Ternary supramolecular system for photocatalytic oxidation with air by consecutive photo-induced electron transfer processes

被引:71
作者
He, Jiachen [1 ]
Han, Qiuxia [1 ]
Li, Jie [1 ]
Shi, Zhuolin [1 ]
Shi, Xiaoyun [1 ]
Niu, Jingyang [1 ]
机构
[1] Henan Univ, Coll Chem & Chem Engn, Inst Mol & Crystal Engn, Henan Key Lab Polyoxometalate Chem, Kaifeng 475004, Henan, Peoples R China
基金
中国国家自然科学基金;
关键词
Polyoxometalate; Metal-organic framework; Photocatalysis; Ammoxidation; Epoxidation; METAL-ORGANIC FRAMEWORKS; VISIBLE-LIGHT PHOTOCATALYST; SELECTIVE OXIDATION; NAPHTHALENE DIIMIDES; AEROBIC OXIDATION; ARYL HALIDES; POLYOXOMETALATE; EFFICIENT; PHOTOREDOX; CHARGE;
D O I
10.1016/j.jcat.2019.06.040
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
Developing new photocatalysts for settling the tightest bottlenecks that lower efficiency, inferior selectivity and harsh conditions in organic oxidation reactions with air is very significant. Herein, ZnW-DPNDI-PYI was achieved by assembling a functional photosensitizer, an oxidation catalyst [BW(12)O40](5-), and an organocatalyst into one single framework. The anion center dot center dot center dot pi and N-H center dot center dot center dot O hydrogen bonds interactions facilitate the consecutive photo-induced electron transfer (conPET) process for the photocatalytic oxidation by stabilizing the radical-anion intermediate and catalyst-substrate interacted moiety. Besides, N,N'-bis(4-pyridylmethyl)naphthalene diimide (DPNDI) can be excited by visible light, the photogenerated electron and hole would further activate oxygen and substrates, respectively, to give the corresponding redox products. High conversion and selectivity of ZnW-DPNDI-PYI in photocatalytic coupling of primary amines and olefins epoxidation with air under visible-light have been demonstrated. (C) 2019 Elsevier Inc. All rights reserved.
引用
收藏
页码:161 / 167
页数:7
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