Efficient photocatalytic reduction of CO_(2)is crucial to decrease the atmospheric concentration of CO_(2).Pairing this process with H_(2)O_(2)production is of considerable importance for simultaneously producing valu...Efficient photocatalytic reduction of CO_(2)is crucial to decrease the atmospheric concentration of CO_(2).Pairing this process with H_(2)O_(2)production is of considerable importance for simultaneously producing value-added chemicals.However,the photocatalysts reported for such a process suffer from a high recombination rate of the surface/bulk charges,as well as inefficient enrichment and activation toward CO_(2)and O_(2),resulting in low conversion efficiency even in the presence of organic sacrificial agents and expensive metal co-catalysts.Herein,two 1,3,5-triphenylbenzene-based organic polymers with high ionic density and porosity are prepared through a facile Sonogashira polymerization.The ionic imidazolium sites embedded in the polymeric skeleton provide the two polymers(iCMP-1 and iCMP-2)with adsorptive selectivity for CO_(2)/N_(2) up to 98-102 at 273 K,facilitating the enrichment of CO_(2)and O_(2)molecules around the catalytic centers,thus boosting their catalytic conversion directly from air under solar light(100 mW cm^(-2)).Benefiting from the improved charge separation and broad light absorption,along with high CO_(2)and O_(2)uptake,iCMP-2 can deliver excellent CO and H_(2)O_(2)yields(611.8 and 810.6μmol h^(-1)g^(-1),respectively)under an atmosphere composed of water vapor and air without any co-catalysts.展开更多
基金supported by the Excellent Youth Foundation of Jiangxi Scientific Committee(no.20232ACB213012)National Science Foundation of Jiangxi Province of China(no.20242BAB25236)+2 种基金Jiangxi Talent Program(no.DHSQT32022005)Beijing Institute of Technology Research Fund Program for Young Scholars(XSQD-202215006)National Natural Science Foundation of China(no.22202008 and 22202039).
文摘Efficient photocatalytic reduction of CO_(2)is crucial to decrease the atmospheric concentration of CO_(2).Pairing this process with H_(2)O_(2)production is of considerable importance for simultaneously producing value-added chemicals.However,the photocatalysts reported for such a process suffer from a high recombination rate of the surface/bulk charges,as well as inefficient enrichment and activation toward CO_(2)and O_(2),resulting in low conversion efficiency even in the presence of organic sacrificial agents and expensive metal co-catalysts.Herein,two 1,3,5-triphenylbenzene-based organic polymers with high ionic density and porosity are prepared through a facile Sonogashira polymerization.The ionic imidazolium sites embedded in the polymeric skeleton provide the two polymers(iCMP-1 and iCMP-2)with adsorptive selectivity for CO_(2)/N_(2) up to 98-102 at 273 K,facilitating the enrichment of CO_(2)and O_(2)molecules around the catalytic centers,thus boosting their catalytic conversion directly from air under solar light(100 mW cm^(-2)).Benefiting from the improved charge separation and broad light absorption,along with high CO_(2)and O_(2)uptake,iCMP-2 can deliver excellent CO and H_(2)O_(2)yields(611.8 and 810.6μmol h^(-1)g^(-1),respectively)under an atmosphere composed of water vapor and air without any co-catalysts.
