首页|Surface engineering of ZnO electrocatalyst by N doping towards electrochemical CO2 reduction

Surface engineering of ZnO electrocatalyst by N doping towards electrochemical CO2 reduction

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The discovery of efficient,selective,and stable electrocatalysts can be a key point to produce the large-scale chemical fuels via electrochemical CO2 reduction(ECR).In this study,an earth-abundant and non-toxic ZnO-based electrocatalyst was developed for use in gas-diffusion electrodes(GDE),and the effect of nitrogen(N)doping on the ECR activity of ZnO electrocatalysts was investigated.Initially,a ZnO nanosheet was prepared via the hydrothermal method,and nitridation was performed at different times to control the N-doping content.With an increase in the N-doping content,the morphological properties of the nanosheet changed significantly,namely,the 2D nanosheets transformed into irregularly shaped nanoparticles.Furthermore,the ECR performance of ZnO electrocatalysts with different N-doping content was assessed in 1.0 M KHCO3 electrolyte using a gas-diffusion electrode-based ECR cell.While the ECR activity increased after a small amount of N doping,it decreased for higher N doping content.Among them,the N∶ZnO-1 h electrocatalysts showed the best CO selectivity,with a faradaic efficiency(FECO)of 92.7％at-0.73 V vs.reversible hydrogen electrode(RHE),which was greater than that of an undoped ZnO electrocatalyst(FECO of 63.4％at-0.78 VRHE).Also,the N∶ZnO-1 h electrocatalyst exhibited outstand-ing durability for 16 h,with a partial current density of-92.1 mA cm-2.This improvement of N∶ZnO-1 h electrocatalyst can be explained by density functional theory calculations,demonstrating that this improvement of N∶ZnO-1 h electrocatalyst comes from(ⅰ)the optimized active sites lowering the free energy barrier for the rate-determining step(RDS),and(ⅱ)the modification of electronic structure enhancing the electron transfer rate by N doping.

ZnON-doped ZnOGas-diffusion electrodeCO SelectivityElectrochemical CO2 reduction

Rohini Subhash Kanase、Getasew Mulualem Zewdie、Maheswari Arunachalam、Jyoti Badiger、Suzan Abdelfattah Sayed、Kwang-Soon Ahn、Jun-Seok Ha、Uk Sim、Hyeyoung Shin、Soon Hyung Kang

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Department of Interdisciplinary Program for Photonic Engineering,Chonnam National University,Gwangju 61186,Republic of Korea

Graduate School of Energy Science and Technology(GEST),Chungnam National University,99 Daehak-ro,Yuseong-gu,Daejeon 34134,Republic of Korea

Department of Chemistry Education and Optoelectronic Convergence Research Center,Chonnam National University,Gwangju 61186,Republic of Korea

Department of Advanced Chemicals and Engineering,Chonnam National University,Gwangju 61186,Republic of Korea

School of Chemical Engineering,Yeungnam University,Gyeongsan 38541,Republic of Korea

Department of Energy Engineering,Korea Institute of Energy Technology(KENTECH),Naju 58217,Republic of Korea

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Basic Science Research Program through the National Research Foundation of Korea(NRF)Basic Science Research Program through the National Research Foundation of Korea(NRF)Basic Science Research Program through the National Research Foundation of Korea(NRF)Basic Science Research Program through the National Research Foundation of Korea(NRF)Basic Science Research Capacity Enhancement Project through Korea Basic Science Institute

2018R1A6A1A030243342019R1A2C10076372021M3I3A10828802021R1I1A1A010441742019R1A6C1010024

2024

10.1016/j.jechem.2023.09.007

能源化学
中国科学院大连化学物理研究所 中国科学院成都有机化学研究所

能源化学

CSTPCDEI
影响因子：0.654
ISSN：2095-4956
年,卷(期)：2024.88(1)
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