Wang Yuancheng, Liu Hui, Pan Qingyan, Ding Naixiu, Yang Chunming, Zhang Zhaohui, Jia Changchao, Li Zhibo, Liu Jian, Zhao Yingjie
College of Polymer Science and Engineering, Qingdao University of Science and Technology, Qingdao 266042, China.
Shanghai Synchrotron Radiation Facility, Shanghai Advanced Research Institute, Chinese Academy of Sciences, 239 Zhang Heng Road, Pudong New District, Shanghai 201204, China.
ACS Appl Mater Interfaces. 2020 Oct 14;12(41):46483-46489. doi: 10.1021/acsami.0c12173. Epub 2020 Oct 2.
The efficient conversion of CO to chemical fuels driven by solar energy is still a challenging research area in photosynthesis, in which the conversion efficiency greatly relies on photocatalytic coenzyme NADH regeneration. Herein, a photocatalyst/biocatalyst synergetic system based on a conjugated microporous polymer (CMP) was prepared for sustainable and highly selective photocatalytic reduction of CO to methanol. Two thiazolo[5,4-]thiazole-linked CMPs ( and ) were designed and synthesized as photocatalysts. Slight skeleton modification led to a great difference in their photocatalytic performance. Triazine-based exhibited an unprecedentedly high NADH regeneration efficiency of 82.0% yield within 5 min. Furthermore, the in situ photocatalytic NADH regeneration system could integrate with three consecutive enzymes for efficient conversion of CO into methanol. This CMP-enzyme hybrid system provides a new avenue for accomplishing the liquid sunshine from CO.
由太阳能驱动的将一氧化碳高效转化为化学燃料，在光合作用领域仍是一个具有挑战性的研究方向，其中转化效率很大程度上依赖于光催化辅酶NADH的再生。在此，制备了一种基于共轭微孔聚合物（CMP）的光催化剂/生物催化剂协同体系，用于将一氧化碳可持续且高选择性地光催化还原为甲醇。设计并合成了两种噻唑并[5,4-]噻二唑连接的CMP（和）作为光催化剂。轻微的骨架修饰导致它们的光催化性能有很大差异。基于三嗪的在5分钟内展现出前所未有的82.0%产率的高NADH再生效率。此外，原位光催化NADH再生系统可与三种连续的酶整合，以实现将一氧化碳高效转化为甲醇。这种CMP-酶杂化体系为实现由一氧化碳产生“液态阳光”提供了一条新途径。
