Organic dyes with multi-branched structures for highly efficient photocatalytic hydrogen evolution under visible-light irradiation

光催化 分子内力 光化学 材料科学 偶极子 辐照 光催化分解水 可见光谱 载流子 氮化碳 分解水 化学工程 化学 纳米技术 光电子学 催化作用 有机化学 物理 核物理学 工程类
作者
Siwei Liu,Peixuan Lin,Meng Wu,Zhi‐An Lan,Hangyu Zhuzhang,Mengmeng Han,Yunhao Fan,Xiong Chen,Wei Wang,Qianqian Li,Zhen Li
出处
期刊:Applied Catalysis B-environmental [Elsevier BV]
卷期号:309: 121257-121257 被引量:12
标识
DOI:10.1016/j.apcatb.2022.121257
摘要

Direct photocatalytic water splitting is an attractive strategy for clean energy, in which, organic photocatalytic systems with broad light-harvesting region and efficient charge separation are highly desired and still challenging. In this paper, three multi-branched organic dyes were designed and synthesized with dipolar, V-shaped, and octupolar geometries, respectively. The multiple intramolecular charge transfer processes by electronic pull-push effect along the branches can provide more channels for light-harvesting and carrier transporting. Also, the interactions with polymeric carbon nitride (PCN) can be optimized by multiple anchoring units and defect filling effect, resulting in the gradually enhanced photocatalytic hydrogen evolution performance with the increased number of branches. Accordingly, the highest one of 996.9 μmol h −1 was achieved, which is over 40-folders that of PCN/Pt (24.8 μmol h −1 ) under the same conditions. It provides an efficient strategy for molecular design of organic dyes as photocatalyst, promoting development of PHE system from the molecular level. Organic dyes with different branched structures, as dipolar, V-shaped and octupolar configurations, were applied to PCN surface as photocatalyst, with the aim to promote photocatalytic hydrogen evolution (PHE). Accordingly, PHE rates enhanced with increased number of branches, and the highest one of 996.9 μmol h −1 was achieved by octupolar dye, which was over 40-folders that of PCN/Pt (24.8 μmol h −1 ). It indicated the superiority of branched structure, which is mainly related to the stronger light-harvesting ability and optimized interactions between dye and PCN with multiple anchoring units. • Organic dyes with multi-branched structure can promote photocatalytic hydrogen evolution by optimized interactions. • The highest PHE rate reach to 996.9 μmol h −1 , and AQY efficiency of 12.5% at 490 nm. • The charge transfer processes were investigated systematically by varied emission properties under different conditions.
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