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Title: Pt alloy nanoparticles decorated on large-size nitrogen-doped graphene tubes for highly stable oxygen-reduction catalysts

Abstract

Pt alloy nanoparticles supported on Vulcan XC-72 (Pt/C) are the most effective catalysts for kinetically sluggish oxygen reduction reaction (ORR) in proton exchange membrane fuel cells. However, significant performance degradation has been observed with the Pt/C catalysts due to agglomeration and Ostwald ripening of Pt nanoparticles largely resulting from the corrosion of carbon supports. In this paper, we developed a Pt alloy catalyst through annealing Pt nanoparticles deposited on nitrogen/metal co-doped large-size graphene tubes (NGTs). The in-situ formation of PtM (M: Co and Ni) alloy during the annealing process contributes to the improvement of the catalytic activity and stability. During the accelerated stress tests (AST), after 20 000 potential cycles (0.6–1.0 V vs. RHE), the retained electrochemical surface area (ECSA) of the PtM/NGT catalyst is more than 2 times larger than that of the Pt/C catalyst. As for the AST tests of carbon corrosion, after 30 000 potential cycles (1.0–1.5 V vs. RHE) at room temperature, the NGT morphologies are well maintained and no ECSA loss of this PtM catalyst is observed, indicating excellent corrosion-resistance. Even at harsher 60 °C, the PtM/NGT catalyst exhibits only insignificant loss (6 mV) of E 1/2 while the Pt/C catalyst shows significant degradation (47more » mV loss in E 1/2). Finally, the improved stability of PtM/NGT catalyst is attributed to the highly graphitized NGTs and possible synergistic effects between the NGT carbon support and the PtM alloy nanoparticles.« less

Authors:
 [1];  [2];  [1]; ORCiD logo [3];  [1]; ORCiD logo [1];  [1]; ORCiD logo [2]; ORCiD logo [1]
  1. 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
  3. Univ. of South Carolina, Columbia, SC (United States). Dept. of Chemical Engineering
Publication Date:
Research Org.:
Brookhaven National Lab. (BNL), Upton, NY (United States); Univ. at Buffalo, NY (United States)
Sponsoring Org.:
USDOE Office of Energy Efficiency and Renewable Energy (EERE), Fuel Cell Technologies Office (EE-3F); USDOE Office of Science (SC)
OSTI Identifier:
1476277
Alternate Identifier(s):
OSTI ID: 1469234
Report Number(s):
BNL-209135-2018-JAAM
Journal ID: ISSN 2040-3364
Grant/Contract Number:  
SC0012704
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Nanoscale
Additional Journal Information:
Journal Volume: 10; Journal Issue: 36; Journal ID: ISSN 2040-3364
Publisher:
Royal Society of Chemistry
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Chen, Mengjie, Hwang, Sooyeon, Li, Jiazhan, Karakalos, Stavros, Chen, Kate, He, Yanghua, Mukherjee, Shreya, Su, Dong, and Wu, Gang. Pt alloy nanoparticles decorated on large-size nitrogen-doped graphene tubes for highly stable oxygen-reduction catalysts. United States: N. p., 2018. Web. doi:10.1039/C8NR05888A.
Chen, Mengjie, Hwang, Sooyeon, Li, Jiazhan, Karakalos, Stavros, Chen, Kate, He, Yanghua, Mukherjee, Shreya, Su, Dong, & Wu, Gang. Pt alloy nanoparticles decorated on large-size nitrogen-doped graphene tubes for highly stable oxygen-reduction catalysts. United States. doi:10.1039/C8NR05888A.
Chen, Mengjie, Hwang, Sooyeon, Li, Jiazhan, Karakalos, Stavros, Chen, Kate, He, Yanghua, Mukherjee, Shreya, Su, Dong, and Wu, Gang. Mon . "Pt alloy nanoparticles decorated on large-size nitrogen-doped graphene tubes for highly stable oxygen-reduction catalysts". United States. doi:10.1039/C8NR05888A.
@article{osti_1476277,
title = {Pt alloy nanoparticles decorated on large-size nitrogen-doped graphene tubes for highly stable oxygen-reduction catalysts},
author = {Chen, Mengjie and Hwang, Sooyeon and Li, Jiazhan and Karakalos, Stavros and Chen, Kate and He, Yanghua and Mukherjee, Shreya and Su, Dong and Wu, Gang},
abstractNote = {Pt alloy nanoparticles supported on Vulcan XC-72 (Pt/C) are the most effective catalysts for kinetically sluggish oxygen reduction reaction (ORR) in proton exchange membrane fuel cells. However, significant performance degradation has been observed with the Pt/C catalysts due to agglomeration and Ostwald ripening of Pt nanoparticles largely resulting from the corrosion of carbon supports. In this paper, we developed a Pt alloy catalyst through annealing Pt nanoparticles deposited on nitrogen/metal co-doped large-size graphene tubes (NGTs). The in-situ formation of PtM (M: Co and Ni) alloy during the annealing process contributes to the improvement of the catalytic activity and stability. During the accelerated stress tests (AST), after 20 000 potential cycles (0.6–1.0 V vs. RHE), the retained electrochemical surface area (ECSA) of the PtM/NGT catalyst is more than 2 times larger than that of the Pt/C catalyst. As for the AST tests of carbon corrosion, after 30 000 potential cycles (1.0–1.5 V vs. RHE) at room temperature, the NGT morphologies are well maintained and no ECSA loss of this PtM catalyst is observed, indicating excellent corrosion-resistance. Even at harsher 60 °C, the PtM/NGT catalyst exhibits only insignificant loss (6 mV) of E1/2 while the Pt/C catalyst shows significant degradation (47 mV loss in E1/2). Finally, the improved stability of PtM/NGT catalyst is attributed to the highly graphitized NGTs and possible synergistic effects between the NGT carbon support and the PtM alloy nanoparticles.},
doi = {10.1039/C8NR05888A},
journal = {Nanoscale},
number = 36,
volume = 10,
place = {United States},
year = {Mon Sep 03 00:00:00 EDT 2018},
month = {Mon Sep 03 00:00:00 EDT 2018}
}

