{"title":"Dipole-Manipulated Built-In Electric Field Enables Ultrafast Charge Separation in Perylene Diimide Polymers for Photoelectrochemical Water Splitting.","authors":"Ying-Xin Qiao, Zicong Situ, Yi-Jing Chen, Shuo-Xiang Liu, Jing-Lan Zhang, Xingqing Li, Luo-Han Xie, Si-Hang Xie, Qing-Xiao Tong, Andong Xia, Zhuoran Kuang, Jing-Xin Jian","doi":"10.1002/advs.75610","DOIUrl":null,"url":null,"abstract":"<p><p>Molecular dipole engineering in dendrimeric perylene diimide (PDI) polymers creates powerful built-in electric fields (BIEFs) that dramatically enhance photoelectrochemical performance. By strategically tuning nitrogen content in aromatic linkers (pyridine, pyrimidine, and 1,3,5-triazine), the pyridine-linked C<sub>5</sub>N<sub>1</sub>-PDI achieves exceptional photocurrent density (68.7 µA cm<sup>-</sup> <sup>2</sup> at 1.23 V vs. RHE), outperforming its counterparts by 3.42-229 times. Ultrafast spectroscopy reveals this enhancement originates from sub-picosecond charge separation and efficient multi-electron accumulation, while theoretical modeling confirms the critical role of linker polarity in BIEF amplification. This work establishes a fundamental structure-kinetics relationship for designing high-performance organic photoelectrodes, providing a versatile strategy for advancing solar energy conversion technologies.</p>","PeriodicalId":117,"journal":{"name":"Advanced Science","volume":" ","pages":"e75610"},"PeriodicalIF":14.1000,"publicationDate":"2026-08-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC13336128/pdf/","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Advanced Science","FirstCategoryId":"88","ListUrlMain":"https://doi.org/10.1002/advs.75610","RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"2026/5/7 0:00:00","PubModel":"Epub","JCR":"Q1","JCRName":"CHEMISTRY, MULTIDISCIPLINARY","Score":null,"Total":0}
引用次数: 0
Abstract
Molecular dipole engineering in dendrimeric perylene diimide (PDI) polymers creates powerful built-in electric fields (BIEFs) that dramatically enhance photoelectrochemical performance. By strategically tuning nitrogen content in aromatic linkers (pyridine, pyrimidine, and 1,3,5-triazine), the pyridine-linked C5N1-PDI achieves exceptional photocurrent density (68.7 µA cm-2 at 1.23 V vs. RHE), outperforming its counterparts by 3.42-229 times. Ultrafast spectroscopy reveals this enhancement originates from sub-picosecond charge separation and efficient multi-electron accumulation, while theoretical modeling confirms the critical role of linker polarity in BIEF amplification. This work establishes a fundamental structure-kinetics relationship for designing high-performance organic photoelectrodes, providing a versatile strategy for advancing solar energy conversion technologies.
分子偶极子工程在枝状苝二酰亚胺（PDI）聚合物中产生强大的内置电场（BIEFs），显著提高了光电化学性能。通过调整芳香连接剂（吡啶，嘧啶和1,3,5-三嗪）中的氮含量，吡啶连接的C5N1-PDI获得了优异的光电流密度（在1.23 V vs. RHE下为68.7 μ A cm- 2），比同类产品高出3.42-229倍。超快光谱揭示了这种增强源于亚皮秒电荷分离和高效的多电子积累，而理论模型证实了连接器极性在BIEF放大中的关键作用。这项工作为设计高性能有机光电极建立了基本的结构-动力学关系，为推进太阳能转换技术提供了一种通用的策略。
期刊介绍：
Advanced Science is a prestigious open access journal that focuses on interdisciplinary research in materials science, physics, chemistry, medical and life sciences, and engineering. The journal aims to promote cutting-edge research by employing a rigorous and impartial review process. It is committed to presenting research articles with the highest quality production standards, ensuring maximum accessibility of top scientific findings. With its vibrant and innovative publication platform, Advanced Science seeks to revolutionize the dissemination and organization of scientific knowledge.
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