三苯胺
材料科学
氮化碳
光催化
异质结
共轭体系
光化学
接受者
电子受体
分子
聚合物
化学工程
电子供体
有机太阳能电池
氢
纳米技术
光电子学
有机化学
催化作用
化学
物理
工程类
复合材料
凝聚态物理
作者
Kui Li,Lei Wang,Zhongxin Chen,Xianfeng Yang,Yu‐Xiang Yu,Wei‐De Zhang,Ye Wang,Yumeng Shi,Kian Ping Loh,Qing‐Hua Xu
标识
DOI:10.1002/adfm.202005106
摘要
Abstract Efficient solar‐to‐hydrogen (STH) energy conversion under ambient conditions (room temperature and atmospheric pressure) is important for pursuing scalable solar hydrogen generation. Modification of polymeric carbon nitride (PCN) by conjugated polymers has attracted great attention for improving photocatalytic hydrogen evolution (PHE) performance. However, the limited interfacial junction between PCN and conjugated polymers leads to a low density of free charges, resulting in unsatisfactory PHE activity. Herein, three donor‐π‐acceptor‐structured organic molecules (OMs) with different electron‐donating units (amino, N,N ‐diethyl and triphenylamine) and same electron‐accepting unit (benzothiadiazole) are designed to modify PCN to enlarge the interfacial junction. The optimized PHE performance under AM 1.5G simulated sunlight and ambient conditions can maintain as high as 4.63 mmol h −1 g −1 (the highest record among all the reported PCN‐based photocatalysts to the best of the authors knowledge). The improved performance can be partially attributed to the strong visible light harvesting capability of OMs. Specifically, the triphenylamine unit in the formed type II molecule heterojunctions (MHJ) enables efficient charge separation at the interfacial junction, which prolongs the photogenerated electron lifetime for PHE. The designed MHJ photocatalysts show outstanding PHE performance under ambient conditions, which is highly promising for scalable STH conversion.
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