Low-coordinated Ni-N_(1)-C_(3)sites atomically dispersed on hollow carbon nanotubes for efficient CO_(2)reduction  

作　　者：Fangqi Yang Haoming Yu Yun Su Jingwen Chen Shixia Chen Zheling Zeng Shuguang Deng Jun Wang 

机构地区：[1]School of Resource and Environment,Nanchang University,Nanchang 330031,China [2]Chemistry and Chemical Engineering School,Nanchang University,Nanchang 330031,China [3]School for Engineering of Matter,Transport and Energy,Arizona State University,Tempe,AZ 85287,USA

出　　处：《Nano Research》2023年第1期146-154,共9页纳米研究（英文版）

基　　金：supported by the National Natural Science Foundation of China(Nos.21908090,22008101,22108243,and 22168023);the Natural Science Foundation of Jiangxi Province(No.20212BAB213038);Y.F.acknowledges the 2020 Nanchang University Scholarship for Doctoral Visiting Abroad.

摘　　要：Low-coordinated single atom catalysts compared to M-N4 are appealing in optimized electronic structure for CO_(2)electroreduction,but the preparation is still very challenging.Herein,a novel single Ni atom catalyst with Ni-N_(1)-C_(3)configuration is in-situ evolved on curved carbon nanotubes.The obtained Ni-N_(1)-C_(3)catalyst exhibits a superior CO Faradaic efficiency of 97%and turnover frequency of 2,890 h^(−1)at−0.9 V versus the reversible hydrogen electrode,as well as long-term stability over 45 h.High current densities exceeding 200 mA·cm^(−2)and CO Faradaic efficiency of 99%are achieved in flow-cell.Moreover,in-situ potentialand time-dependent Raman spectra identify the key intermediates of*COOH and*CO during CO_(2)-to-CO conversion.Theoretical calculations reveal that the upward-shifted d-band center and charge-rich Ni sites of Ni-N_(1)-C_(3)facilitate the electron transfer to*COOH and thus reduce the*COOH formation energy barrier.This work demonstrates a strategy for modulating the coordination environment for efficient CO_(2)reduction.

关 键 词：CO_(2)reduction reaction single atom catalyst low-coordination DFT calculations in-situ Raman spectra 

分 类 号：O64[理学—物理化学]