Coordination engineering in single-atom covalent organic framework photocatalysts for solar-driven nitrogen fixation

作者：Weiguo Li, Helong Wu, Liangchun Wu, Yuan Hu, Yuansong Ye, Diwen Liu, Dejing Li, Yanjie Zhang, Zuju Ma, Rongjian Sa · 发表于：Physical Chemistry Chemical Physics · 年份：2026 · DOI：10.1039/d6cp00037a · 被引用次数：3 · 研究领域：Ammonia Synthesis and Nitrogen Reduction、Advanced Photocatalysis Techniques、Electrocatalysts for Energy Conversion

), achieving competitive values of -0.59 V, -0.42 V, and -0.76 V for Fe@NpdiCOF, Co@3NpdiCOF, and Ni@2NpdiCOF, respectively, while thermodynamically suppressing the competing hydrogen evolution reaction. Furthermore, this heteroatom doping strategy induces a synergistic optimization of photophysical properties, manifesting as a pronounced spectral blue shift and moderate band-gap narrowing to enhance visible-light harvesting. These insights establish ligand modulation as a robust design principle to concurrently optimize reaction energetics and optical properties for efficient solar-driven nitrogen fixation.