Journal
ACS APPLIED ENERGY MATERIALS
Volume 5, Issue 4, Pages 5245-5255Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acsaem.2c00631
Keywords
one-step synthesis; fuel cells; oxygen reduction; platinum-nickel nanoparticles; nitrogen doping; rotating disk electrode; membrane electrode assembly
Funding
- U.S. Department of Energy (DOE) [DE-SC0012704]
- U.S. DOE, Office of Energy Efficiency and Renewable Energy, Hydrogen and Fuel Cell Technologies Office [DE-SC0012704]
- Integrated Mesoscale Architectures for Sustainable Catalysis (IMASC), an Energy Frontier Research Center - U.S. Department of Energy, Office of Science, Basic Energy Sciences [DE-SC0012573]
- General Motors [NF-17-33]
- U.S. DOE Office of Science Facilities, at Brookhaven National Laboratory [DE-SC0012704]
- U.S. DOE, Office of Basic Energy Sciences [DE-SC0012335]
- Ministry of Science and Technology (MOST) [110-2221-E-A49-017-MY3]
- National Center for High-performance Computing (NCHC)
- Higher Education Sprout Project of the National Yang Ming Chiao Tung University
- Ministry of Education (MOE), Taiwan
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A facile one-step synthesis method was developed to prepare PtNiN/C catalyst with high ORR performance and stability. Superior performance was demonstrated in electrochemical testing and fuel cell experiments, supported by in situ X-ray absorption spectroscopy confirming the formation of Pt monolayer shells on nitrided cores.
PtM alloy electrocatalysts (M = Fe, Co, Ni) have been the subject of many investigations aimed at increasing their attractive properties, in particular their 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 study, we developed a facile onestep 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)(4)N 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.
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