Constructing Donor-Acceptor Covalent Organic Frameworks for Highly Efficient H2O2 Photosynthesis Coupled with Oxidative Organic Transformations.

Autor: Liu JC; Jilin University, Chemistry, CHINA., Tuo C; Zhuhai College of Science and Technology, Life Science, CHINA., Xiao WY; Fuzhou University, Chemistry, CHINA., Qi MY; University of Electronic Science and Technology of China, Fundamental and Frontier Sciences, CHINA., Yusran Y; Jilin University, Chemistry, CHINA., Wang ZT; Jilin University, Chemistry, CHINA., Li H; Jilin University, Chemistry, CHINA., Guo CS; Jilin University, Chemistry, CHINA., Song JL; Zhuhai College of Science and Technology, Life Science, CHINA., Qiu SL; Jilin University, Chemistry, CHINA., Xu YJ; Fuzhou University, Chemistry, CHINA., Fang Q; Jilin University, Department of Chemistry, 2699 Qianjin Street, 130012, Changchun, CHINA.
Jazyk: angličtina
Zdroj: Angewandte Chemie (International ed. in English) [Angew Chem Int Ed Engl] 2024 Sep 19, pp. e202416240. Date of Electronic Publication: 2024 Sep 19.
DOI: 10.1002/anie.202416240
Abstrakt: 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.)
Databáze: MEDLINE
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