摘要
Ambient electrocatalytic nitrogen fixation is an emerging technology for green ammonia synthesis,but the absence of optimized,stable and performant catalysts can render its practical application challenging.Herein,bimetallic NiCo boride nanoparticles confined in MXene are shown to accomplish highperformance nitrogen reduction electrolysis.Ta king advantage of the synergistic effect in specific compositions with unique electronic d and p orbits and typical architecture of rich nanosized particles embedded in the interconnected conductive network,the synthesized MXene@NiCoB composite demonstrates extensive improvements in nitrogen molecule chemisorption,active area exposure and charge transport.As a result,optimal NH3 yield rate of 38.7μg h^(-1) mgcat^(-1).and Faradaic efficiency of 6.92%are acquired in0.1 M Na_(2)SO_(4) electrolyte.Moreover,the great catalytic performance can be almost entirely maintained in the cases of repeatedly-cycled and long-term electrolysis.Theoretical investigations reveal that the nitrogen reduction reaction on MXene@NiCoB catalyst proceeds according to the distal pathway,with a distinctly-reduced energy barrier relative to the Co2B counterpart.This work may inspire a new route towards the rational catalyst design for the nitrogen reduction reaction.
基金
financially supported by the National Natural Science Foundation of China(No.21878063)
Key Program of Shandong Provincial Natural Science Foundation(No.ZR2020KB011)
Taishan Scholars Program of Shandong Province(No.tsqn201909119)
financial support from the Flemish Government through the Moonshot cSBO project P2C(HBC.2019.0108)
through long-term structural funding(Methusalem CASAS2,Meth/15/04)。