Chen Jinqing, Zhong Hong, Lv Haowei, Liu Ruixia, Wang Ruihu
State Key Laboratory of Structural Chemistry, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, 350007, Fuzhou, P. R. China.
University of Chinese Academy of Sciences, Beijing, 100049, P. R. China.
ChemSusChem. 2021 Jul 6;14(13):2749-2756. doi: 10.1002/cssc.202100772. Epub 2021 May 26.
Photocatalytic CO reduction offers a promising approach for managing global carbon balance. The smooth delivery of the photoexcited electrons to the active sites without the extra photosensitizers is still challenging. Herein, a series of donor-π-acceptor conjugated organic polymers (COPs) were produced using anthracene, cobalt-coordinated bipyridyl, and benzene as donor, acceptor, and π linker units, respectively. The introduction of phenyl linker significantly improved the activities of photocatalytic CO reduction upon visible light illumination. Structure-performance relationship examinations uncovered that donor-π-acceptor structure promotes mobility of charge carriers and utilization efficiency on the catalytically active sites, resulting in high photocatalytic activity and durability for CO photoreduction. The in-depth insights into the electron transport processes open new perspectives for further optimization and rational design of photoactive polymers with high efficiency for solar-energy conversion.
光催化一氧化碳还原为管理全球碳平衡提供了一种很有前景的方法。在没有额外光敏剂的情况下将光激发电子顺利输送到活性位点仍然具有挑战性。在此，使用蒽、钴配位联吡啶和苯分别作为供体、受体和π连接单元制备了一系列供体-π-受体共轭有机聚合物（COP）。苯基连接基的引入显著提高了可见光照射下光催化一氧化碳还原的活性。结构-性能关系研究发现，供体-π-受体结构促进了电荷载流子的迁移率和催化活性位点上的利用效率，从而导致高光催化活性和一氧化碳光还原的耐久性。对电子传输过程的深入洞察为进一步优化和合理设计高效太阳能转换光活性聚合物开辟了新的前景。
