Li Jingjing, Xia Wei, Tang Jing, Gao Yong, Jiang Cheng, Jia Yining, Chen Tao, Hou Zhufeng, Qi Ruijuan, Jiang Dong, Asahi Toru, Xu Xingtao, Wang Tao, He Jianping, Yamauchi Yusuke
College of Materials Science and Technology, Jiangsu Key Laboratory of Electrochemical Energy Storage Technologies, Nanjing University of Aeronautics and Astronautics, Nanjing 210016, China.
School of Chemistry and Molecular Engineering, Shanghai Key Laboratory of Green Chemistry and Chemical Processes, Institute of Eco-Chongming, East China Normal University, Shanghai 200062, China.
J Am Chem Soc. 2022 Jun 1;144(21):9280-9291. doi: 10.1021/jacs.2c00719. Epub 2022 May 23.
This study demonstrates a special ultrathin N-doped graphene nanomesh (NGM) as a robust scaffold for highly exposed Fe-N active sites. Significantly, the pore sizes of the NGM can be elaborately regulated by adjusting the thermal exfoliation conditions to simultaneously disperse and anchor Fe-N moieties, ultimately leading to highly loaded Fe single-atom catalysts (SA-Fe-NGM) and a highly exposed morphology. The SA-Fe-NGM is found to deliver a superior oxygen reduction reaction (ORR) activity in acidic media (half-wave potential = 0.83 V RHE) and a high power density of 634 mW cm in the H/O fuel cell test. First-principles calculations further elucidate the possible catalytic mechanism for ORR based on the identified Fe-N active sites and the pore size distribution analysis. This work provides a novel strategy for constructing highly exposed transition metals and nitrogen co-doped carbon materials (M-N-C) catalysts for extended electrocatalytic and energy storage applications.
本研究展示了一种特殊的超薄氮掺杂石墨烯纳米网（NGM），作为用于高度暴露的Fe-N活性位点的坚固支架。值得注意的是，通过调节热剥离条件可以精细调控NGM的孔径，以同时分散和锚定Fe-N部分，最终得到高负载的Fe单原子催化剂（SA-Fe-NGM）和高度暴露的形态。研究发现，SA-Fe-NGM在酸性介质中具有优异的氧还原反应（ORR）活性（半波电位 = 0.83 V vs RHE），并且在氢氧燃料电池测试中具有634 mW cm的高功率密度。第一性原理计算基于所确定的Fe-N活性位点和孔径分布分析，进一步阐明了ORR可能的催化机制。这项工作为构建用于扩展电催化和储能应用的高度暴露的过渡金属与氮共掺杂碳材料（M-N-C）催化剂提供了一种新策略。
