The linker defect engineering for MOFs is a viable strategy that usually can effectively augment conductivity to further promote charge carrier separation,which is the most excellent conductivity of preserved metal cl...The linker defect engineering for MOFs is a viable strategy that usually can effectively augment conductivity to further promote charge carrier separation,which is the most excellent conductivity of preserved metal clusters.However,the partially missing photosensitive linker often leads to the diminished light utilization efficiency.As we know,in the linker defect engineering,addressing the lack of photosensitivity while maintaining outstanding conductivity is still in its infancy.In this essay,the linkerdefective NH_(2)-MIL-125 was obtained by adding the glacial acetic acid regulator,subsequently,the excellent light-responsive Pt/CQDs with up-conversion effect was in-situ encapsulated into the enlarged pore space of linker-defective NH_(2)-MIL-125.It is excited that the fabricated dual-functional composite ideally integrates photosensitivity and conductivity for photocatalytic hydrogen evolution and NO elimination.The optimal Pt/CQDs@NM-125-4 exhibited very superior photocatalytic hydrogen evolution(28.75mmol/g),it was 11.63 times as that of the initial NH_(2)-MIL-125(2.47 mmol/g)and 1.4 times as that of the defective NM-125-4(20.46 mmol/g).In addition,the excellent photocatalytic NO removal efficiency was 52.12%for Pt/CQDs@NM-125-4,whereas the original NH_(2)-MIL-125 only reached 30%and the defective NM-125-4 achieved 44.96%.The corresponding optical and electrical characterization based on UV-vis,up-conversion photoluminescence(UCPL),and electrochemical impedance spectroscopy(EIS)etc.demonstrated the defect engineering accelerates the charge carriers transfer via enhancing conductivity,and the in-situ confined up-conversion Pt/CQDs promote the visible light response.Our work presents a feasible avenue to integrate photosensitivity and conductivity via in-situ fabricating excellent lightresponsive Pt/CQDs within linker-defective NH_(2)-MIL-125 for further significantly boosting photocatalytic performance.展开更多
基金supported by the National Natural Science Foundation of China(Nos.22001026,22171233,22201193)Sichuan Science and Technology Program(No.2023NSFSC0109)+1 种基金the Fundamental Research Funds for the Central Universitiesthe Hundred Talent Program of Sichuan University(No.YJ2021158)。
文摘The linker defect engineering for MOFs is a viable strategy that usually can effectively augment conductivity to further promote charge carrier separation,which is the most excellent conductivity of preserved metal clusters.However,the partially missing photosensitive linker often leads to the diminished light utilization efficiency.As we know,in the linker defect engineering,addressing the lack of photosensitivity while maintaining outstanding conductivity is still in its infancy.In this essay,the linkerdefective NH_(2)-MIL-125 was obtained by adding the glacial acetic acid regulator,subsequently,the excellent light-responsive Pt/CQDs with up-conversion effect was in-situ encapsulated into the enlarged pore space of linker-defective NH_(2)-MIL-125.It is excited that the fabricated dual-functional composite ideally integrates photosensitivity and conductivity for photocatalytic hydrogen evolution and NO elimination.The optimal Pt/CQDs@NM-125-4 exhibited very superior photocatalytic hydrogen evolution(28.75mmol/g),it was 11.63 times as that of the initial NH_(2)-MIL-125(2.47 mmol/g)and 1.4 times as that of the defective NM-125-4(20.46 mmol/g).In addition,the excellent photocatalytic NO removal efficiency was 52.12%for Pt/CQDs@NM-125-4,whereas the original NH_(2)-MIL-125 only reached 30%and the defective NM-125-4 achieved 44.96%.The corresponding optical and electrical characterization based on UV-vis,up-conversion photoluminescence(UCPL),and electrochemical impedance spectroscopy(EIS)etc.demonstrated the defect engineering accelerates the charge carriers transfer via enhancing conductivity,and the in-situ confined up-conversion Pt/CQDs promote the visible light response.Our work presents a feasible avenue to integrate photosensitivity and conductivity via in-situ fabricating excellent lightresponsive Pt/CQDs within linker-defective NH_(2)-MIL-125 for further significantly boosting photocatalytic performance.