催化作用
阴极
溶解
降级(电信)
材料科学
化学工程
燃料电池
浸出(土壤学)
耐久性
化学
计算机科学
物理化学
复合材料
环境科学
电信
生物化学
土壤科学
工程类
土壤水分
作者
Geunsu Bae,Minho M. Kim,Man Ho Han,Junsic Cho,Dong Hyun Kim,Moulay Tahar Sougrati,Jinjong Kim,Kug‐Seung Lee,Sang Hoon Joo,William A. Goddard,Hyung‐Suk Oh,Hyungjun Kim,Frédéric Jaouen,Chang Hyuck Choi
出处
期刊:Nature Catalysis
[Springer Nature]
日期:2023-09-28
卷期号:6 (12): 1140-1150
被引量:25
标识
DOI:10.1038/s41929-023-01039-7
摘要
Beyond great advances in initial activity, Fe–N–C catalysts face the next challenge of stability issue in acidic medium that must be overcome to replace Pt in fuel cell cathode. However, the complex phenomena in fuel cells and consequential difficulty in understanding deactivation mechanisms of Fe–N–C cathodes impede solutions for prolonged stability. Here we show time-resolved changes in active site density and turnover frequency of Fe–N–C along with concurrent decrease in oxygen reduction reaction current in a temperature/gas controllable gas-diffusion electrode flow cell. Operando diagnosis of Fe leaching identifies a strong dependence of site density changes on operating parameters and draws a lifetime-dependent stability diagram that reveals a shift in the prime degradation mechanism during operation. A proof-of-concept strategy with site-isolated Pt ions as a non-catalytic stabilizer, supported by theoretical calculations, demonstrates enhanced fuel cell stability with reduced Fe dissolution, offering design principles for durable Fe–N–C catalysts. Inexpensive Fe–N–C single-atom catalysts are a promising solution to replace costly Pt-based cathode catalysts in fuel cells, but they typically suffer from low durability. Now, the degradation mechanisms of Fe–N–C catalysts are identified under operando conditions as a function of time, and potential solutions are proposed.
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