TY - JOUR
T1 - MOF Encapsulating N-Heterocyclic Carbene-Ligated Copper Single-Atom Site Catalyst towards Efficient Methane Electrosynthesis
AU - Chen, Shenghua
AU - Li, Wen-Hao
AU - Jiang, Wenjun
AU - Yang, Jiarui
AU - Zhu, Jiexin
AU - Wang, Liqiang
AU - Ou, Honghui
AU - Zhuang, Zechao
AU - Chen, Mingzhao
AU - Sun, Xiaohui
AU - Wang, Dingsheng
AU - Li, Yadong
PY - 2022/1/21
Y1 - 2022/1/21
N2 - The exploitation of highly efficient carbon dioxide reduction (CO2RR) electrocatalyst for methane (CH4) electrosynthesis has attracted great attention for the intermittent renewable electricity storage but remains challenging. Here, N-heterocyclic carbene (NHC)-ligated copper single atom site (Cu SAS) embedded in metal–organic framework is reported (2Bn-Cu@UiO-67), which can achieve an outstanding Faradaic efficiency (FE) of 81 % for the CO2 reduction to CH4 at −1.5 V vs. RHE with a current density of 420 mA cm−2. The CH4 FE of our catalyst remains above 70 % within a wide potential range and achieves an unprecedented turnover frequency (TOF) of 16.3 s−1. The σ donation of NHC enriches the surface electron density of Cu SAS and promotes the preferential adsorption of CHO* intermediates. The porosity of the catalyst facilitates the diffusion of CO2 to 2Bn-Cu, significantly increasing the availability of each catalytic center. © 2021 Wiley-VCH GmbH.
AB - The exploitation of highly efficient carbon dioxide reduction (CO2RR) electrocatalyst for methane (CH4) electrosynthesis has attracted great attention for the intermittent renewable electricity storage but remains challenging. Here, N-heterocyclic carbene (NHC)-ligated copper single atom site (Cu SAS) embedded in metal–organic framework is reported (2Bn-Cu@UiO-67), which can achieve an outstanding Faradaic efficiency (FE) of 81 % for the CO2 reduction to CH4 at −1.5 V vs. RHE with a current density of 420 mA cm−2. The CH4 FE of our catalyst remains above 70 % within a wide potential range and achieves an unprecedented turnover frequency (TOF) of 16.3 s−1. The σ donation of NHC enriches the surface electron density of Cu SAS and promotes the preferential adsorption of CHO* intermediates. The porosity of the catalyst facilitates the diffusion of CO2 to 2Bn-Cu, significantly increasing the availability of each catalytic center. © 2021 Wiley-VCH GmbH.
KW - CH4 electrosynthesis
KW - CO2RR
KW - Cu single-atom site catalyst
KW - n-heterocyclic carbene
UR - http://www.scopus.com/inward/record.url?scp=85120942651&partnerID=8YFLogxK
UR - https://www.scopus.com/record/pubmetrics.uri?eid=2-s2.0-85120942651&origin=recordpage
U2 - 10.1002/anie.202114450
DO - 10.1002/anie.202114450
M3 - RGC 21 - Publication in refereed journal
C2 - 34767294
SN - 1433-7851
VL - 61
JO - Angewandte Chemie - International Edition
JF - Angewandte Chemie - International Edition
IS - 4
M1 - e202114450
ER -
