文献类型：期刊文献

英文题名：Rational Design of Methylated Triazine-Based Linear Conjugated Polymers for Efficient CO2 Photoreduction with Water

作者：Zhu, Xiang[1];Yang, Na[1];Zhou, Li-An[2];Tian, Chengcheng[2];Wu, Jiwei[1];Wang, Tao[3];Li, Xiaodong[4];Jiang, Xia[1];Dai, Sheng[3]

机构：[1]Sichuan Univ, Sch Carbon Neutral Future Technol, Chengdu 610065, Peoples R China;[2]East China Univ Sci & Technol, Sch Resources & Environm Engn, Shanghai 200237, Peoples R China;[3]Oak Ridge Natl Lab, Chem Sci Div, Oak Ridge, TN 37831 USA;[4]Max Planck Inst Microstruct Phys, Weinberg 2, D-06120 Halle, Germany

年份：2025

卷号：37

期号：14

外文期刊名：ADVANCED MATERIALS

收录：;EI(收录号：20250717859994);WOS:【SCI-EXPANDED(收录号:WOS:001420786400001)】；

基金：X.Z. and N.Y. contributed equally to this work. X.Z. thanks the financial support from "the Fundamental Research Funds for the Central Universities", Sichuan Science and Technology Program (2025YFHZ0177) and the National Natural Science Foundation of China (22078349 and 22005319). C.T. was supported by the Shanghai Science and Technology Innovation Plan (22DZ1208600), the Innovation Program of Shanghai Municipal Education Commission (2023ZKZD41), and the National Natural Science Foundation of China (52170109). S.D. and T.W. were supported by the Division of Chemical Sciences, Geosciences, and Biosciences, Office of Basic Energy Sciences, US Department of Energy. The Supercomputing Center of Max Planck Computing & Data Facility (MPCDF) is acknowledged for computational support. The authors thank Dr. Wenkai Yan and prof. Yingpu Bi for help of photoelectrochemical measurements.

语种：英文

外文关键词：CO2 photoreduction; H2O photo-oxidation; linear conjugated polymers; methylated triazine linkages; molecular junctions engineerings

摘要：The development of semiconducting conjugated polymers for photoredox catalysis holds great promise for sustainable utilization of solar energy. Herein a new family of porous methylated triazine-based linear conjugated polymers is reported that enable efficient photoreduction of carbon dioxide (CO2) with water (H2O) vapor, in the absence of any additional photosensitizer, sacrificial agents or cocatalysts. It is demonstrated that the key lies in the generation of methylated triazine linkages through a facile condensation reaction between benzamidine and acetic anhydride, which impedes the formation of conventional triazine-based frameworks. It is also shown that regulating conjugated linear backbones with different lengths of electron-donated benzyl units provides a facile means to modulate their optical properties and the exciton dissociation, thereby affording more long-lived photogenerated charge carriers and boosting charge separation and transfer. A high-performance carbon monoxide (CO) production rate of 218.9 mu mol g(-1) h(-1) is achieved with approximate to 100% CO selectivity, which is accompanied by exceptional H2O oxidation to oxygen (O-2). It anticipates this new study will advance synthetic approaches toward polymeric semiconductors and facilitate new possibilities for triazine-based conjugated polymers with promising potential in artificial photocatalysis.