Strategic Structure Tuning of Yolk-Shell Microcages for Efficient Nitrogen Fixation
journal contribution
posted on 2024-11-17, 14:19authored byHuinan Guo, Weiqin Li, Kai Chen, Mengyuan Yue, Yike Huang, Yafei Liu, Huaxu Shao, Chengcheng Chen, Caiyun Wang, Yijing Wang
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 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 . This catalyst displayed excellent catalytic activities for ENRR: a high NH yield of 12.87 μg mg h 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 yield rate was 11.29 μg mg h , 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 and achieve NH fixation. 2 3 3 cat 3 cat 2 3 −1 −1 −1 −1
Funding
National Natural Science Foundation of China (51871123)