Repurposing of carbon dioxide to valuable chemicals and fuels with the assistance of renewable energy is essential for balanced carbon cycle.Here,a new CO_(2)conversion strategy was demonstrated that utilized concentr...Repurposing of carbon dioxide to valuable chemicals and fuels with the assistance of renewable energy is essential for balanced carbon cycle.Here,a new CO_(2)conversion strategy was demonstrated that utilized concentrated solar energy to directly drive chemical looping reverse water gas shift process,which simultaneously coupled the photothermal and photochemical effects to achieve enhanced CO_(2)reduction reactivity and 100%CO selectivity.The solar-driven chemical looping CO_(2)reduction on Ni-Fe_(2)O_(3/)La_(0.8)Sr_(0.2)FeO_(3)exhibited great activity,with an average CO production rate of up to 0.28 mmol/g_(oc)/min at 283℃The product yield of the solar-driven reaction was almost 600%higher than that of the thermal reaction at the same temperature.The CO production overcame the thermodynamic equilibrium limitation under the combined impact of thermal and non-thermal effects of direct-light illumination.Light irradiation reinforced reactive gas adsorption and dissociation of carbonate intermediates,and stimulated oxygen ion migration and lattice oxygen transformation,thus promoting the reactivity.The concept of concentrated solar energy to drive chemical looping reverse water gas shift opens a new avenue for effective CO_(2)resource utilization and solar fuel production.展开更多
基金support by National Natural Science Foundation of China(NSFC)under Grant No.52488201(Basic Science Center Program),Grant No.52241601and 52176026。
文摘Repurposing of carbon dioxide to valuable chemicals and fuels with the assistance of renewable energy is essential for balanced carbon cycle.Here,a new CO_(2)conversion strategy was demonstrated that utilized concentrated solar energy to directly drive chemical looping reverse water gas shift process,which simultaneously coupled the photothermal and photochemical effects to achieve enhanced CO_(2)reduction reactivity and 100%CO selectivity.The solar-driven chemical looping CO_(2)reduction on Ni-Fe_(2)O_(3/)La_(0.8)Sr_(0.2)FeO_(3)exhibited great activity,with an average CO production rate of up to 0.28 mmol/g_(oc)/min at 283℃The product yield of the solar-driven reaction was almost 600%higher than that of the thermal reaction at the same temperature.The CO production overcame the thermodynamic equilibrium limitation under the combined impact of thermal and non-thermal effects of direct-light illumination.Light irradiation reinforced reactive gas adsorption and dissociation of carbonate intermediates,and stimulated oxygen ion migration and lattice oxygen transformation,thus promoting the reactivity.The concept of concentrated solar energy to drive chemical looping reverse water gas shift opens a new avenue for effective CO_(2)resource utilization and solar fuel production.
