光催化
铜
镍
双稳态
六方晶系
化学
离子
催化作用
材料科学
结晶学
化学工程
冶金
有机化学
光电子学
工程类
作者
Xinxin Wang,Dongdong Xu,Yucheng Jin,Dongdong Qi,Hailong Wang,Yuesheng Han,Tianyu Wang,Jianzhuang Jiang
标识
DOI:10.1002/anie.202302808
摘要
Rational 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 (Cu3 Py3 ) 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 /CuII state nature of Cu3 Py3 in USTB-11(Cu,Ni) with a uniform bistable Cu34+ (CuI2 CuII ) : Cu35+ (CuI CuII2 ) (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 CO2 to CO performance with a conversion rate of 22 130 μmol g-1 h-1 and selectivity of 98 %.
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