Organic Photovoltaic Catalyst with Extended Exciton Diffusion for High-Performance Solar Hydrogen Evolution

Yufan Zhu; Zhenzhen Zhang; Wenqin Si; Qianlu Sun; Guilong Cai; Yawen Li; Yixiao Jia; Xinhui Lu; Weigao Xu; Shiming Zhang; Yuze Lin

doi:10.1021/jacs.2c03161

Organic Photovoltaic Catalyst with Extended Exciton Diffusion for High-Performance Solar Hydrogen Evolution

J Am Chem Soc. 2022 Jul 20;144(28):12747-12755. doi: 10.1021/jacs.2c03161. Epub 2022 Jul 11.

Authors

Yufan Zhu^{1

2}, Zhenzhen Zhang^{1

3}, Wenqin Si^{1

3}, Qianlu Sun⁴, Guilong Cai⁵, Yawen Li^{1

3}, Yixiao Jia^{1

2}, Xinhui Lu⁵, Weigao Xu⁴, Shiming Zhang², Yuze Lin^{1

3}

Affiliations

¹ Beijing National Laboratory for Molecular Sciences, CAS Key Laboratory of Organic Solids, Institute of Chemistry, Chinese Academy of Sciences, Beijing 100190, China.
² Key Laboratory of Flexible Electronics (KLOFE) & Institute of Advanced Materials (IAM), Jiangsu National Synergetic Innovation, Center for Advanced Materials (SICAM), Nanjing Tech University, Nanjing 211816, Jiangsu, China.
³ University of Chinese Academy of Sciences, Beijing 100049, China.
⁴ Key Laboratory of Mesoscopic Chemistry, School of Chemistry and Chemical Engineering, Nanjing University, Nanjing 210023, China.
⁵ Department of Physics, The Chinese University of Hong Kong, Hong Kong 999077, China.

PMID: 35815841
DOI: 10.1021/jacs.2c03161

Abstract

The short exciton diffusion length (L_D) associated with most classical organic photocatalysts (5-10 nm) imposes severe limits on photocatalytic hydrogen evolution efficiency. Here, a photovoltaic molecule (F1) without electron-deficient units at the central building block was designed and synthesized to improve the photoluminescence quantum yield (PLQY). With the enhanced PLQY of 9.3% and a large integral spectral overlap of 3.32 × 10¹⁶ nm⁴ M^-1 cm^-1, the average L_D of F1 film increases to 20 nm, nearly twice the length of the control photovoltaic molecule (Y6). Then, the single-component organic nanoparticles (SC-NPs) based on F1 show an optimized average hydrogen evolution rate (HER) of 152.60 mmol h^-1 g^-1 under AM 1.5G sunlight (100 mW cm^-2) illumination for 10 h, which is among the best results for photocatalytic hydrogen evolution.