文献类型：期刊文献

英文题名：Molecular Engineering of Donor-Acceptor Conjugated Polymer/g-C3N4 Heterostructures for Significantly Enhanced Hydrogen Evolution Under Visible-Light Irradiation

作者：Yu, Fengtao[1];Wang, Zhiqiang[2,3];Zhang, Shicong[1];Ye, Haonan[1];Kong, Kangyi[1];Gong, Xueqing[2,3];Hua, Jianli[1];Tian, He[1]

机构：[1]East China Univ Sci & Technol, Sch Chem & Mol Engn, Inst Fine Chem, Key Lab Adv Mat, 130 Meilong Rd, Shanghai 200237, Peoples R China;[2]East China Univ Sci & Technol, Ctr Computat Chem, 130 Meilong Rd, Shanghai 200237, Peoples R China;[3]East China Univ Sci & Technol, Res Inst Ind Catalysis, Sch Chem & Mol Engn, 130 Meilong Rd, Shanghai 200237, Peoples R China

年份：2018

卷号：28

期号：47

外文期刊名：ADVANCED FUNCTIONAL MATERIALS

收录：;EI(收录号：20184205949808);WOS:【SCI-EXPANDED(收录号:WOS:000450371400020)】；

基金：F.Y. and Z.W. contributed equally to this work. This work was supported by the National Nature Science Foundation of China (21421004, 21772040, 21572062, 21573067, and 21372082), the Fundamental Research Funds for the Central Universities (222201717003), and the Programme of Introducing Talents of Discipline to Universities (B16017).

语种：英文

外文关键词：donor-acceptor conjugated polymer; g-C3N4; hydrogen evolution; molecular engineering; Type II heterojunction

摘要：Polymer heterojunctions (PHJs) have emerged as promising photocatalysts for the photocatalytic hydrogen evolution (PHE). Nevertheless, most PHJs exhibit unsatisfactory hydrogen evolution rate (HER), primarily attributing to their own high-energy Frenkel excitons and poor light capturing ability. In this paper, a molecular engineering strategy is developed to further broaden spectral response range and simultaneously accelerate Frenkel excitons dissociation within PHJs. For this purpose, three donor-acceptor (D-A) conjugated polymers/g-C3N4 heterojunctions with alternative donor units (fluorene, carbazole, N-annulated perylene for P1, P2, and P3, respectively) and the invariant acceptor unit (benzothiadiazole) have been designed and fabricated for efficient PHE. Experimental results show that copolymerizing different donor units into the polymer skeleton not only extends the visible-light response range but also promotes photoexciton separation within polymer/g-C3N4 PHJs. Notably, copolymerizing the strongest electron donor unit (N-annulated perylene) achieves the best light capture ability and the most effective photoexcitation separation of the P3/g-C3N4, leading to significantly increase HRE of 13.0 mmol h(-1) g(-1) with a recorded apparent quantum yield of 27.32% at 520 nm. Importantly, the Type II heterojunction mechanism within P3/CN was first proved by theoretical calculation. This work provides a promising strategy for reasonably developing efficient PHJs for solar fuel production.