Azine-based covalent organic frameworks as metal-free visible light photocatalysts for CO2 reduction with H2O
Azine-based covalent organic frameworks as metal-free visible light photocatalysts for CO2 reduction with H2O
复制标题
基于吖嗪的共价有机骨架作为无金属可见光光催化剂用于用水还原二氧化碳
DOI：
10.1016/j.apcatb.2018.08.004
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发表时间：
2018-12-30
影响因子：
22.1
通讯作者：
Zhu, Weidong
中科院分区：
文献类型：
--
作者：
Fu, Yanghe;Zhu, Xiaoli;Zhu, Weidong
利用太阳能将二氧化碳转化为有价值的有机产品是解决全球变暖和能源短缺的最佳方案之一。由于共价键的存在，共价有机骨架（COFs）具有上级的热稳定性和化学稳定性，此外，基于连氮的COFs作为一类新型光活性材料，可以将CO2捕获和多相催化转化CO2的优点联合收割机结合起来。在这里，第一次使用两种基于连氮的COF作为光催化剂，在可见光照射下催化CO2与H2O反应生成甲醇，而不需要任何牺牲剂。此外，这些基于连氮的COF在用H2O光催化还原CO2方面比g-C3 N4和其他报道的与无机半导体偶联的光催化剂更活跃。各种技术被用来表征合成的连氮基COFs结合分子模拟，以阐明两个连氮基COFs之间的CO2光催化还原的差异研究。研究结果表明，基于连氮基的COFs是一种理想的无金属有机半导体材料，其组成、结构和性能可调，有望成为新型柔性光催化剂，用于CO2的还原。此外，本研究将促进COFs基光催化剂和其他新型光催化剂作为能量转换器的研究和开发。
The conversion of CO2 into valuable organic products by means of solar energy is one of the best solutions to both global warming and energy shortage. Covalent organic frameworks (COFs) show a superior thermal and chemical stability due to their covalent bonds, besides, azine-based COFs, an interesting new class of photoactive materials, can combine advantages in CO2 capture and heterogeneous photocatalysis for the conversion of CO2. Here, for the first time two azine-based COFs were used as photocatalysts that catalyzed the reaction of CO2 with H2O into methanol under visible-light irradiation without any sacrificial agents. In addition, these azine-based COFs were more active in the photocatalytic reduction of CO2 with H2O than g-C3N4 and other reported photocatalysts coupling with inorganic semiconductors. Various techniques were used to characterize the synthesized azine-based COFs in combination with molecular simulation to elucidate the differences in the photo catalytic reduction of CO2 between the two azine-based COFs investigated. The current work indicates that azine-based COFs would be ideal metal-free organic semiconductors, which might be developed into new flexible photocatalysts for CO2 reduction due to their tunable composition, structure, and property. Furthermore, the present study would stimulate research and development in COFs-based photocatalysts and other new photo catalysts as energy transducers.