Docking MOF crystals on graphene support for highly selective electrocatalytic peroxide production

被引：20

作者：

Huang, Xiaofeng ^{[1
]}

Oleynikov, Peter ^{[1
]}

He, Hailong ^{[1
]}

Mayoral, Alvaro ^{[1
]}

Mu, Linqin ^{[2
]}

Lin, Feng ^{[2
]}

Zhang, Yue-Biao ^{[1
]}

机构：

[1] ShanghaiTech Univ, Sch Phys Sci & Technol, Shanghai 201210, Peoples R China

[2] Virginia Tech, Dept Chem, Blacksburg, VA 24061 USA

来源：

NANO RESEARCH | 2022年 / 15卷 / 01期

基金：

中国国家自然科学基金;

关键词：

metal-organic frameworks; nanocomposites; support effect; oxygen reduction reaction; peroxide selectivity;

D O I：

10.1007/s12274-021-3382-3

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：

Tailoring the reaction kinetics is the central theme of designer electrocatalysts, which enables the selective conversion of abundant and inert atmospheric species into useful products. Here we show a supporting effect in tuning the electrocatalytic kinetics of oxygen reduction reaction (ORR) from four-electron to two-electron mechanism by docking metalloporphyrin-based metal-organic frameworks (MOFs) crystals on graphene support, leading to highly selective peroxide production with faradaic efficiency as high as 93.4%. A magic angle of 38.1 degrees tilting for the co-facial alignment was uncovered by electron diffraction tomography, which is attributed to the maximization of pi-pi interaction for mitigating the lattice and symmetry mismatch between MOF and graphene. The facilitated electron migration and oxygen chemisorption could be ascribed to the supportive effect of graphene that disperses of the electron state of the active center, and ultimately regulates rate-determining step.

引用

页码：145 / 152

页数：8

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