TY - JOUR
T1 - Siliceous mesocellular foam (MCF) supported Cu catalysts for promoting non-thermal plasma activated CO2 hydrogenation towards methanol synthesis
AU - Chen, Yi
AU - Shao, Yan
AU - Quan, Cui
AU - Gao, Ningbo
AU - Fan, Xiaolei
AU - Chen, Huanhao
PY - 2024/1/20
Y1 - 2024/1/20
N2 - Electrified non-thermal plasma (NTP) catalytic hydrogenation is the promising alternative to the thermal counterparts, being able to be operated under mild conditions and compatible with green electricity/hydrogen. Rational design of the catalysts for such NTP-catalytic systems is one of the keys to improve the process efficiency. Here, we present the development of siliceous mesocellular foam (MCF) supported Cu catalysts for NTP-catalytic CO2 hydrogenation to methanol. The findings show that the pristine MCF support with high specific surface area and large mesopore of 784 m2 g−1 and ~8.5 nm could promote the plasma discharging and the diffusion of species through its framework, outperforming other control porous materials (viz., silicalite-1, SiO2, and SBA-15). Compared to the NTP system employing the bare MCF, the inclusion of Cu and Zn in MCF (i.e., Cu1Zn1/MCF) promoted the methanol formation of the NTP-catalytic system with a higher space-time yield (STY) of methanol at ~275 μmol gcat−1 h−1 and a lower energy consumption of 26.4 kJ mmolCH3OH−1 (conversely, ~225 μmol gcat−1 h−1 and ~71 kJ mmolCH3OH−1, respectively, for the bare MCF system at 10.1 kV). The findings suggest that inclusion of active metal sites (especially Zn species) could stabilize the CO2/CO-related intermediates to facilitate the surface reaction towards methanol formation.
AB - Electrified non-thermal plasma (NTP) catalytic hydrogenation is the promising alternative to the thermal counterparts, being able to be operated under mild conditions and compatible with green electricity/hydrogen. Rational design of the catalysts for such NTP-catalytic systems is one of the keys to improve the process efficiency. Here, we present the development of siliceous mesocellular foam (MCF) supported Cu catalysts for NTP-catalytic CO2 hydrogenation to methanol. The findings show that the pristine MCF support with high specific surface area and large mesopore of 784 m2 g−1 and ~8.5 nm could promote the plasma discharging and the diffusion of species through its framework, outperforming other control porous materials (viz., silicalite-1, SiO2, and SBA-15). Compared to the NTP system employing the bare MCF, the inclusion of Cu and Zn in MCF (i.e., Cu1Zn1/MCF) promoted the methanol formation of the NTP-catalytic system with a higher space-time yield (STY) of methanol at ~275 μmol gcat−1 h−1 and a lower energy consumption of 26.4 kJ mmolCH3OH−1 (conversely, ~225 μmol gcat−1 h−1 and ~71 kJ mmolCH3OH−1, respectively, for the bare MCF system at 10.1 kV). The findings suggest that inclusion of active metal sites (especially Zn species) could stabilize the CO2/CO-related intermediates to facilitate the surface reaction towards methanol formation.
KW - Non-thermal plasma (NTP) catalysis
KW - Cu catalyst
KW - CO2 hydrogenation
KW - methanol
KW - siliceous mesocellular foam (MCF)
M3 - Article
SN - 2095-0179
JO - Frontiers of Chemical Science and Engineering
JF - Frontiers of Chemical Science and Engineering
ER -