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Works referenced in this record:

Raman spectroscopy of graphene and graphite: Disorder, electron–phonon coupling, doping and nonadiabatic effects
journal, July 2007


Activity benchmarks and requirements for Pt, Pt-alloy, and non-Pt oxygen reduction catalysts for PEMFCs
journal, March 2005

  • Gasteiger, Hubert A.; Kocha, Shyam S.; Sompalli, Bhaskar
  • Applied Catalysis B: Environmental, Vol. 56, Issue 1-2, p. 9-35
  • DOI: 10.1016/j.apcatb.2004.06.021

Understanding and approaches for the durability issues of Pt-based catalysts for PEM fuel cell
journal, September 2007


High-Performance Electrocatalysts for Oxygen Reduction Derived from Polyaniline, Iron, and Cobalt
journal, April 2011


Raman spectroscopy in graphene
journal, April 2009


Improved Oxygen Reduction Activity on Pt3Ni(111) via Increased Surface Site Availability
journal, January 2007

  • Stamenkovic, V. R.; Fowler, B.; Mun, B. S.
  • Science, Vol. 315, Issue 5811, p. 493-497
  • DOI: 10.1126/science.1135941

Influence of Nitrogen Doping on Oxygen Reduction Electrocatalysis at Carbon Nanofiber Electrodes
journal, March 2005

  • Maldonado, Stephen; Stevenson, Keith J.
  • The Journal of Physical Chemistry B, Vol. 109, Issue 10, p. 4707-4716
  • DOI: 10.1021/jp044442z

Octahedral PtNi Nanoparticle Catalysts Exceptional Oxygen Reduction Activity by Tuning the Alloy Particle Surface Composition
journal, October 2012

  • Cui, Chunhua; Gan, Lin; Li, Hui-Hui
  • Nano Letters, Vol. 12, Issue 11, p. 5885-5889
  • DOI: 10.1021/nl3032795