催化作用
氮气
合金
铂金
氮化物
渗氮
兴奋剂
退火(玻璃)
氧还原反应
氧还原
金属
化学
耐久性
电极
材料科学
无机化学
化学工程
纳米技术
冶金
电化学
物理化学
复合材料
图层(电子)
有机化学
光电子学
工程类
作者
Liang Song,Yun Cai,Yang Liu,Xueru Zhao,Kurian A. Kuttiyiel,Nebojsa Marinkovic,Anatoly I. Frenkel,Anusorn Kongkanand,YongMan Choi,Radoslav R. Adzic,Kotaro Sasaki
出处
期刊:ACS Applied Energy Materials
日期:2022-04-14
卷期号:5 (4): 5245-5255
被引量:6
标识
DOI:10.1021/acsaem.2c00631
摘要
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 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.
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