Overcoming small-bandgap charge recombination in visible and NIR-light-driven hydrogen evolution by engineering the polymer photocatalyst structure

Mohamed Hammad Elsayed, Mohamed Abdellah, Ahmed Zaki Alhakemy, Islam M. A. Mekhemer, Ahmed Esmail A. Aboubakr, Bo-Han Chen, Amr Sabbah, Kun-Han Lin, Wen-Sheng Chiu, Sheng-Jie Lin, Che-Yi Chu, Chih-Hsuan Lu, Shang-Da Yang, Mohamed Gamal Mohamed, Shiao-Wei Kuo, Chen-Hsiung Hung, Li-Chyong Chen, Kuei-Hsien Chen and Ho-Hsiu Chou ()
Additional contact information
Mohamed Hammad Elsayed: Al-Azhar University
Mohamed Abdellah: United Arab Emirates University
Ahmed Zaki Alhakemy: Al-Azhar University
Islam M. A. Mekhemer: National Tsing Hua University
Ahmed Esmail A. Aboubakr: Taiwan International Graduate Program
Bo-Han Chen: National Tsing Hua University
Amr Sabbah: National Taiwan University
Kun-Han Lin: National Tsing Hua University
Wen-Sheng Chiu: National Chung Hsing University
Sheng-Jie Lin: National Chung Hsing University
Che-Yi Chu: National Chung Hsing University
Chih-Hsuan Lu: National Tsing Hua University
Shang-Da Yang: National Tsing Hua University
Mohamed Gamal Mohamed: National Sun Yat-Sen University
Shiao-Wei Kuo: National Sun Yat-Sen University
Chen-Hsiung Hung: Institute of Chemistry
Li-Chyong Chen: National Taiwan University
Kuei-Hsien Chen: Academia Sinica
Ho-Hsiu Chou: National Tsing Hua University

Nature Communications, 2024, vol. 15, issue 1, 1-13

Abstract: Abstract Designing an organic polymer photocatalyst for efficient hydrogen evolution with visible and near-infrared (NIR) light activity is still a major challenge. Unlike the common behavior of gradually increasing the charge recombination while shrinking the bandgap, we present here a series of polymer nanoparticles (Pdots) based on ITIC and BTIC units with different π-linkers between the acceptor-donor-acceptor (A-D-A) repeated moieties of the polymer. These polymers act as an efficient single polymer photocatalyst for H2 evolution under both visible and NIR light, without combining or hybridizing with other materials. Importantly, the difluorothiophene (ThF) π-linker facilitates the charge transfer between acceptors of different repeated moieties (A-D-A-(π-Linker)-A-D-A), leading to the enhancement of charge separation between D and A. As a result, the PITIC-ThF Pdots exhibit superior hydrogen evolution rates of 279 µmol/h and 20.5 µmol/h with visible (>420 nm) and NIR (>780 nm) light irradiation, respectively. Furthermore, PITIC-ThF Pdots exhibit a promising apparent quantum yield (AQY) at 700 nm (4.76%).

Date: 2024
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DOI: 10.1038/s41467-024-45085-6

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