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Switching on the Photocatalysis of Metal–Organic Frameworks by Engineering Structural Defects

Xing MaHefei National Laboratory for Physical Sciences at the Microscale CAS Key Laboratory of Soft Matter Chemistry Collaborative Innovation Center of Suzhou Nano Science and Technology Department of Chemistry University of Science and Technology of China Hefei Anhui 230026 P. R. ChinaLi WangHefei National Laboratory for Physical Sciences at the Microscale Synergetic Innovation Center of Quantum Information and Quantum Physics Department of Chemical Physics University of Science and Technology of China Hefei Anhui 230026 P. R. ChinaQun ZhangHefei National Laboratory for Physical Sciences at the Microscale Synergetic Innovation Center of Quantum Information and Quantum Physics Department of Chemical Physics University of Science and Technology of China Hefei Anhui 230026 P. R. ChinaHai‐Long JiangHefei National Laboratory for Physical Sciences at the Microscale CAS Key Laboratory of Soft Matter Chemistry Collaborative Innovation Center of Suzhou Nano Science and Technology Department of Chemistry University of Science and Technology of China Hefei Anhui 230026 P. R. China
2019en
ABI

Аннотация

Abstract Defect engineering is a versatile approach to modulate band and electronic structures as well as materials performance. Herein, metal–organic frameworks (MOFs) featuring controlled structural defects, namely UiO‐66‐NH 2 ‐X (X represents the molar equivalents of the modulator, acetic acid, with respect to the linker in synthesis), were synthesized to systematically investigate the effect of structural defects on photocatalytic properties. Remarkably, structural defects in MOFs are able to switch on the photocatalysis. The photocatalytic H 2 production rate presents a volcano‐type trend with increasing structural defects, where Pt@UiO‐66‐NH 2 ‐100 exhibits the highest activity. Ultrafast transient absorption spectroscopy unveils that UiO‐66‐NH 2 ‐100 with moderate structural defects possesses the fastest relaxation kinetics and the highest charge separation efficiency, while excessive defects retard the relaxation and reduce charge separation efficiency.

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