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<p>Covalent organic frameworks (COFs) are promising for photocatalytic hydrogen peroxide (H<sub>2</sub>O<sub>2</sub>) production coupled with biomass valorization owing to their programmable architectures and tunable optoelectronic properties. Nevertheless, facile synthesis of COFs and achieving their high performance in economically photocatalytic co-production of H<sub>2</sub>O<sub>2</sub> and high-value-added chemicals remains challenging. Herein, by rationally regulating the functionality of organic building blocks, we fabricate two donor-acceptor (D-A) COFs with distinct topologies, including the fully condensed fc-Ph-COF via stoichiometric synthesis and the partially condensed pc-Ph-COF via sub-stoichiometric synthesis. Compared to fc-Ph-COF, pc-Ph-COF can be rapidly prepared under mild conditions and easily scaled up to a decagram-scale batch. Furthermore, the sub-stoichiometric pc-Ph-COF exhibits improved exciton dissociation and charge separation and migration. In pure water, pc-Ph-COF achieves a 3.3-fold higher H<sub>2</sub>O<sub>2</sub> production rate than fc-Ph-COF within the batch reactor. Moreover, we established a biphasic flow system to demonstrate more efficient H<sub>2</sub>O<sub>2</sub> production coupled with the dehydrogenation of 1,2,3,4-tetrahydroisoquinoline (THIQ) to value-added 3,4-dihydroisoquinoline (DHIQ). Under optimized conditions, an exceptional H<sub>2</sub>O<sub>2</sub> production rate of 25.33 mmol g<sup>−1</sup> h<sup>−1</sup> is achieved over pc-Ph-COF within the flow reactor, along with high conversion of THIQ to DHIQ (selectivity: ∼96%). A techno-economic analysis (TEA) showcases the facile synthesis of high-performance photocatalysts towards economical and sustainable H<sub>2</sub>O<sub>2</sub> production coupled with biomass valorization.</p>

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Topology-induced facile synthesis of donor-acceptor covalent organic frameworks for economically photocatalytic co-production of H2O2 and 3,4-dihydroisoquinoline in a flow system

  • 期刊论文

  • 发表日期：

    2026年4月1日

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  • Chaochen Shao,
  • Haocheng Xu,
  • Yongpan Hu,
  • Xiaolin Jiang,
  • Xingchao Ma,
  • Yang Xu,
  • Jingyu Wang,
  • Qiaobo Liao,
  • Kai Xi

摘要

Covalent organic frameworks (COFs) are promising for photocatalytic hydrogen peroxide (H2O2) production coupled with biomass valorization owing to their programmable architectures and tunable optoelectronic properties. Nevertheless, facile synthesis of COFs and achieving their high performance in economically photocatalytic co-production of H2O2 and high-value-added chemicals remains challenging. Herein, by rationally regulating the functionality of organic building blocks, we fabricate two donor-acceptor (D-A) COFs with distinct topologies, including the fully condensed fc-Ph-COF via stoichiometric synthesis and the partially condensed pc-Ph-COF via sub-stoichiometric synthesis. Compared to fc-Ph-COF, pc-Ph-COF can be rapidly prepared under mild conditions and easily scaled up to a decagram-scale batch. Furthermore, the sub-stoichiometric pc-Ph-COF exhibits improved exciton dissociation and charge separation and migration. In pure water, pc-Ph-COF achieves a 3.3-fold higher H2O2 production rate than fc-Ph-COF within the batch reactor. Moreover, we established a biphasic flow system to demonstrate more efficient H2O2 production coupled with the dehydrogenation of 1,2,3,4-tetrahydroisoquinoline (THIQ) to value-added 3,4-dihydroisoquinoline (DHIQ). Under optimized conditions, an exceptional H2O2 production rate of 25.33 mmol g−1 h−1 is achieved over pc-Ph-COF within the flow reactor, along with high conversion of THIQ to DHIQ (selectivity: ∼96%). A techno-economic analysis (TEA) showcases the facile synthesis of high-performance photocatalysts towards economical and sustainable H2O2 production coupled with biomass valorization.