Inspired by the natural photosynthesis systems,the integrated harnessing and conversion of CO_(2) present a promising solution for addressing the ever-rising global atmospheric concentration of CO_(2).Hollow multi-she...Inspired by the natural photosynthesis systems,the integrated harnessing and conversion of CO_(2) present a promising solution for addressing the ever-rising global atmospheric concentration of CO_(2).Hollow multi-shelled structured(HoMS)photocatalysts,featuring alternating shells and cavities,have recently gained recognition as efficient nano-reactors for capturing CO_(2) molecules and facilitating effective photoreduction within these hierarchical structures,leveraging the preeminent enrichment effect.In this work,to augment the photocatalytic efficacy of HoMS in CO_(2) treatment,highly dispersed Cu_(x)O nanoparticles(NPs)were incorporated on the CeO2 shells through a polymer-assisted impregnation method to create more active sites and strengthen the interaction between the hetero-shells and CO_(2) molecules.The photoreduction of the CO_(2)-to-CO rate under a diluted CO_(2)(15%,volume fraction)atmosphere is improved by the introduction of Cu_(x)O NPs,with the highest CO yielding rate reaching 120µmol·h^(−1)·g^(−1) without any sacrificial reagents.Further comparison experiments and theoretical calculations reveal that the Cu_(x)O NPs promote the adsorption of CO_(2) molecules in HoMS,accelerate the charge transfer efficiency,and stabilize the surface oxygen vacancies(Ovs)during the photoreduction CO_(2) conversion process.We hope these easy-to-prepare HoMS nanoreactors can contribute to the effective enrichment and valorization of CO_(2) in industrial exhaust gases.展开更多
基金This work was supported by the National Natural Science Foundation of China(Nos.51932001,52272097,and 52372170)the Beijing Natural Science Foundation,China(Nos.2242019 and 2232068)the National Key Research and Development Program of China(No.2018YFA0703503).
文摘Inspired by the natural photosynthesis systems,the integrated harnessing and conversion of CO_(2) present a promising solution for addressing the ever-rising global atmospheric concentration of CO_(2).Hollow multi-shelled structured(HoMS)photocatalysts,featuring alternating shells and cavities,have recently gained recognition as efficient nano-reactors for capturing CO_(2) molecules and facilitating effective photoreduction within these hierarchical structures,leveraging the preeminent enrichment effect.In this work,to augment the photocatalytic efficacy of HoMS in CO_(2) treatment,highly dispersed Cu_(x)O nanoparticles(NPs)were incorporated on the CeO2 shells through a polymer-assisted impregnation method to create more active sites and strengthen the interaction between the hetero-shells and CO_(2) molecules.The photoreduction of the CO_(2)-to-CO rate under a diluted CO_(2)(15%,volume fraction)atmosphere is improved by the introduction of Cu_(x)O NPs,with the highest CO yielding rate reaching 120µmol·h^(−1)·g^(−1) without any sacrificial reagents.Further comparison experiments and theoretical calculations reveal that the Cu_(x)O NPs promote the adsorption of CO_(2) molecules in HoMS,accelerate the charge transfer efficiency,and stabilize the surface oxygen vacancies(Ovs)during the photoreduction CO_(2) conversion process.We hope these easy-to-prepare HoMS nanoreactors can contribute to the effective enrichment and valorization of CO_(2) in industrial exhaust gases.
