Self-supported transition-metal single-atom catalysts(SACs)facilitate the industrialization of electro-chemical CO2 reduction,but suffer from high structural heterogeneity with limited catalytic selectivity.Here we present a facile and scalable approach for the synthesis of self-supported nickel@nitrogen-doped carbon nanotubes grown on carbon nanofiber membrane(Ni@NCNTs/CFM),where the Ni single atoms and nanoparticles(NPs)are anchored on the wall and inside of nitrogen-doped carbon nanotubes,re-spectively.The side effect of Ni NPs was further effectively inhibited by alloying Ni with Cu atoms to alter their d-band center,which is theoretically predicted and experimentally proved.The optimal cata-lyst Ni9Cu1@NCNTs/CFM exhibits an ultrahigh CO Faradic efficiency over 97％at-0.7 V versus reversible hydrogen electrode.Additionally,this catalyst shows excellent mechanical strength which can be directly used as a self-supporting catalyst for Zn-CO2 battery with a peak power density of～0.65 mW/cm2 at 2.25 mA/cm2 and a long-term stability for 150 cycles.This work opens up a general avenue to facilely prepare self-supported SACs with unitary single-atom site for CO2 utilization.

Science and Technology on Advanced Ceramic Fibers and Composites Laboratory,College of Aerospace Science and Engineering,National University of Defense Technology,Changsha 410073,China

[1]Shujin Shen;Cheng Han;Bing Wang;Yingde Wang-.Engineering d-band center of nickel in nickel@nitrogen-doped carbon nanotubes array for electrochemical reduction of CO2 to CO and Zn-CO2 batteries)[J].中国化学快报（英文版）,2022(08):3721-3725

Ni9Cu1

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