A pyrolysis-free path toward superiorly catalytic nitrogen-coordinated single atom

氮原子 催化作用 路径(计算) 热解 化学 Atom(片上系统) 氮气 计算机科学 生物化学 并行计算 计算机网络 有机化学 群(周期表)
作者
Peng Peng,Lei Shi,Feng Huo,Chunxia Mi,Xiaohong Wu,Suojiang Zhang,Zhonghua Xiang
出处
期刊:Science Advances [American Association for the Advancement of Science]
卷期号:5 (8) 被引量:323
标识
DOI:10.1126/sciadv.aaw2322
摘要

Nitrogen-coordinated single-atom catalysts (SACs) have emerged as a frontier for electrocatalysis (such as oxygen reduction) with maximized atom utilization and highly catalytic activity. The precise design and operable synthesis of SACs are vital for practical applications but remain challenging because the commonly used high-temperature treatments always result in unpredictable structural changes and randomly created single atoms. Here, we develop a pyrolysis-free synthetic approach to prepare SACs with a high electrocatalytic activity using a fully π-conjugated iron phthalocyanine (FePc)-rich covalent organic framework (COF). Instead of randomly creating Fe-nitrogen moieties on a carbon matrix (Fe-N-C) through pyrolysis, we rivet the atomically well-designed Fe-N-C centers via intermolecular interactions between the COF network and the graphene matrix. The as-synthesized catalysts demonstrate exceptional kinetic current density in oxygen reduction catalysis (four times higher than the benchmark Pt/C) and superior power density and cycling stability in Zn-air batteries compared with Pt/C as air electrodes.
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