Highly Active Porous Carbon-Supported CoNi Bimetallic Catalysts for Four-Electron Reduction of Oxygen

催化作用 双金属片 合金 化学工程 碳纤维 材料科学 金属 阴极 浸出(土壤学) 氧化物 化学 无机化学 冶金 有机化学 复合材料 物理化学 环境科学 土壤水分 土壤科学 工程类 复合数
作者
Changke Shao,Mingsheng Luo,Huanqiao Song,Shixin Zhang,Fengli Wang,Xinyue Liu,Zitian Huang
出处
期刊:Energy & Fuels [American Chemical Society]
卷期号:37 (5): 4026-4037 被引量:9
标识
DOI:10.1021/acs.energyfuels.2c03812
摘要

Great interest has been taken in oxygen reduction reaction (ORR), as a common cathode reaction in new energy sources such as fuel cells and metal–air batteries, to improve the current energy structure and develop new green energy sources. Noble metal Pt is still considered the best catalyst for this reaction. However, its disadvantages such as high cost, low selectivity, poor stability, and susceptibility to impurity poisoning severely limit its further industrial applications. Therefore, development of efficient and low-cost ORR reduction catalysts is particularly critical. M-Nx-C materials have been extensively studied to achieve a high ORR activity close to that of Pt catalysts. In this study, CoNi bimetallic alloy carbon-based oxygen reduction catalysts named CoNi-950 (Zn) were successfully synthesized, using a metal–organic framework (MOF) as a carbon precursor and a nitrogen source. The experimental results show that CoNi-950 (Zn) exhibits good ORR catalytic performance with an ultimate current density of 6.27 mA cm–2, which even exceeds that of some Pt/C catalysts with a mass loading of 20 wt % (5.92 mA cm–2). In addition, the active site of the catalyst was also identified by acid leaching and SCN– poisoning experiments, showing two sites in the form of CoNi-Nx and the CoNi alloy or its oxides in the material. Further experiments demonstrate that these two active sites have distinct ORR catalytic mechanisms, generating positive synergism in ORR. A mechanism in which O2 was catalytically reduced by CoNi-950 (Zn) in a four-electron transfer, i.e., a continuous two-step dual-electron transfer reduction process in alkaline electrolytes, is proposed.
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