Recently, faculty and students from School of Materials Science and Engineering of Jiangsu University (JSU) published their latest research paper titled Improving Mass Transport and Charge Transfer in COF-Based Photocatalysts with Three-Dimensional Ordered Macropores for Benzylamine Oxidation and Hydrogen Evolution in Angewandte Chemie International Edition (Angew). JSU is the primary affiliation of the paper. Doctoral student Sun Lijuan from School of Materials Science and Engineering and Researcher Yan Weicheng from School of Chemistry and Chemical Engineering are the co-first authors. Prof. Liu Qinqin and Assoc. Prof. Zhou Yazhou from School of Materials Science and Engineering, Prof. Liang Guijie from Hubei University of Arts and Science, and Assoc. Prof. Silvio Osella from the Centre of New Technologies of University of Warsaw serve as the co-corresponding authors.

Covalent organic frameworks (COFs) are a promising class of photocatalysts. However, their densely packed microporous structures and poor pore connectivity hinder mass transport and charge separation/transfer, thereby limiting their efficiency. This work reports a one-step self-sacrificing template strategy for synthesizing three-dimensionally ordered macroporous COFs (3DOM-COFs). This approach exploits the kinetic match between template decomposition and Tp-Tta COF growth, achieving simultaneous Tp-Tta COF crystallization and polystyrene (PS) template degradation under solvothermal conditions. This confined growth mechanism yields highly ordered 3DOM macroporous structures, facilitating the uniform dispersion of ZnCdS nanoparticles and thereby forming a 3DOM-COF-based composite. The 3DOM structure enables 50 times faster mass transport of benzylamine compared to bulk COFs, while the heterojunction promotes directional charge separation and interfacial charge transfer. The composite exhibits exceptional performance in benzylamine oxidation, simultaneously producing N-benzylidenebenzylamine (selectivity: 99%) and hydrogen gas. This work provides novel insights for addressing pore-structure challenges in COFs.