Triphenylene-Derived Polyimide Covalent Organic Frameworks for Efficient Photosynthesis of Hydrogen Peroxide

作者：Wei Zhao, Zhihua Li, Guanhua Ren, Jing Qi, Haiyang Huang, Qiang Zhu, Mounib Bahri, Yu-Lin Lu, Zekun Wang, He Li, Xiansong Shi, Binting Huang, Peiyao Yan, Chunqing Ji, Kexin Yu, Nigel D. Browning, Chaobin He, Haifeng Wang, Wei Zhang, Dan Zhao · 发表于：Journal of the American Chemical Society · 年份：2026 · DOI：10.1021/jacs.6c01900 · 被引用次数：2 · 研究领域：Covalent Organic Framework Applications、Advanced battery technologies research、Advanced Photocatalysis Techniques

Photocatalytic hydrogen peroxide (H 2 O 2 ) production offers a sustainable route for on-demand generation. Covalent organic frameworks (COFs) are attractive candidates, as their modular architectures can be engineered for optimal light capture and charge separation. However, their practical use has been hindered by the limited chemical stability of imine-linked COFs under prolonged operation. This challenge is further compounded by the narrow selection of building blocks suitable for efficient H 2 O 2 generation, restricting advancements in catalytic performance. Here, we present two polyimide-based COFs (NUS-76 and NUS-77) constructed with a newly designed fused-ring triphenylene building block, enabling efficient photocatalytic H 2 O 2 production. Utilizing a simple water-assisted microwave synthesis, both COFs exhibit remarkable robustness, retaining their crystalline structure even in strongly acidic and alkaline environments, outperforming the established imine-linked COF. Remarkably, NUS-77 integrates triphenylene and oligo(phenylenevinylene) moieties, delivering an impressive photocatalytic H 2 O 2 evolution rate up to 23,284 μmol g –1 h –1 . To further showcase their practical potential, we developed a continuous-flow photoreactor incorporating NUS-77, which produces 40.7 mM H 2 O 2 in 9 h and retains activity over four consecutive cycles (36 h) under 1 sun irradiation (P = 100 mW cm –2 ), a product concentration exceeding that of most reported COF photocatalysts. Th...