TY - JOUR
T1 - Highly correlation of CO2 reduction selectivity and surface electron Accumulation
T2 - A case study of Au-MoS2 and Ag-MoS2 catalyst
AU - Sun, Songmei
AU - An, Qi
AU - Watanabe, Motonori
AU - Cheng, Junfang
AU - Ho Kim, Hack
AU - Akbay, Taner
AU - Takagaki, Atsushi
AU - Ishihara, Tatsumi
N1 - Funding Information:
This work received financial support from National Natural Science Foundation of China (No. 21671197 ), the World Premier International Research Center Initiative (WPI Initiative) on Carbon-Neutral Energy Research (I 2 CNER) , MEXT (Japan) and Technology Commission and Grant-in-Aid for Specially Promoted Research (No.16H06293) from MEXT (Japan).
Publisher Copyright:
© 2020
PY - 2020/8/15
Y1 - 2020/8/15
N2 - Artificial photosynthesis from CO2 reduction to methane is severely hampered by the kinetically challenging eight-electron transfer process. Accumulated electrons has been demonstrated can decrease this kinetic barrier. However, charge accumulation were mainly reported in several homogenous systems because of its difficulties in heterogenous systems. Here we identify that highly accumulated electrons exist in Au loaded ultrathin MoS2 under light irradiation, resulting in a superior performance of CO2 reduction to methane. The selectivity for methane is up to 80 % with an average production rate of about 19.38 μmolg−1 h−1 in pure water. Further detailed studies reveal that plasmon-excited hot electrons transfer from Au to charged excitons in ultrathin MoS2 promotes electron accumulation and multi-electron CO2 reduction kinetics for methane generation. This is further supported by the CO2 reduction performance of Ag-MoS2. Along with the vanished accumulated electrons, CO is the main product with a selectivity of 98 %.
AB - Artificial photosynthesis from CO2 reduction to methane is severely hampered by the kinetically challenging eight-electron transfer process. Accumulated electrons has been demonstrated can decrease this kinetic barrier. However, charge accumulation were mainly reported in several homogenous systems because of its difficulties in heterogenous systems. Here we identify that highly accumulated electrons exist in Au loaded ultrathin MoS2 under light irradiation, resulting in a superior performance of CO2 reduction to methane. The selectivity for methane is up to 80 % with an average production rate of about 19.38 μmolg−1 h−1 in pure water. Further detailed studies reveal that plasmon-excited hot electrons transfer from Au to charged excitons in ultrathin MoS2 promotes electron accumulation and multi-electron CO2 reduction kinetics for methane generation. This is further supported by the CO2 reduction performance of Ag-MoS2. Along with the vanished accumulated electrons, CO is the main product with a selectivity of 98 %.
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U2 - 10.1016/j.apcatb.2020.118931
DO - 10.1016/j.apcatb.2020.118931
M3 - Article
AN - SCOPUS:85082670654
SN - 0926-3373
VL - 271
JO - Applied Catalysis B: Environmental
JF - Applied Catalysis B: Environmental
M1 - 118931
ER -