Dual Function of Naphthalenediimide Supramolecular Photocatalyst with Giant Internal Electric Field for Efficient Hydrogen and Oxygen Evolution

• Published in: Small (Weinheim an der Bergstrasse, Germany) Vol. 20; no. 32; pp. e2400344 - n/a
• Main Authors: Xu, Shicheng, Chen, Siqi, Li, Yuxin, Gao, Qiong, Luo, Xingjian, Li, Min, Ren, Lirong, Wang, Peng, Liu, Liping, Wang, Jun, Chen, Xianjie, Chen, Qian, Zhu, Yongfa
• Format: Journal Article
• Language: English
• Published: Germany Wiley Subscription Services, Inc 01.08.2024
• Subjects: Catalytic activity; Charge efficiency; Dipole moments; Electric fields; Hydrogen evolution; internal electric field; molecular dipole moment; Molecular structure; naphthalenediimide supramolecular; Oxygen; Photocatalysis; Photocatalysts; photocatalytic water splitting; Quantum efficiency; Self-assembly; short‐range ordered stacking structure; Water splitting; short-range ordered stacking structure; photocatalytic water splitting; internal electric field; molecular dipole moment; naphthalenediimide supramolecular
• ISSN: 1613-6810; 1613-6829; 1613-6829
• DOI: 10.1002/smll.202400344

Organic supramolecular photocatalysts have garnered widespread attention due to their adjustable structure and exceptional photocatalytic activity. Herein, a novel bis‐dicarboxyphenyl‐substituent naphthalenediimide self‐assembly supramolecular photocatalyst (SA‐NDI‐BCOOH) with efficient dual‐functional photocatalytic performance is successfully constructed. The large molecular dipole moment and short‐range ordered stacking structure of SA‐NDI‐BCOOH synergistically create a giant internal electric field (IEF), resulting in a remarkable 6.7‐fold increase in its charge separation efficiency. Additionally, the tetracarboxylic structure of SA‐NDI‐BCOOH greatly enhances its hydrophilicity. Thus, SA‐NDI‐BCOOH demonstrates efficient dual‐functional activity for photocatalytic hydrogen and oxygen evolution, with rates of 372.8 and 3.8 µmol h−1, respectively. Meanwhile, a notable apparent quantum efficiency of 10.86% at 400 nm for hydrogen evolution is achieved, prominently surpassing many reported supramolecular photocatalysts. More importantly, with the help of dual co‐catalysts, it exhibits photocatalytic overall water splitting activity with H2 and O2 evolution rates of 3.2 and 1.6 µmol h−1. Briefly, this work sheds light on enhancing the IEF by controlling the molecular polarity and stacking structure to dramatically improve the photocatalytic performance of supramolecular materials. The bis‐dicarboxyphenyl‐substituent naphthalenediimide self‐assembly supramolecular photocatalyst with a giant internal electric field is successfully constructed, which demonstrats efficient dual‐functional activity for photocatalytic hydrogen and oxygen evolution of 372.8 and 3.8 µmol h−1, with a notable apparent quantum efficiency of 10.86% at 400 nm, prominently surpassing many reported supramolecular photocatalysts.