Affiliation:
1. Beijing Advanced Innovation Center for Materials Genome Engineering Beijing Key Laboratory for Science and Application of Functional Molecular and Crystalline Materials Department of Chemistry and Chemical Engineering School of Chemistry and Biological Engineering University of Science and Technology Beijing Beijing 100083 China
Abstract
AbstractRational regulation of electronic structures and functionalities of framework materials still remains challenging. Herein, reaction of 4,4′,4′′‐nitrilo‐tribenzhydrazide with tris(μ2‐4‐carboxaldehyde‐pyrazolato‐N,N′)‐tricopper (Cu3Py3) generates the crystalline copper organic framework USTB‐11(Cu). Post‐modification with divalent nickel ions affords the heterometallic framework USTB‐11(Cu,Ni). Powder X‐ray diffraction and theoretical simulations reveal their two‐dimensional hexagonal structure geometry. A series of advanced spectroscopic techniques disclose the mixed CuI/CuIIstate nature of Cu3Py3in USTB‐11(Cu,Ni) with a uniform bistable Cu34+(CuI2CuII) : Cu35+(CuICuII2) (ca. 1 : 3) oxidation state, resulting in a significantly improved formation efficiency of the charge‐separation state. This endows the Ni sites with enhanced activity and USTB‐11(Cu,Ni) with outstanding photocatalytic CO2to CO performance with a conversion rate of 22 130 μmol g−1 h−1and selectivity of 98 %.
Funder
National Natural Science Foundation of China
Subject
General Chemistry,Catalysis
Cited by
13 articles.
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