Modulating the electronic spin state by constructing dual-metal atomic pairs for activating the dynamic site of oxygen reduction reaction

被引:0
作者
Shenghua Ye
Shuhua Xie
Yaqi Lei
Xiuyuan Yang
Jing Hu
Lirong Zheng
Zhida Chen
Yonghuan Fu
Xiangzhong Ren
Yongliang Li
Xiaoping Ouyang
Qianling Zhang
Jianhong Liu
Xueliang Sun
机构
[1] Shenzhen University,College of Chemistry and Environmental Engineering, Graphene Composite Research Center
[2] University of Western Ontario,Department of Mechanical and Materials Engineering
[3] Shenzhen Eigen-Equation Graphene Technology Co. Ltd.,School of Materials Science and Engineering
[4] Institute of High Energy Physics Chinese Academy of Sciences,undefined
[5] Xiangtan University,undefined
关键词
manganese (Mn)-iron (Fe) binuclear sites; synergistic effect; spin state; oxygen reduction reaction;
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学科分类号
摘要
In this study, dual-metal atomic pairs of manganese (Mn)-iron (Fe) binuclear sites (BNSs) with two conjoint MnN4 and FeN4 moieties (MnFeN8) anchored onto a graphite-like structure (GLS) (Mn-Fe BNSs/GLS) were constructed. The binuclear MnFeN8 structure was verified experimentally and theoretically. Magnetic measurements and Gaussian calculations reveal that this unique Mn-Fe BNSs exhibit strong short-range electronic interaction between Mn and Fe sites, which decouples two paired d electrons in Fe sites, thereby transforming Fe sites from an intermediate to a high spin state. The optimal electronic configuration of Fe sites and their binuclear structure facilitate an oxygen reduction reaction (ORR) thermodynamically and dynamically, respectively, endowing Mn-Fe BNSs with improved ORR performance.
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页码:1869 / 1877
页数:8
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