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

Elsayed, Mohamed Hammad ; Abdellah, Mohamed LU ; Alhakemy, Ahmed Zaki ; Mekhemer, Islam M.A. ; Aboubakr, Ahmed Esmail A. ; Chen, Bo Han ; Sabbah, Amr ; Lin, Kun Han ; Chiu, Wen Sheng and Lin, Sheng Jie , et al. (2024) In Nature Communications 15(1).
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... (More)

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%).

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type
Contribution to journal
publication status
published
subject
in
Nature Communications
volume
15
issue
1
article number
707
publisher
Nature Publishing Group
external identifiers
  • pmid:38267492
  • scopus:85183006589
ISSN
2041-1723
DOI
10.1038/s41467-024-45085-6
language
English
LU publication?
yes
id
c6d880fd-9303-4f31-9264-f6674337eb7c
date added to LUP
2024-02-16 15:54:05
date last changed
2024-04-17 09:39:43
@article{c6d880fd-9303-4f31-9264-f6674337eb7c,
  abstract     = {{<p>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 (&gt;420 nm) and NIR (&gt;780 nm) light irradiation, respectively. Furthermore, PITIC-ThF Pdots exhibit a promising apparent quantum yield (AQY) at 700 nm (4.76%).</p>}},
  author       = {{Elsayed, Mohamed Hammad and Abdellah, Mohamed and Alhakemy, Ahmed Zaki and Mekhemer, Islam M.A. and Aboubakr, Ahmed Esmail A. and Chen, Bo Han and Sabbah, Amr and Lin, Kun Han and Chiu, Wen Sheng and Lin, Sheng Jie and Chu, Che Yi and Lu, Chih Hsuan and Yang, Shang Da and Mohamed, Mohamed Gamal and Kuo, Shiao Wei and Hung, Chen Hsiung and Chen, Li Chyong and Chen, Kuei Hsien and Chou, Ho Hsiu}},
  issn         = {{2041-1723}},
  language     = {{eng}},
  number       = {{1}},
  publisher    = {{Nature Publishing Group}},
  series       = {{Nature Communications}},
  title        = {{Overcoming small-bandgap charge recombination in visible and NIR-light-driven hydrogen evolution by engineering the polymer photocatalyst structure}},
  url          = {{http://dx.doi.org/10.1038/s41467-024-45085-6}},
  doi          = {{10.1038/s41467-024-45085-6}},
  volume       = {{15}},
  year         = {{2024}},
}