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Title: One-Step Facile Synthesis of High-Activity Nitrogen-Doped PtNiN Oxygen Reduction Catalyst

Abstract

PtM alloy electrocatalysts (M = Fe, Co, Ni) have been the subject of many investigations aimed at increasing their attractive properties, in particular oxygen reduction reaction (ORR) activity, while reducing total platinum-group-metal content and improving durability. Despite some success, these catalysts still have relatively high Pt content and lack the necessary durability as M metals leach out from the alloys during potential cycling. Previously, we synthesized nitrogen (N)-doped PtMN/C catalysts consisting of thin Pt shells on M nitride cores by a two-step method, which showed higher ORR activity and stability than their PtM counterparts. In the present work, we developed a facile one-step synthesis method, which comprises a single thermal annealing process of the N-doped PtNiN/C alloy. The ORR performance of the one-step synthesized PtNiN/C catalyst is much higher than that of the two-step synthesized PtNiN/C, as revealed by rotating disk electrode measurements. Membrane electrode assembly fuel cell testing demonstrated superb durability and high activity. Formation of Pt monolayer shells on the nitrided (PtxNi1-x)4N cores was confirmed by in situ X-ray absorption spectroscopy. The origins of the enhanced activity and stability of the one-step synthesized PtNiN/C catalyst are elucidated based on density functional theory calculations together with the experimental results.

Authors:
 [1];  [2]; ORCiD logo [3];  [4];  [4];  [5]; ORCiD logo [1];  [2];  [6];  [4]; ORCiD logo [4]
+ Show Author Affiliations
  1. Brookhaven National Lab. (BNL), Upton, NY (United States); Stony Brook Univ., NY (United States)
  2. General Motors LLC, Pontiac, MI (United States)
  3. Stony Brook Univ., NY (United States)
  4. Brookhaven National Lab. (BNL), Upton, NY (United States)
  5. Columbia Univ., New York, NY (United States)
  6. National Yang Ming Chiao Tung University, Tainan (Taiwan)
Publication Date:
Research Org.:
Brookhaven National Lab. (BNL), Upton, NY (United States)
Sponsoring Org.:
USDOE Office of Energy Efficiency and Renewable Energy (EERE), Transportation Office. Vehicle Technologies Office; USDOE Office of Science (SC), Basic Energy Sciences (BES); General Motors; Ministry of Science and Technology; National Center for High-performance Computing (NCHC); National Yang Ming Chiao Tung University and Ministry of Education (MOE), Taiwan
OSTI Identifier:
1889130
Report Number(s):
BNL-223455-2022-JAAM
Journal ID: ISSN 2574-0962
Grant/Contract Number:  
SC0012704; SC0012573; NF-17-33; SC0012335; 110-2221-E-A49-017-MY3
Resource Type:
Accepted Manuscript
Journal Name:
ACS Applied Energy Materials
Additional Journal Information:
Journal Volume: 5; Journal Issue: 4; Journal ID: ISSN 2574-0962
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
30 DIRECT ENERGY CONVERSION; one-step synthesis; fuel cells; oxygen reduction; platinum-nickel nanoparticles; nitrogen doping; rotating disk electrode; membrane electrode assembly

Citation Formats

Song, Liang, Cai, Yun, Liu, Yang, Zhao, Xueru, Kuttiyiel, Kurian A., Marinkovic, Nebojsa, Frenkel, Anatoly I., Kongkanand, Anusorn, Choi, YongMan, Adzic, Radoslav R., and Sasaki, Kotaro. One-Step Facile Synthesis of High-Activity Nitrogen-Doped PtNiN Oxygen Reduction Catalyst. United States: N. p., 2022. Web. doi:10.1021/acsaem.2c00631.
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Song, Liang, Cai, Yun, Liu, Yang, Zhao, Xueru, Kuttiyiel, Kurian A., Marinkovic, Nebojsa, Frenkel, Anatoly I., Kongkanand, Anusorn, Choi, YongMan, Adzic, Radoslav R., & Sasaki, Kotaro. One-Step Facile Synthesis of High-Activity Nitrogen-Doped PtNiN Oxygen Reduction Catalyst. United States. https://doi.org/10.1021/acsaem.2c00631
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Song, Liang, Cai, Yun, Liu, Yang, Zhao, Xueru, Kuttiyiel, Kurian A., Marinkovic, Nebojsa, Frenkel, Anatoly I., Kongkanand, Anusorn, Choi, YongMan, Adzic, Radoslav R., and Sasaki, Kotaro. Thu . "One-Step Facile Synthesis of High-Activity Nitrogen-Doped PtNiN Oxygen Reduction Catalyst". United States. https://doi.org/10.1021/acsaem.2c00631. https://www.osti.gov/servlets/purl/1889130.
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@article{osti_1889130,
title = {One-Step Facile Synthesis of High-Activity Nitrogen-Doped PtNiN Oxygen Reduction Catalyst},
author = {Song, Liang and Cai, Yun and Liu, Yang and Zhao, Xueru and Kuttiyiel, Kurian A. and Marinkovic, Nebojsa and Frenkel, Anatoly I. and Kongkanand, Anusorn and Choi, YongMan and Adzic, Radoslav R. and Sasaki, Kotaro},
abstractNote = {PtM alloy electrocatalysts (M = Fe, Co, Ni) have been the subject of many investigations aimed at increasing their attractive properties, in particular oxygen reduction reaction (ORR) activity, while reducing total platinum-group-metal content and improving durability. Despite some success, these catalysts still have relatively high Pt content and lack the necessary durability as M metals leach out from the alloys during potential cycling. Previously, we synthesized nitrogen (N)-doped PtMN/C catalysts consisting of thin Pt shells on M nitride cores by a two-step method, which showed higher ORR activity and stability than their PtM counterparts. In the present work, we developed a facile one-step synthesis method, which comprises a single thermal annealing process of the N-doped PtNiN/C alloy. The ORR performance of the one-step synthesized PtNiN/C catalyst is much higher than that of the two-step synthesized PtNiN/C, as revealed by rotating disk electrode measurements. Membrane electrode assembly fuel cell testing demonstrated superb durability and high activity. Formation of Pt monolayer shells on the nitrided (PtxNi1-x)4N cores was confirmed by in situ X-ray absorption spectroscopy. The origins of the enhanced activity and stability of the one-step synthesized PtNiN/C catalyst are elucidated based on density functional theory calculations together with the experimental results.},
doi = {10.1021/acsaem.2c00631},
journal = {ACS Applied Energy Materials},
number = 4,
volume = 5,
place = {United States},
year = {Thu Apr 14 00:00:00 EDT 2022},
month = {Thu Apr 14 00:00:00 EDT 2022}
}
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https://doi.org/10.1021/acsaem.2c00631
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