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Title: Highly uniform distribution of Pt nanoparticles on N-doped hollow carbon spheres with enhanced durability for oxygen reduction reaction

Abstract

Here, carbon-supported Pt nanostructures currently exhibited great potential in polymer electrolyte membrane fuel cells. Nitrogen-doped hollow carbon spheres (NHCSs) with extra low density and high specific surface area are promising carbon support for loading Pt NPs. The doped heteroatom of nitrogen could not only contribute to the active activity for the oxygen reduction reaction (ORR), but also shows a strong interaction with Pt NPs for entrapping them from dissolution/migration. This synergetic effect/interaction resulted in the uniform dispersion and strong combination of the Pt NPs on the carbon support and thus play a significant role in hindering the degradation of the catalytic activities of Pt NPs. As expected, the as-obtained Pt/NHCSs displayed improved catalytic activity and superior durability toward ORR.

Authors:
 [1];  [1];  [2];  [1];  [1]
  1. Washington State Univ., Pullman, WA (United States)
  2. Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Publication Date:
Research Org.:
Pacific Northwest National Lab. (PNNL), Richland, WA (United States). Environmental Molecular Sciences Lab. (EMSL)
Sponsoring Org.:
USDOE
OSTI Identifier:
1347853
Report Number(s):
PNNL-SA-123162
Journal ID: ISSN 2046-2069; RSCACL; 48920; KP1704020
Grant/Contract Number:
AC05-76RL01830
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
RSC Advances
Additional Journal Information:
Journal Volume: 7; Journal Issue: 11; Journal ID: ISSN 2046-2069
Publisher:
Royal Society of Chemistry
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Environmental Molecular Sciences Laboratory

Citation Formats

Shi, Qiurong, Zhu, Chengzhou, Engelhard, Mark H., Du, Dan, and Lin, Yuehe. Highly uniform distribution of Pt nanoparticles on N-doped hollow carbon spheres with enhanced durability for oxygen reduction reaction. United States: N. p., 2017. Web. doi:10.1039/c6ra25391a.
Shi, Qiurong, Zhu, Chengzhou, Engelhard, Mark H., Du, Dan, & Lin, Yuehe. Highly uniform distribution of Pt nanoparticles on N-doped hollow carbon spheres with enhanced durability for oxygen reduction reaction. United States. doi:10.1039/c6ra25391a.
Shi, Qiurong, Zhu, Chengzhou, Engelhard, Mark H., Du, Dan, and Lin, Yuehe. Thu . "Highly uniform distribution of Pt nanoparticles on N-doped hollow carbon spheres with enhanced durability for oxygen reduction reaction". United States. doi:10.1039/c6ra25391a. https://www.osti.gov/servlets/purl/1347853.
@article{osti_1347853,
title = {Highly uniform distribution of Pt nanoparticles on N-doped hollow carbon spheres with enhanced durability for oxygen reduction reaction},
author = {Shi, Qiurong and Zhu, Chengzhou and Engelhard, Mark H. and Du, Dan and Lin, Yuehe},
abstractNote = {Here, carbon-supported Pt nanostructures currently exhibited great potential in polymer electrolyte membrane fuel cells. Nitrogen-doped hollow carbon spheres (NHCSs) with extra low density and high specific surface area are promising carbon support for loading Pt NPs. The doped heteroatom of nitrogen could not only contribute to the active activity for the oxygen reduction reaction (ORR), but also shows a strong interaction with Pt NPs for entrapping them from dissolution/migration. This synergetic effect/interaction resulted in the uniform dispersion and strong combination of the Pt NPs on the carbon support and thus play a significant role in hindering the degradation of the catalytic activities of Pt NPs. As expected, the as-obtained Pt/NHCSs displayed improved catalytic activity and superior durability toward ORR.},
doi = {10.1039/c6ra25391a},
journal = {RSC Advances},
number = 11,
volume = 7,
place = {United States},
year = {Thu Jan 19 00:00:00 EST 2017},
month = {Thu Jan 19 00:00:00 EST 2017}
}

Journal Article:
Free Publicly Available Full Text
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  • Pt-based nanomaterials are regarded as the most efficient electrocatalysts for the oxygen reduction reaction (ORR) in proton exchange membrane fuel cells (PEMFCs). However, widespread adoption of PEMFCs requires solutions to major challenges encountered with ORR catalysts, namely high cost, sluggish kinetics, and low durability. In this paper, a new efficient method utilizing Co-based metal-organic frameworks is developed to produce PtCo bimetallic nanoparticles embedded in unique nitrogen-doped hollow porous carbon capsules. The obtained catalyst demonstrates an outstanding ORR performance, with a mass activity that is 5.5 and 13.5 times greater than that of commercial Pt/C and Pt black, respectively. Most importantly,more » the product exhibits dramatically improved durability in terms of both electrochemically active surface area (ECAS) and mass activity compared to commercial Pt/C and Pt black catalysts. Finally, the remarkable ORR performance demonstrated here can be attributed to the structural features of the catalyst (its alloy structure, high dispersion and fine particle size) and the carbon support (its nitrogen dopant, large surface area and hollow porous structure).« less
  • The need for inexpensive and high-activity oxygen reduction reaction (ORR) electrocatalysts has attracted considerable research interest over the past years. Here we report a novel hybrid that contains cobalt nitride/nitrogen-rich hollow carbon spheres (CoxN/NHCS) as a high-performance catalyst for ORR. The CoxN nanoparticles were uniformly dispersed and confined in the hollow NHCS shell. The performance of the resulting CoxN/NHCS hybrid was comparable with that of a commercial Pt/C at the same catalyst loading toward ORR, but the mass activity of the former was 5.7 times better than that of the latter. The nitrogen in both CoxN and NHCS, especially CoxN,more » could weaken the adsorption of reaction intermediates (O and OOH), which follows the favourable reaction pathway on CoxN/NHCS according to the DFT-calculated Gibbs free energy diagrams. Our results demonstrated a new strategy for designing and developing inexpensive, non-precious metal electrocatalysts for next-generation fuels. The authors acknowledge the financial support from the National Basic Research Program (973 program, No. 2013CB733501) and the National Natural Science Foundation of China (No. 21306169, 21101137, 21136001, 21176221 and 91334013). Dr. D. Mei is supported by the US Department of Energy (DOE), Office of Science, Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences & Biosciences. Pacific Northwest National Laboratory (PNNL) is a multiprogram national laboratory operated for DOE by Battelle. Computing time was granted by the grand challenge of computational catalysis of the William R. Wiley Environmental Molecular Sciences Laboratory (EMSL). EMSL is a national scientific user facility located at Pacific Northwest National Laboratory (PNNL) and sponsored by DOE’s Office of Biological and Environmental Research.« less