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Metal–Organic‐Framework‐Derived Hybrid Carbon Nanocages as a Bifunctional Electrocatalyst for Oxygen Reduction and Evolution
Author(s) -
Liu Shaohong,
Wang Zhiyu,
Zhou Si,
Yu Fengjiao,
Yu Mengzhou,
Chiang ChangYang,
Zhou Wuzong,
Zhao Jijun,
Qiu Jieshan
Publication year - 2017
Publication title -
advanced materials
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 10.707
H-Index - 527
eISSN - 1521-4095
pISSN - 0935-9648
DOI - 10.1002/adma.201700874
Subject(s) - nanocages , bifunctional , electrocatalyst , materials science , oxygen evolution , catalysis , metal organic framework , carbon fibers , chemical engineering , microporous material , electron transfer , nanotechnology , water splitting , adsorption , photochemistry , electrode , chemistry , photocatalysis , organic chemistry , electrochemistry , composite number , composite material , engineering
The oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) are cornerstone reactions for many renewable energy technologies. Developing cheap yet durable substitutes of precious‐metal catalysts, especially the bifunctional electrocatalysts with high activity for both ORR and OER reactions and their streamlined coupling process, are highly desirable to reduce the processing cost and complexity of renewable energy systems. Here, a facile strategy is reported for synthesizing double‐shelled hybrid nanocages with outer shells of Co‐N‐doped graphitic carbon (Co‐NGC) and inner shells of N‐doped microporous carbon (NC) by templating against core–shell metal–organic frameworks. The double‐shelled NC@Co‐NGC nanocages well integrate the high activity of Co‐NGC shells into the robust NC hollow framework with enhanced diffusion kinetics, exhibiting superior electrocatalytic properties to Pt and RuO 2 as a bifunctional electrocatalyst for ORR and OER, and hold a promise as efficient air electrode catalysts in Zn–air batteries. First‐principles calculations reveal that the high catalytic activities of Co‐NGC shells are due to the synergistic electron transfer and redistribution between the Co nanoparticles, the graphitic carbon, and the doped N species. Strong yet favorable adsorption of an OOH* intermediate on the high density of uncoordinated hollow‐site C atoms with respect to the Co lattice in the Co‐NGC structure is a vital rate‐determining step to achieve excellent bifunctional electrocatalytic activity.