly at 80°C, exceeding the DOE 2020 targets on Pt activity and durability (0.44 A/mg Pt in MA and <40% loss in MA after 30,000 cycles). Lastly, density functional theory calculations suggest that the ligand effect of Co and the biaxial strain (-4.50%/-4.25%) of the Pt shell weaken the binding of oxygenated species, leading to enhanced ORR performance in fuel cells.
Authors:
 [1] ;  [2] ;  [3] ; ORCiD logo [4] ; ORCiD logo [4] ;  [3] ;  [5] ;  [5] ;  [6] ;  [1] ;  [1] ;  [1] ;  [1] ;  [1] ;  [1] ; ORCiD logo [4] ;  [2] ;  [3] ;  [7] ;  [1]
  1. Brown Univ., Providence, RI (United States). Dept. of Chemistry
  2. Brown Univ., Providence, RI (United States). School of Engineering
  3. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Science (CNMS)
  4. Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
  5. Dalhousie Univ., Halifax, NS (Canada). Dept. of Chemistry
  6. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Materials Science & Technology Division
  7. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Chemical Sciences Division
Publication Date:
Report Number(s):
LA-UR-18-28949
Journal ID: ISSN 2542-4351
Grant/Contract Number:
89233218CNA000001
Type:
Accepted Manuscript
Journal Name:
Joule
Additional Journal Information:
Journal Volume: 3; Journal Issue: 1; Journal ID: ISSN 2542-4351
Publisher:
Elsevier - Cell Press
Research Org:
Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
Sponsoring Org:
USDOE Office of Energy Efficiency and Renewable Energy (EERE), Fuel Cell Technologies Office (EE-3F)
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE; Energy Sciences; intermetallic; L10-CoPt; nanoparticles; oxygen reduction reaction catalysis; proton exchange membrane fuel cell; hard magnet; stabilizing non-precious metal in acidic condition; meeting DOE 2020 targets on activity and durability of catalyst; atomically thin Pt shell
OSTI Identifier:
1494465

Li, Junrui, Sharma, Shubham, Liu, Xiaoming, Pan, Yung-Tin, Spendelow, Jacob S., Chi, Miaofang, Jia, Yukai, Zhang, Peng, Cullen, David A., Xi, Zheng, Lin, Honghong, Yin, Zhouyang, Shen, Bo, Muzzio, Michelle, Yu, Chao, Kim, Yu Seung, Peterson, Andrew A., More, Karren L., Zhu, Huiyuan, and Sun, Shouheng. Hard-Magnet L10-CoPt Nanoparticles Advance Fuel Cell Catalysis. United States: N. p., Web. doi:10.1016/j.joule.2018.09.016.
Li, Junrui, Sharma, Shubham, Liu, Xiaoming, Pan, Yung-Tin, Spendelow, Jacob S., Chi, Miaofang, Jia, Yukai, Zhang, Peng, Cullen, David A., Xi, Zheng, Lin, Honghong, Yin, Zhouyang, Shen, Bo, Muzzio, Michelle, Yu, Chao, Kim, Yu Seung, Peterson, Andrew A., More, Karren L., Zhu, Huiyuan, & Sun, Shouheng. Hard-Magnet L10-CoPt Nanoparticles Advance Fuel Cell Catalysis. United States. doi:10.1016/j.joule.2018.09.016.
Li, Junrui, Sharma, Shubham, Liu, Xiaoming, Pan, Yung-Tin, Spendelow, Jacob S., Chi, Miaofang, Jia, Yukai, Zhang, Peng, Cullen, David A., Xi, Zheng, Lin, Honghong, Yin, Zhouyang, Shen, Bo, Muzzio, Michelle, Yu, Chao, Kim, Yu Seung, Peterson, Andrew A., More, Karren L., Zhu, Huiyuan, and Sun, Shouheng. 2018. "Hard-Magnet L10-CoPt Nanoparticles Advance Fuel Cell Catalysis". United States. doi:10.1016/j.joule.2018.09.016.
@article{osti_1494465,
title = {Hard-Magnet L10-CoPt Nanoparticles Advance Fuel Cell Catalysis},
author = {Li, Junrui and Sharma, Shubham and Liu, Xiaoming and Pan, Yung-Tin and Spendelow, Jacob S. and Chi, Miaofang and Jia, Yukai and Zhang, Peng and Cullen, David A. and Xi, Zheng and Lin, Honghong and Yin, Zhouyang and Shen, Bo and Muzzio, Michelle and Yu, Chao and Kim, Yu Seung and Peterson, Andrew A. and More, Karren L. and Zhu, Huiyuan and Sun, Shouheng},
abstractNote = {Stabilizing transition metals (M) in MPt alloy under acidic conditions is challenging, yet crucial to boost Pt catalysis toward oxygen reduction reaction (ORR). We synthesized ~9 nm hard-magnet core/shell L10-CoPt/Pt nanoparticles with 2–3 atomic layers of strained Pt shell for ORR. At 60°C in acid, the hard-magnet L10-CoPt better stabilizes Co (5% loss after 24 hr) than soft-magnet A1-CoPt (34% loss in 7 hr). L10-CoPt/Pt achieves mass activities (MA) of 0.56 A/mgPt initially and 0.45 A/mgPt after 30,000 voltage cycles in the membrane electrode assembly at 80°C, exceeding the DOE 2020 targets on Pt activity and durability (0.44 A/mgPt in MA and <40% loss in MA after 30,000 cycles). Lastly, density functional theory calculations suggest that the ligand effect of Co and the biaxial strain (-4.50%/-4.25%) of the Pt shell weaken the binding of oxygenated species, leading to enhanced ORR performance in fuel cells.},
doi = {10.1016/j.joule.2018.09.016},
journal = {Joule},
number = 1,
volume = 3,
place = {United States},
year = {2018},
month = {10}
}