光催化
材料科学
异质结
偶极子
羧酸盐
化学工程
半导体
化学物理
光化学
纳米技术
催化作用
光电子学
化学
有机化学
工程类
作者
Huaming Sun,Jianan Fan,Rong Fan,Po Sun,Shifan Wang,Danfeng Wang,Peiyang Gu,Wenyi Tan,Yongfa Zhu
出处
期刊:Angewandte Chemie
[Wiley]
日期:2025-04-24
卷期号:64 (27): e202503792-e202503792
被引量:9
标识
DOI:10.1002/anie.202503792
摘要
Achieving ultrafast dissociation of photogenerated excitons and efficient charge transport within the photocatalyst is a fundamental issue. Additionally, enhancing the interaction between semiconductors and water is crucial for efficient photocatalytic water splitting. Herein, we synthesized a carboxylate-based hydrophilic polymer, hPTB7-Th. Exposed carboxylates enhance semiconductor-water interfacial compatibility, reducing contact resistance and accelerating charge transfer kinetics. Furthermore, the carboxylate substitution shifts polarity centers, amplifying the molecular dipole moment by 10-fold. This induces a giant built-in electric field, enabling ultrafast electron-transfer process (ca. 0.31 ps) in the hPTB7-Th:PCBM bulk heterojunction. Consequently, the hPTB7-Th:PCBM-based bulk heterojunction nanoparticles exhibit excellent photocatalytic activity, achieving an optimal hydrogen evolution rate of 111.5 mmol g-1 h-1, four times over the ester-based counterpart (PTB7-Th:PCBM). Moreover, the electrostatic stability imparted by the carboxylates endows hPTB7-Th:PCBM with outstanding operational stability, maintaining 81% of its initial hydrogen evolution rate after 100 h operation. This result places it among the state-of-the-art organic photovoltaic bulk heterojunction photocatalysts in terms of stability. This work establishes a molecular engineering strategy for high-performance bulk heterojunction photocatalysts, emphasizing synergistic optimization of hydrophilicity, dipole engineering, and interfacial dynamics.
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