Coupling Fe and Mo single atoms on hierarchical N-doped carbon nanotubes enhances electrochemical nitrogen reduction reaction performance  

作　　者：Wenjie Cui Baokang Geng Xiang Chu Jianing He Lingxi Jia Xiaoxiao Han Xiao Wang Shuyan Song Hongjie Zhang 

机构地区：[1]State Key Laboratory of Rare Earth Resource Utilization,Changchun Institute of Applied Chemistry,Chinese Academy of Sciences,Changchun 130022,China [2]School of Applied Chemistry and Engineering,University of Science and Technology of China,Hefei 230026,China [3]Department of Chemistry,Tsinghua University,Beijing 100084,China

出　　处：《Nano Research》2023年第4期5743-5749,共7页纳米研究（英文版）

基　　金：supported by the financial aid from National Science and Technology Major Project of China(No.2021YFB3500700);National Natural Science Foundation of China(Nos.22020102003,22025506,and 22271274);Key Research Program of the Chinese Academy of Sciences(No.ZDRW-CN-2021-3-3);K.C.Wong Education Foundation(No.GJTD-2018-09);Innovation and Entrepreneurship Program of Jilin Province(No.E2390202).

摘　　要：Electrochemical nitrogen reduction reaction(NRR)paves a new way to cost-efficient production of ammonia,but is still challenging in the sluggish kinetics caused by hydrogen evolution reaction competition and chemical inertness of N≡N bond.Herein,we report a“dual-site”strategy for boosting NRR performance.A high-performance catalyst is successfully constructed by anchoring isolated Fe and Mo atoms on hierarchical N doped carbon nanotubes through a facile self-sacrificing template route,which exhibits a remarkably improved NH3 yield rate of 26.8μg·h^(−1)·mg with 11.8%Faradaic efficiency,which is 2.5 and 1.6 times larger than those of Fe/NC and Mo/NC.The enhancement can be attributed to the unique hierarchical structure that profits from the contact of electrode and electrolyte,thus improving the mass and electron transport.More importantly,the in situ Fourier transform infrared spectroscopy(in situ FTIR)result firmly demonstrates the crucial role of the coupling of Fe and Mo atoms,which can efficiently boost the generation and transmission of*N2Hy intermediates,leading to an accelerated reaction rate.

关 键 词：dual-site single atom hard template synergetic effect nitrogen reduction reaction(NRR) 

分 类 号：O64[理学—物理化学]