4.8 Article

Copper-Bridged Tetrakis(4-ethynylphenyl)ethene Aggregates with Photo-Regulated 1O2 and O2.- Generation for Selective Photocatalytic Aerobic Oxidation

Journal

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
Volume 61, Issue 29, Pages -

Publisher

WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202202914

Keywords

Active Oxygen Radical Regulation; Aggregation-Induced Emission; Cu-Alkynyl; Photocatalysis Aerobic Oxidation; Photocatalyst Design

Funding

  1. National Key Basic Research Program of China [2020YFA0406101, 2020YFA0406104]
  2. National MCF Energy RD Program [2018YFE0306105]
  3. Innovative Research Group Project of the National Natural Science Foundation of China [51821002]
  4. National Natural Science Foundation of China [22171041, 22071020, 21771033, 21901035, 51725204, 21771132, 21471106, 51972216]
  5. Natural Science Foundation of Jilin Province Science and Technology Department (discipline layout project) [20190201206JC]
  6. China Postdoctoral Science Foundation [2018M631849]
  7. Fundamental Research Funds for the Central Universities [2412018BJ001, 2412018ZD007, 2412018QD005]
  8. Opening Project of Key Laboratory of Polyoxometalate Science of the Ministry of Education [130014556]
  9. Foundation of Jilin Educational Committee [JJKH20190268KJ]
  10. Collaborative Innovation Center of Suzhou Nano Science Technology
  11. Priority Academic Program Development of Jiangsu Higher Education Institutions (PAPD)
  12. 111 Project

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The Cu-I-bridged tetrakis(4-ethynylphenyl)ethene aggregates (T4EPE-Cu) demonstrated photo-regulated O-1(2) and O-2(.-) generation for selective photocatalytic aerobic oxidation, with Cu-alkynyl confirmed as the main oxygen activation site. The O-1(2) to O-2(.-) product ratios can be controlled in a range from 1.3 to 10.7, and T4EPE-Cu shows ultrahigh photocatalytic performance for Glaser coupling and benzylamine oxidation, with over 99 % conversion and selectivity.
Active species regulation is a key scientific issue that essentially determines the selectivity and activity of a photocatalyst. Herein, Cu-I-bridged tetrakis(4-ethynylphenyl)ethene aggregates (T4EPE-Cu) with photo-regulated O-1(2) and O-2(.-) generation were demonstrated for selective photocatalytic aerobic oxidation. In this system, transient photovoltage combined with the density functional theory calculations confirmed that Cu-alkynyl was the main oxygen activation site. The adsorbed O-2 tends to produce O-2(.-) because of the potential well effect of Cu-alkynyl under high-energy light excitation. But under low-energy light, O-2 tends to produce O-1(2) via resonance energy transfer with Cu-alkynyl. For alpha-terpinene oxidation, the ratios of O-1(2) products to O-2(.-) products can be controlled from 1.3 (380 nm) to 10.7 (600 nm). Furthermore, T4EPE-Cu exhibited ultrahigh photocatalytic performance for Glaser coupling and benzylamine oxidation, with a conversion and selectivity of over 99 %.

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