Bao Hailian, Chen Xiaodi, Yuan Rui, Zhang Chao, Xu Shiai
School of Chemical Engineering, Qinghai University Xining 810016 Qinghai China
Shanghai Key Laboratory of Advanced Polymeric Materials, Key Laboratory for Ultrafine Materials of Ministry of Education, School of Materials Science and Engineering, East China University of Science and Technology Shanghai 200237 China
RSC Adv. 2021 Oct 5;11(52):32671-32679. doi: 10.1039/d1ra05527e. eCollection 2021 Oct 4.
A surface heterojunction catalyst of g-CN-PEDOT/P3HT with P3HT and PEDOT as the polymer sensitizer and hole transport pathway is successfully prepared. The as constructed g-CN-PEDOT/P3HT composite exhibits a photocatalyst H evolution rate up to 427703.3 μmol h g which is 1059 times higher than that of g-CN, 118 times higher than that of g-CN-PEDOT with ascorbic acid as sacrificial reagents. What's more, the g-CN-PEDOT/P3HT can even show an obviously enhanced photocatalytic H evolution rate which is 6.1 times higher than that of pure g-CN in pure water without any sacrificial reagent. Combining the experimental results and molecular dynamic (MD) simulation results, a possible mechanism can be drawn that the existed PEDOT possesses relatively higher hole mobility and can be used as a hole conductor between g-CN and P3HT. Then, the photogenerated holes migration can be accelerated by PEDOT from the VB of g-CN to the VB of P3HT. All those factors may benefit the synergy among g-CN, PEDOT and P3HT, which finally facilitates the rapid migration of photoinduced electron-hole pairs and eventually improves the photocatalytic H activity process of g-CN-PEDOT/P3HT with visible light. The present work may provide useful insights for designing a surface heterojunction composite photocatalyst with high photocatalytic activity for H production.
成功制备了一种以P3HT和PEDOT作为聚合物敏化剂及空穴传输通道的g-CN-PEDOT/P3HT表面异质结催化剂。所构建的g-CN-PEDOT/P3HT复合材料表现出的光催化析氢速率高达427703.3 μmol h g,比g-CN高1059倍,以抗坏血酸作为牺牲试剂时比g-CN-PEDOT高118倍。此外,在没有任何牺牲试剂的纯水中,g-CN-PEDOT/P3HT甚至能表现出明显增强的光催化析氢速率,比纯g-CN高6.1倍。结合实验结果和分子动力学(MD)模拟结果,可以得出一种可能的机制:存在的PEDOT具有相对较高的空穴迁移率,可作为g-CN和P3HT之间的空穴导体。然后,PEDOT可加速光生空穴从g-CN的价带迁移到P3HT的价带。所有这些因素可能有利于g-CN、PEDOT和P3HT之间的协同作用,最终促进光生电子 - 空穴对的快速迁移,并最终改善g-CN-PEDOT/P3HT在可见光下的光催化析氢活性过程。本工作可能为设计具有高光催化产氢活性的表面异质结复合光催化剂提供有用的见解。