Construction of planar-type defect-engineered metal–organic frameworks with both mixed-valence sites and copper-ion vacancies for photocatalysis

Yuan Guo; Chao Feng; Shixin Wang; Yuehong Xie; Changyan Guo; Ziran Liu; Naeem Akram; Yi Zhang; Yansong Zhao; Jide Wang

doi:10.1039/D0TA08085C

Construction of planar-type defect-engineered metal–organic frameworks with both mixed-valence sites and copper-ion vacancies for photocatalysis†

Yuan Guo,^a Chao Feng,^a Shixin Wang,^a Yuehong Xie,^a Changyan Guo,*^a Ziran Liu,^a Naeem Akram,

^a Yi Zhang,

^b Yansong Zhao^c and Jide Wang

*^a

Author affiliations

* Corresponding authors

^a Key Laboratory of Oil and Gas Fine Chemicals, College of Chemical Industry, Xinjiang University, Urumqi, China
E-mail: gcyslw@126.com, awangjd@sina.cn

^b Hunan Provincial Key Laboratory of Chemical Power Sources, College of Chemistry and Chemical Engineering, Central South University, Changsha, China

^c Department of Safety, Chemistry and Biomedical Laboratory Sciences, Faculty of Engineering and Science, Western Norway University of Applied Sciences, Inndalsveien28, 5063 Bergen, Norway

Abstract

This manuscript presents a facile paradigm for controllably developing planar-type defect-engineered metal–organic frameworks (DEMOFs) by systematically doping reductive defect linker vanillin (VAN) during the synthesis of HKUST-1. The as-prepared DEMOF variants were designed to carry copper-ion vacancies and mixed-valence Cu¹⁺/Cu²⁺ sites on the {220} and {111} planes of NR-HKUST-1 and {100}, {110} and {111} planes of NS-HKUST-1 via reversible and irreversible growth modes. The photocatalysis results indicate that the mixed-valence Cu¹⁺/Cu²⁺ sites (with special electronic properties) in planar-type defective HKUST-1 have a greater effect on performance improvement than copper-ion vacancies (with special steric properties). The HOMO–LUMO gap of the Cu¹⁺/Cu²⁺ unit is significantly reduced to promote the separation of photogenerated electron–hole pairs and overcome the transfer resistance of electron–hole pairs, leading to an outstanding catalytic activity (3784.2 μmol g⁻¹ h⁻¹). This strategy of creating mixed-valence sites and vacancies by doping a reductive defect linker can provide a new way to prepare catalysts with higher photocatalytic activity.

This article is part of the themed collection: Journal of Materials Chemistry A HOT Papers

Journal of Materials Chemistry A

Construction of planar-type defect-engineered metal–organic frameworks with both mixed-valence sites and copper-ion vacancies for photocatalysis†

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Construction of planar-type defect-engineered metal–organic frameworks with both mixed-valence sites and copper-ion vacancies for photocatalysis

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