Photocatalysis

ARTICLE pubs.acs.org/JACS Doping MetalÀ native Frameworks for Water Oxidation, Carbon Dioxide Reduction, and original Photocatalysis Cheng Wang, Zhigang Xie, Kathryn E. deKra?t, and Wenbin Lin* Department of Chemistry, CB #3290, University of North Carolina, Chapel Hill, North Carolina 27599, United States S b Supporting Information ABSTRACT: Catalytically workmanlike Ir, Re, and Ru complexes H2L1À H2L6 with dicarboxylic acid functionalities were incorporated into a highly electrostatic and porous Zr6O4(OH)4(bpdc)6 (UiO-67, bpdc = para-biphenyldicarboxylic acid) framework using a mix-and-match synthetic strategy. The twin(a) ligand lengths between bpdc and L1ÀL6 ligands allowed the construction of highly crystalline UiO-67 frameworks (metalÀorganic frameworks (MOFs) 1À6) that were doped with L1ÀL6 ligands. MOFs 1À6 were isostructural to the p arent UiO-67 framework as shown by powder X-ray di?raction (PXRD) and exhibited high surface areas ranging from 1092 to 149 7 m2/g. MOFs 1À6 were stable in air up to quaternary hundred °C and active catalysts in a hold of reactions that are relevant to solar energy utilization.

MOFs 1À3 containing [Cp*IrIII(dcppy)Cl] (H2L1), [Cp*IrIII(dcbpy)Cl]Cl (H2L2), and [IrIII(dcppy)2(H2O)2]OTf (H2L3) (where Cp* is pentamethylcyclopentadienyl, dcppy is 2-phenylpyridine-5,40 -dicarboxylic acid, and dcbpy is 2,20 -bipyridine-5,50 -dicarboxylic acid) were e?ective water oxidation catalysts (WOCs), with turnover frequencies (TOFs) of up to 4.8 hÀ1. The [ReI(CO)3(dcbpy)Cl] (H2L4) derivatized MOF 4 served as an active catalyst for photocatalytic CO2 step-down with a total turnover number (TON! ) of 10.9, three times high than that of the homogeneous complex H2L4. MOFs 5 and 6 contained phosphorescent [IrIII(ppy)2(dcbpy)]Cl (H2L5) and [RuII(bpy)2(dcbpy)]Cl2 (H2L6) (where ppy is 2-phenylpyridine and bpy is 2,20 -bipyridine) and were employ in three photocatalytic organic transformations (aza-Henry reaction, aerobiotic aminoalkane coupling, and aerobic oxidation of...If you want to get a exuberant essay, show it on our website: OrderCustomPaper.com

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