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Title: High-Performance Core–Shell Catalyst with Nitride Nanoparticles as a Core: Well-Defined Titanium Copper Nitride Coated with an Atomic Pt Layer for the Oxygen Reduction Reaction

Abstract

A class of core–shell structured low-platinum catalysts with well-dispersed inexpensive titanium copper nitride nanoparticles as cores and atomic platinum layers as shells exhibiting high activity and stability for the oxygen reduction reaction is successfully developed. In using nitrided carbon nanotubes (NCNTs) as the support greatly improved the morphology and dispersion of the nitride nanoparticles, resulting in significant enhancement of the performance of the catalyst. The optimized catalyst, Ti 0.9Cu 0.1N@Pt/NCNTs, has a Pt mass activity 5 times higher than that of commercial Pt/C, comparable to that of core–shell catalysts with precious metal nanoparticles as the core, and much higher than that the latter if we take into account the mass activity of all platinum group metals. Furthermore, only a minimal loss of activity can be observed after 10000 potential cycles, demonstrating the catalyst’s high stability. After durability testing, atomic-scale elemental mapping confirmed that the core–shell structure of the catalyst remained intact. This approach may open a pathway for the design and preparation of high-performance inexpensive core–shell catalysts for a wide range of applications in energy conversion processes.

Authors:
 [1];  [1];  [1];  [1];  [1];  [1];  [1]; ORCiD logo [1];  [2]
  1. South China Univ. of Technology (SCUT), Guangzhou (China). School of Chemistry and Chemical Engineering; Guangdong Univ., Guangzhou (China). Key Lab. of Fuel Cell Technology of Guangdong Province and Key Lab. of New Energy Technology
  2. Brookhaven National Lab. (BNL), Upton, NY (United States). Chemistry Dept.
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:
1377049
Report Number(s):
BNL-114180-2017-JA
Journal ID: ISSN 2155-5435; R&D Project: MA510MAEA; KC0302010
Grant/Contract Number:
SC00112704
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
ACS Catalysis
Additional Journal Information:
Journal Volume: 7; Journal Issue: 6; Journal ID: ISSN 2155-5435
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; core−shell structure; fuel cells; oxygen reduction reaction; stability; transition metal nitride

Citation Formats

Tian, Xinlong, Tang, Haibo, Luo, Junming, Nan, Haoxiong, Shu, Ting, Du, Li, Zeng, Jianhuang, Liao, Shijun, and Adzic, Radoslav R. High-Performance Core–Shell Catalyst with Nitride Nanoparticles as a Core: Well-Defined Titanium Copper Nitride Coated with an Atomic Pt Layer for the Oxygen Reduction Reaction. United States: N. p., 2017. Web. doi:10.1021/acscatal.7b00366.
Tian, Xinlong, Tang, Haibo, Luo, Junming, Nan, Haoxiong, Shu, Ting, Du, Li, Zeng, Jianhuang, Liao, Shijun, & Adzic, Radoslav R. High-Performance Core–Shell Catalyst with Nitride Nanoparticles as a Core: Well-Defined Titanium Copper Nitride Coated with an Atomic Pt Layer for the Oxygen Reduction Reaction. United States. doi:10.1021/acscatal.7b00366.
Tian, Xinlong, Tang, Haibo, Luo, Junming, Nan, Haoxiong, Shu, Ting, Du, Li, Zeng, Jianhuang, Liao, Shijun, and Adzic, Radoslav R. Tue . "High-Performance Core–Shell Catalyst with Nitride Nanoparticles as a Core: Well-Defined Titanium Copper Nitride Coated with an Atomic Pt Layer for the Oxygen Reduction Reaction". United States. doi:10.1021/acscatal.7b00366. https://www.osti.gov/servlets/purl/1377049.
@article{osti_1377049,
title = {High-Performance Core–Shell Catalyst with Nitride Nanoparticles as a Core: Well-Defined Titanium Copper Nitride Coated with an Atomic Pt Layer for the Oxygen Reduction Reaction},
author = {Tian, Xinlong and Tang, Haibo and Luo, Junming and Nan, Haoxiong and Shu, Ting and Du, Li and Zeng, Jianhuang and Liao, Shijun and Adzic, Radoslav R.},
abstractNote = {A class of core–shell structured low-platinum catalysts with well-dispersed inexpensive titanium copper nitride nanoparticles as cores and atomic platinum layers as shells exhibiting high activity and stability for the oxygen reduction reaction is successfully developed. In using nitrided carbon nanotubes (NCNTs) as the support greatly improved the morphology and dispersion of the nitride nanoparticles, resulting in significant enhancement of the performance of the catalyst. The optimized catalyst, Ti0.9Cu0.1N@Pt/NCNTs, has a Pt mass activity 5 times higher than that of commercial Pt/C, comparable to that of core–shell catalysts with precious metal nanoparticles as the core, and much higher than that the latter if we take into account the mass activity of all platinum group metals. Furthermore, only a minimal loss of activity can be observed after 10000 potential cycles, demonstrating the catalyst’s high stability. After durability testing, atomic-scale elemental mapping confirmed that the core–shell structure of the catalyst remained intact. This approach may open a pathway for the design and preparation of high-performance inexpensive core–shell catalysts for a wide range of applications in energy conversion processes.},
doi = {10.1021/acscatal.7b00366},
journal = {ACS Catalysis},
number = 6,
volume = 7,
place = {United States},
year = {Tue Apr 25 00:00:00 EDT 2017},
month = {Tue Apr 25 00:00:00 EDT 2017}
}

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  • We report the synthesis of core/shell face-centered tetragonal (fct)-FePd/Pd nanoparticles (NPs) via reductive annealing of core/shell Pd/Fe 3O 4 NPs followed by temperature-controlled Fe etching in acetic acid. Among three different kinds of core/shell FePd/Pd NPs studied (FePd core at similar to 8 nm and Pd shell at 0.27, 0.65, or 0.81 nm), the fct-FePd/Pd-0.65 NPs are the most efficient catalyst for the oxygen reduction reaction (ORR) in 0.1 M HClO 4 with Pt-like activity and durability. This enhanced ORR catalysis arises from the desired Pd lattice compression in the 0.65 nm Pd shell induced by the fct-FePd core. Lastly,more » our study offers a general approach to enhance Pd catalysis in acid for ORB.« less
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