Photo-thermal cooperation for the conversion of C02 and CH4 with H2O to C2 oxygenates over SrTiOx supported CuCo
Photosynthesis is a potential strategy to enable endergonic process that usually needs high-temperature in thermochemistry to supply the energy for inert-bond activation and/or strong endothermic reaction.The conversion of CO2 into value-added C2-oxygenates is a promising process to realize artificial photosynthesis,but suffers from relatively lower efficiency due to complex mul-ti-electron(≥ 10)transfer processes and sluggish kinetics of C-C coupling.This work proposes an all-new H2O-promoted strategy for efficient production of C2 oxygenates from the concurrent acti-vation and subsequent co-conversion of CO2 with CH4 under photo-thermal cooperation,in which photocatalytic H2O-splitting derived active hydrogen species for CO2 activation,and concomitant active oxygen species for CH4 activation.A formation rate of as high as 2.05 mmol g-1 h-1 for C2-oxygenates(CH3CHO and CH3CH2OH)in a selectivity of＞86％has been afforded over SrTiOx supported CuCo under 200 ℃ and ultraviolet-visible illumination.It has been revealed that SrTiOx drives photocatalytic H 2O-splitting under the excitation primary from ultraviolet light,paired CuⅠ/Cu0 sites promote the formation of*CHxO intermediate from CO2,Co sites conduct CH4-to-*CH3,and C-C coupling of*CHxO and*CH3 on adjacent Cu-Co facilitates the generation of C2-oxygenates.
Photo-thermal cooperationCo-conversion of CO2 and CH4SrTiOx supported Cu-CoWater-splittingC2-oxygenates
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