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Strategic Structure Tuning of Yolk‐Shell Microcages for Efficient Nitrogen Fixation
Author(s) -
Guo Huinan,
Li Weiqin,
Chen Kai,
Yue Mengyuan,
Huang Yike,
Liu Yafei,
Shao Huaxu,
Chen Chengcheng,
Wang Caiyun,
Wang Yijing
Publication year - 2021
Publication title -
chemsuschem
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 2.412
H-Index - 157
eISSN - 1864-564X
pISSN - 1864-5631
DOI - 10.1002/cssc.202100502
Subject(s) - catalysis , faraday efficiency , chemical engineering , reversible hydrogen electrode , yield (engineering) , chemistry , materials science , electrochemistry , ammonia , dissolution , inorganic chemistry , electrode , organic chemistry , composite material , working electrode , engineering
The electrocatalytic nitrogen reduction reaction (ENRR) under ambient conditions is considered as a promising process to produce ammonia. Towards highly efficient catalysts, here an optimized one‐step pyrolysis strategy was tailored to design yolk–shell microcages (YS Co@C/BLCNTs), consisting of Co nanocrystals encapsulated in N‐doped carbon framework and bridged by bamboo‐like carbon nanotubes (BLCNTs). The cavity created between yolk and shell not only served as a “micro‐bag” to store the reactant N 2 and enhance its dissolution, but also induced a “cage effect” to confine the diffusion of reaction intermediate, hence making the reaction proceed in the direction of producing NH 3 . This catalyst displayed excellent catalytic activities for ENRR: a high NH 3 yield of 12.87 μg mg cat −1 h −1 at a high faradaic efficiency of 20.7 % at −0.45 V (vs. reversible hydrogen electrode, RHE). After 5 cycles of consecutive ENRR process, the NH 3 yield rate was 11.29 μg mg cat −1 h −1 , indicating the excellent electrocatalytic stability. These results provide a structural engineering for ENRR catalyst with doped N, cooperating with non‐precious metal to activate the inert triple bond of N 2 and achieve NH 3 fixation.