TY - JOUR
T1 - Boosting electrocatalytic CO2–to–ethanol production via asymmetric C–C coupling
AU - Wang, Pengtang
AU - Yang, Hao
AU - Tang, Cheng
AU - Wu, Yu
AU - Zheng, Yao
AU - Cheng, Tao
AU - Davey, Kenneth
AU - Huang, Xiaoqing
AU - Qiao, Shi Zhang
N1 - Publisher Copyright:
© 2022, The Author(s).
PY - 2022/12
Y1 - 2022/12
N2 - Electroreduction of carbon dioxide (CO2) into multicarbon products provides possibility of large-scale chemicals production and is therefore of significant research and commercial interest. However, the production efficiency for ethanol (EtOH), a significant chemical feedstock, is impractically low because of limited selectivity, especially under high current operation. Here we report a new silver–modified copper–oxide catalyst (dCu2O/Ag2.3%) that exhibits a significant Faradaic efficiency of 40.8% and energy efficiency of 22.3% for boosted EtOH production. Importantly, it achieves CO2–to–ethanol conversion under high current operation with partial current density of 326.4 mA cm−2 at −0.87 V vs reversible hydrogen electrode to rank highly significantly amongst reported Cu–based catalysts. Based on in situ spectra studies we show that significantly boosted production results from tailored introduction of Ag to optimize the coordinated number and oxide state of surface Cu sites, in which the *CO adsorption is steered as both atop and bridge configuration to trigger asymmetric C–C coupling for stablization of EtOH intermediates.
AB - Electroreduction of carbon dioxide (CO2) into multicarbon products provides possibility of large-scale chemicals production and is therefore of significant research and commercial interest. However, the production efficiency for ethanol (EtOH), a significant chemical feedstock, is impractically low because of limited selectivity, especially under high current operation. Here we report a new silver–modified copper–oxide catalyst (dCu2O/Ag2.3%) that exhibits a significant Faradaic efficiency of 40.8% and energy efficiency of 22.3% for boosted EtOH production. Importantly, it achieves CO2–to–ethanol conversion under high current operation with partial current density of 326.4 mA cm−2 at −0.87 V vs reversible hydrogen electrode to rank highly significantly amongst reported Cu–based catalysts. Based on in situ spectra studies we show that significantly boosted production results from tailored introduction of Ag to optimize the coordinated number and oxide state of surface Cu sites, in which the *CO adsorption is steered as both atop and bridge configuration to trigger asymmetric C–C coupling for stablization of EtOH intermediates.
UR - http://www.scopus.com/inward/record.url?scp=85133143415&partnerID=8YFLogxK
U2 - 10.1038/s41467-022-31427-9
DO - 10.1038/s41467-022-31427-9
M3 - Article
C2 - 35768462
AN - SCOPUS:85133143415
SN - 2041-1723
VL - 13
JO - Nature Communications
JF - Nature Communications
IS - 1
M1 - 3754
ER -