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author:

Liu, J. (Liu, J..) [1] | Tuo, C. (Tuo, C..) [2] | Xiao, W.-Y. (Xiao, W.-Y..) [3] | Qi, M.-Y. (Qi, M.-Y..) [4] | Yusran, Y. (Yusran, Y..) [5] | Wang, Z. (Wang, Z..) [6] | Li, H. (Li, H..) [7] | Guo, C. (Guo, C..) [8] | Song, J. (Song, J..) [9] | Qiu, S. (Qiu, S..) [10] | Xu, Y.-J. (Xu, Y.-J..) [11] | Fang, Q. (Fang, Q..) [12]

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Scopus

Abstract:

The development of photocatalytic systems that enable the simultaneous production of H2O2 and value-added organic chemicals presents a dual advantage: generating valuable products while maximizing the utilization of solar energy. Despite the potential, there are relatively few reports on photocatalysts capable of such dual functions. In this study, we synthesized a series of donor-acceptor covalent organic frameworks (COFs), designated as JUC-675 to JUC-677, to explore their photocatalytic efficiency in the co-production of H2O2 and N-benzylbenzaldimine (BBAD). Among them, JUC-675 exhibited exceptional performance, achieving a H2O2 production rate of 22.8 mmol g−1 h−1 with an apparent quantum yield of 15.7 %, and its solar-to-chemical conversion efficiency was calculated to be 1.09 %, marking it as the most effective COF-based photocatalyst reported to date. Additionally, JUC-675 demonstrated a high selectivity (99.9 %) and yield (96 %) for BBAD in the oxidative coupling of benzylamine. The underlying reaction mechanism was thoroughly investigated through validation experiments and density functional theory (DFT) calculations. This work represents a significant advancement in the design of COF-based photocatalysts and the development of efficient dual-function photocatalytic platforms, offering new insights and methodologies for enhanced solar energy utilization and the synthesis of value-added products. © 2024 Wiley-VCH GmbH.

Keyword:

co-production systems covalent organic frameworks H2O2 production oxidative organic transformations photocatalytic

Community:

  • [ 1 ] [Liu J.]State Key Laboratory of Inorganic Synthesis and Preparative Chemistry, Department of Chemistry, Jilin University, Changchun, 130012, China
  • [ 2 ] [Tuo C.]School of Life Sciences, Zhuhai College of Science and Technology, Zhuhai, 519040, China
  • [ 3 ] [Xiao W.-Y.]State Key Laboratory of Photocatalysis on Energy and Environment, College of Chemistry, Fuzhou University, Fuzhou, 350116, China
  • [ 4 ] [Qi M.-Y.]Institute of Fundamental and Frontier Sciences, University of Electronic Science and Technology of China, Chengdu, 611731, China
  • [ 5 ] [Yusran Y.]State Key Laboratory of Inorganic Synthesis and Preparative Chemistry, Department of Chemistry, Jilin University, Changchun, 130012, China
  • [ 6 ] [Wang Z.]State Key Laboratory of Inorganic Synthesis and Preparative Chemistry, Department of Chemistry, Jilin University, Changchun, 130012, China
  • [ 7 ] [Li H.]State Key Laboratory of Inorganic Synthesis and Preparative Chemistry, Department of Chemistry, Jilin University, Changchun, 130012, China
  • [ 8 ] [Guo C.]State Key Laboratory of Inorganic Synthesis and Preparative Chemistry, Department of Chemistry, Jilin University, Changchun, 130012, China
  • [ 9 ] [Song J.]School of Life Sciences, Zhuhai College of Science and Technology, Zhuhai, 519040, China
  • [ 10 ] [Qiu S.]State Key Laboratory of Inorganic Synthesis and Preparative Chemistry, Department of Chemistry, Jilin University, Changchun, 130012, China
  • [ 11 ] [Xu Y.-J.]State Key Laboratory of Photocatalysis on Energy and Environment, College of Chemistry, Fuzhou University, Fuzhou, 350116, China
  • [ 12 ] [Fang Q.]State Key Laboratory of Inorganic Synthesis and Preparative Chemistry, Department of Chemistry, Jilin University, Changchun, 130012, China

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Source :

Angewandte Chemie - International Edition

ISSN: 1433-7851

Year: 2025

Issue: 9

Volume: 64

1 6 . 1 0 0

JCR@2023

Cited Count:

WoS CC Cited Count:

SCOPUS Cited Count: 6

ESI Highly Cited Papers on the List: 0 Unfold All

WanFang Cited Count:

Chinese Cited Count:

30 Days PV: 0

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