光催化
四硫富瓦烯
共价键
共价有机骨架
固氮
化学
氮气
结晶度
化学工程
光化学
材料科学
纳米技术
有机化学
催化作用
复合材料
分子
工程类
作者
Yunchao Ma,Liaofang Shang,Jingyang Li,Yuanyuan Wu,Guangbo Che,Chunbo Liu,Qianrong Fang
标识
DOI:10.1016/j.cej.2024.149347
摘要
Preparing photocatalytic nitrogen-fixing catalysts that can effectively produce ammonia under mild conditions is an urgent problem to be solved. Herein, we for the first time present two three-dimensional tetrathiafulvalene-based covalent organic frameworks with high crystallinity and permanent pores, termed 3D-TTF-COFs, specifically designed for photocatalytic nitrogen fixation. The incorporation of TTF-based building blocks not only enhances light absorption capabilities but also facilitates the rapid transfer of photoexcited electrons, ensuring efficient charge carrier separation. It is worth noting that the resultant COFs exhibit remarkable NH3 generation rates of 313.8 ± 5.6 and 106.8 ± 4.2 μmol g−1h−1 under visible light irradiation, surpassing the performance of most photocatalyst materials reported so far. Furthermore, these COFs maintain structural integrity and excellent performance during cyclic testing. Additionally, we carried out density functional theory calculations to elucidate the reaction mechanism between N2 and NH3. This work provides a feasible strategy for constructing 3D COFs to achieve efficient photocatalytic nitrogen fixation.
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