The reduction of CO_(2)into high value-added chemicals and fuels by a photocatalytic technology can relieve energy shortages and the environmental problems caused by greenhouse effects.In the current work,an amino-fun...The reduction of CO_(2)into high value-added chemicals and fuels by a photocatalytic technology can relieve energy shortages and the environmental problems caused by greenhouse effects.In the current work,an amino-functionalized zirconium metal organic framework(Zr-MOF)was covalently modified with different functional groups via the condensation of Zr-MOF with 2-pyridinecarboxaldehyde(PA),salicylaldehyde(SA),benzaldehyde(BA),and trifluoroacetic acid(TA),named Zr-MOF-X(X=PA,SA,BA,and TA),respectively,through the post-synthesis modification.Compared with Zr-MOF and Zr-MOF-TA,the introduction of PA,SA,or BA into the framework of Zr-MOF can not only enhance the visible-light harvesting and CO_(2)capture,but also accelerate the photogenerated charge separation and transfer,thereby improving the photocatalytic ability of Zr-MOF for CO_(2)reduction.These results indicate that the modification of Zr-MOF with electron-donating groups can promote the photocatalytic CO_(2)reduction.Therefore,the current work provides an instructive approach to improve the photocatalytic efficiency of CO_(2)reduction through the covalent modification of MOFs.展开更多
基金We gratefully acknowledge financial support from the Zhejiang Provincial Key R&D Project(No.2019C03118)the Programme of Introducing Talents of Discipline to Universities(No.D17008).
文摘The reduction of CO_(2)into high value-added chemicals and fuels by a photocatalytic technology can relieve energy shortages and the environmental problems caused by greenhouse effects.In the current work,an amino-functionalized zirconium metal organic framework(Zr-MOF)was covalently modified with different functional groups via the condensation of Zr-MOF with 2-pyridinecarboxaldehyde(PA),salicylaldehyde(SA),benzaldehyde(BA),and trifluoroacetic acid(TA),named Zr-MOF-X(X=PA,SA,BA,and TA),respectively,through the post-synthesis modification.Compared with Zr-MOF and Zr-MOF-TA,the introduction of PA,SA,or BA into the framework of Zr-MOF can not only enhance the visible-light harvesting and CO_(2)capture,but also accelerate the photogenerated charge separation and transfer,thereby improving the photocatalytic ability of Zr-MOF for CO_(2)reduction.These results indicate that the modification of Zr-MOF with electron-donating groups can promote the photocatalytic CO_(2)reduction.Therefore,the current work provides an instructive approach to improve the photocatalytic efficiency of CO_(2)reduction through the covalent modification of MOFs.
