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

被引：21

作者：

Ye, Shenghua ^{[1
]}

Xie, Shuhua ^{[1
]}

Lei, Yaqi ^{[1
]}

Yang, Xiuyuan ^{[1
]}

Hu, Jing ^{[1
]}

Zheng, Lirong ^{[4
]}

Chen, Zhida ^{[1
]}

Fu, Yonghuan ^{[1
]}

Ren, Xiangzhong ^{[1
]}

Li, Yongliang ^{[1
]}

Ouyang, Xiaoping ^{[5
]}

Zhang, Qianling ^{[1
]}

Liu, Jianhong ^{[1
,3
]}

Sun, Xueliang ^{[2
]}

机构：

[1] Shenzhen Univ, Graphene Composite Res Ctr, Coll Chem & Environm Engn, Shenzhen 518060, Peoples R China

[2] Univ Western Ontario, Dept Mech & Mat Engn, London, ON N6A 5B9, Canada

[3] Shenzhen Eigen Equat Graphene Technol Co Ltd, Shenzhen 518000, Peoples R China

[4] Chinese Acad Sci, Inst High Energy Phys, Beijing 100049, Peoples R China

[5] Xiangtan Univ, Sch Mat Sci & Engn, Xiangtan 411105, Peoples R China

来源：

NANO RESEARCH | 2023年 / 16卷 / 02期

基金：

中国国家自然科学基金;

关键词：

manganese (Mn)-iron (Fe) binuclear sites; synergistic effect; spin state; oxygen reduction reaction; ACTIVE-SITES; NITROGEN; CATALYSTS;

D O I：

10.1007/s12274-022-4979-x

中图分类号：

O64 [物理化学（理论化学）、化学物理学];

学科分类号：

070304 ; 081704 ;

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 BNSsIGLS) 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.

引用

页码：1869 / 1877

页数：9

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