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Title: Ordered Pt 3Co Intermetallic Nanoparticles Derived from Metal–Organic Frameworks for Oxygen Reduction

Abstract

Highly ordered Pt alloy structures are proved effective to improve their catalytic activity and stability for the oxygen reduction reaction (ORR) for proton exchange membrane fuel cells. Here, we report a new approach to preparing ordered Pt 3Co intermetallic nanoparticles through a facile thermal treatment of Pt nanoparticles supported on Co-doped metal-organic framework (MOF)-derived carbon. In particular, the atomically dispersed Co sites, which are originally embedded into MOF-derived carbon, diffuse into Pt nanocrystals and form ordered Pt 3Co structures. It is very crucial for the formation of the ordered Pt 3Co to carefully control the doping content of Co into the MOFs and the heating temperatures for Co diffusion. The optimal Pt 3Co nanoparticle catalyst has achieved significantly enhanced activity and stability, exhibiting a half-wave potential up to 0.92 V vs. RHE and only losing 12 mV after 30,000 potential cycling between 0.6 and 1.0 V. The highly ordered intermetallic structure was retained after the accelerated stress tests evidenced by atomic-scale elemental mapping. Fuel cell tests further verified the high intrinsic activity of the ordered Pt 3Co catalysts. Unlike the direct use of MOF-derived carbon supports for depositing Pt, we utilized MOF-derived carbon containing atomically dispersed Co sites as Comore » sources to prepare ordered Pt 3Co intermetallic catalysts. Finally, the new synthesis approach provides an effective strategy to develop active and stable Pt alloy catalysts by leveraging the unique properties of MOFs such as 3D structures, high surface areas, and controlled nitrogen doping.« less

Authors:
 [1];  [2];  [3];  [4];  [4]; ORCiD logo [5];  [4];  [3]; ORCiD logo [2]; ORCiD logo [4]
  1. East China Univ. of Science and Technology, Shanghai (China). School of Mechanical and Power Engineering; Univ. at Buffalo, NY (United States). Dept. of Chemical and Biological Engineering
  2. Brookhaven National Lab. (BNL), Upton, NY (United States). Center for Functional Nanomaterials (CFN)
  3. Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
  4. Univ. at Buffalo, NY (United States). Dept. of Chemical and Biological Engineering
  5. Univ. of South Carolina, Columbia, SC (United States). Dept. of Chemical Engineering
Publication Date:
Research Org.:
Brookhaven National Laboratory (BNL), Upton, NY (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1454805
Report Number(s):
BNL-205760-2018-JAAM
Journal ID: ISSN 1530-6984
Grant/Contract Number:  
SC0012704
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Nano Letters
Additional Journal Information:
Journal Name: Nano Letters; Journal ID: ISSN 1530-6984
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE; Pt3Co intermetallic; oxygen reduction reaction; electrocatalysis; metal-organic frameworks; atomically dispersed Co

Citation Formats

Wang, Xiao Xia, Hwang, Sooyeon, Pan, Yung-Tin, Chen, Kate, He, Yanghua, Karakalos, Stavros, Zhang, Hanguang, Spendelow, Jacob S., Su, Dong, and Wu, Gang. Ordered Pt3Co Intermetallic Nanoparticles Derived from Metal–Organic Frameworks for Oxygen Reduction. United States: N. p., 2018. Web. doi:10.1021/acs.nanolett.8b00978.
Wang, Xiao Xia, Hwang, Sooyeon, Pan, Yung-Tin, Chen, Kate, He, Yanghua, Karakalos, Stavros, Zhang, Hanguang, Spendelow, Jacob S., Su, Dong, & Wu, Gang. Ordered Pt3Co Intermetallic Nanoparticles Derived from Metal–Organic Frameworks for Oxygen Reduction. United States. doi:10.1021/acs.nanolett.8b00978.
Wang, Xiao Xia, Hwang, Sooyeon, Pan, Yung-Tin, Chen, Kate, He, Yanghua, Karakalos, Stavros, Zhang, Hanguang, Spendelow, Jacob S., Su, Dong, and Wu, Gang. Wed . "Ordered Pt3Co Intermetallic Nanoparticles Derived from Metal–Organic Frameworks for Oxygen Reduction". United States. doi:10.1021/acs.nanolett.8b00978.
@article{osti_1454805,
title = {Ordered Pt3Co Intermetallic Nanoparticles Derived from Metal–Organic Frameworks for Oxygen Reduction},
author = {Wang, Xiao Xia and Hwang, Sooyeon and Pan, Yung-Tin and Chen, Kate and He, Yanghua and Karakalos, Stavros and Zhang, Hanguang and Spendelow, Jacob S. and Su, Dong and Wu, Gang},
abstractNote = {Highly ordered Pt alloy structures are proved effective to improve their catalytic activity and stability for the oxygen reduction reaction (ORR) for proton exchange membrane fuel cells. Here, we report a new approach to preparing ordered Pt3Co intermetallic nanoparticles through a facile thermal treatment of Pt nanoparticles supported on Co-doped metal-organic framework (MOF)-derived carbon. In particular, the atomically dispersed Co sites, which are originally embedded into MOF-derived carbon, diffuse into Pt nanocrystals and form ordered Pt3Co structures. It is very crucial for the formation of the ordered Pt3Co to carefully control the doping content of Co into the MOFs and the heating temperatures for Co diffusion. The optimal Pt3Co nanoparticle catalyst has achieved significantly enhanced activity and stability, exhibiting a half-wave potential up to 0.92 V vs. RHE and only losing 12 mV after 30,000 potential cycling between 0.6 and 1.0 V. The highly ordered intermetallic structure was retained after the accelerated stress tests evidenced by atomic-scale elemental mapping. Fuel cell tests further verified the high intrinsic activity of the ordered Pt3Co catalysts. Unlike the direct use of MOF-derived carbon supports for depositing Pt, we utilized MOF-derived carbon containing atomically dispersed Co sites as Co sources to prepare ordered Pt3Co intermetallic catalysts. Finally, the new synthesis approach provides an effective strategy to develop active and stable Pt alloy catalysts by leveraging the unique properties of MOFs such as 3D structures, high surface areas, and controlled nitrogen doping.},
doi = {10.1021/acs.nanolett.8b00978},
journal = {Nano Letters},
number = ,
volume = ,
place = {United States},
year = {Wed Jun 06 00:00:00 EDT 2018},
month = {Wed Jun 06 00:00:00 EDT 2018}
}

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