Hypervelocity kinetics blocks harmful intermediates to enhance stability of Fe-N-C catalysts

IF 7.4 2区材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Science China Materials Pub Date : 2024-12-18 DOI:10.1007/s40843-024-3179-5

Zhenyang Xie (, ), Chunyan Zhang (, ), Zhuoyang Xie (, ), Zude Shen (, ), Linsen Liu (, ), Li Li (, ), Wei Ding (, ), Zidong Wei (, )

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Abstract

Hydrogen peroxide that is produced through the two-electron pathway during the catalysis of oxygen reduction reaction (ORR) is recognized as harmful to the stability of nitrogen-doped carbon and Fe-based nonprecious catalyst (Fe-N-C) for fuel cell application. A major remaining scientific question is how fast the removal of these deleterious intermediates can contribute to stability enhancement. Here, we report that the stability of Fe-N-C catalysts is positively correlated with the kinetic constant of hydrogen peroxide decomposition. Modulation of the H₂O₂ decomposition kinetics by applying the frequency factor of the Arrhenius equation from 800 to 30000 s⁻¹ for TiO₂, CeO₂ and ZrO₂ reduced the decay rate of Fe-N-C catalysts from 0.151% to −0.1% in a 100-hour stability test. Fe-N-C/ZrO₂ with a frequency factor of 30000 s⁻¹ showed a 10% increase in current density during a 100-hour stability test and almost no decay during 15 hours of continuous fuel cell operation at a high potential of 0.7 V.

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超高速动力学阻断了有害中间体，提高了Fe-N-C催化剂的稳定性

氧还原反应（ORR）催化过程中通过双电子途径产生的过氧化氢对燃料电池中氮掺杂碳和铁基非贵重催化剂（Fe-N-C）的稳定性有害。剩下的一个主要科学问题是，去除这些有害中间体的速度能多快有助于增强稳定性。本文报道了Fe-N-C催化剂的稳定性与过氧化氢分解的动力学常数呈正相关。采用Arrhenius方程频率因子从800 ~ 30000 s−1调制TiO2、CeO2和ZrO2的H2O2分解动力学，在100小时的稳定性试验中，Fe-N-C催化剂的衰减率从0.151%降低到−0.1%。频率因子为30000 s−1的Fe-N-C/ZrO2在100小时稳定性测试中电流密度增加10%，在0.7 V高电位下连续工作15小时几乎没有衰减。

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来源期刊

Science China Materials Materials Science-General Materials Science

CiteScore

11.40

自引率

7.40%

发文量

949

期刊介绍： Science China Materials (SCM) is a globally peer-reviewed journal that covers all facets of materials science. It is supervised by the Chinese Academy of Sciences and co-sponsored by the Chinese Academy of Sciences and the National Natural Science Foundation of China. The journal is jointly published monthly in both printed and electronic forms by Science China Press and Springer. The aim of SCM is to encourage communication of high-quality, innovative research results at the cutting-edge interface of materials science with chemistry, physics, biology, and engineering. It focuses on breakthroughs from around the world and aims to become a world-leading academic journal for materials science.