TY - JOUR
T1 - Electroreduction of CO2 on Cu, Fe, or Ni-doped Diamane Sheets
T2 - A DFT Study
AU - Zhang, Hongping
AU - Zhang, Run
AU - Hu, Shuchun
AU - Yang, Kun
AU - Sun, Chenghua
AU - Wang, Qingyuan
AU - Tang, Youhong
PY - 2024/4/2
Y1 - 2024/4/2
N2 - Poor mass transfer behavior and inherent activity limit the efficiency of traditional catalysts in electrocatalyzing carbon dioxide reduction reactions. However, the development of novel nanomaterials provides new strategies to solve the above problems. Herein, we propose novel single-metal atom catalysts, namely diamane-based electrocatalysts doped with Cu, Fe, and Ni, explored through density functional theory (DFT) calculations. We thoroughly investigated the doping pattern and energetics for different dopants. Furthermore, we systematically investigated the conversion process of CO2 to C1 or C2+ products, utilizing the free energy analysis of reaction pathways. Our results reveal that dopants could only be introduced into diamane following a specific pattern. Dopants significantly enhance the CO2 adsorption ability of diamane, with Fe and Ni proving notably more effective than Cu. After CO2 adsorption, Cu- and Fe-doped diamane prefer to catalyze CO2RR, while Ni-doped diamane favors hydrogen evolution reaction (HER). The C−C coupling reaction on Cu-hollow diamane, Cu-bridge diamane, and Fe-hollow diamane tends to be from C2+ products. Among all examined catalysts, Cu-hollow diamane shows better electro-catalytic performance. Our study demonstrates the feasibility of and contributes to the development of diamane-based electro-catalysts for CO2RR.
AB - Poor mass transfer behavior and inherent activity limit the efficiency of traditional catalysts in electrocatalyzing carbon dioxide reduction reactions. However, the development of novel nanomaterials provides new strategies to solve the above problems. Herein, we propose novel single-metal atom catalysts, namely diamane-based electrocatalysts doped with Cu, Fe, and Ni, explored through density functional theory (DFT) calculations. We thoroughly investigated the doping pattern and energetics for different dopants. Furthermore, we systematically investigated the conversion process of CO2 to C1 or C2+ products, utilizing the free energy analysis of reaction pathways. Our results reveal that dopants could only be introduced into diamane following a specific pattern. Dopants significantly enhance the CO2 adsorption ability of diamane, with Fe and Ni proving notably more effective than Cu. After CO2 adsorption, Cu- and Fe-doped diamane prefer to catalyze CO2RR, while Ni-doped diamane favors hydrogen evolution reaction (HER). The C−C coupling reaction on Cu-hollow diamane, Cu-bridge diamane, and Fe-hollow diamane tends to be from C2+ products. Among all examined catalysts, Cu-hollow diamane shows better electro-catalytic performance. Our study demonstrates the feasibility of and contributes to the development of diamane-based electro-catalysts for CO2RR.
KW - CO
KW - Density functional theory
KW - Diamane
KW - Electroreduction
KW - Single atom catalyst
UR - http://www.scopus.com/inward/record.url?scp=85184693875&partnerID=8YFLogxK
U2 - 10.1002/chem.202303995
DO - 10.1002/chem.202303995
M3 - Article
C2 - 38246877
AN - SCOPUS:85184693875
SN - 0947-6539
VL - 30
JO - Chemistry - A European Journal
JF - Chemistry - A European Journal
IS - 19
M1 - e202303995
ER -