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; Ho Hsiu Chou

doi:10.1038/s41467-024-45085-6

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, Ho Hsiu Chou

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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%).

Original language	English
Article number	707
Journal	Nature Communications
Volume	15
Issue number	1
DOIs	https://doi.org/10.1038/s41467-024-45085-6
Publication status	Published - 2024 Dec

Subject classification (UKÄ)

Polymer Chemistry
Physical Chemistry

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Elsayed, M. H., Abdellah, M., Alhakemy, A. Z., Mekhemer, I. M. A., Aboubakr, A. E. A., Chen, B. H., Sabbah, A., Lin, K. H., Chiu, W. S., Lin, S. J., Chu, C. Y., Lu, C. H., Yang, S. D., Mohamed, M. G., Kuo, S. W., Hung, C. H., Chen, L. C., Chen, K. H., & Chou, H. H. (2024). Overcoming small-bandgap charge recombination in visible and NIR-light-driven hydrogen evolution by engineering the polymer photocatalyst structure. Nature Communications, 15(1), Article 707. https://doi.org/10.1038/s41467-024-45085-6

@article{c6d880fd93034f319264f6674337eb7c,

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

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%).",

author = "Elsayed, {Mohamed Hammad} and Mohamed Abdellah and Alhakemy, {Ahmed Zaki} and Mekhemer, {Islam M.A.} and Aboubakr, {Ahmed Esmail A.} and Chen, {Bo Han} and Amr Sabbah 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}",

year = "2024",

month = dec,

doi = "10.1038/s41467-024-45085-6",

language = "English",

volume = "15",

journal = "Nature Communications",

issn = "2041-1723",

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Elsayed, MH, Abdellah, M, Alhakemy, AZ, Mekhemer, IMA, Aboubakr, AEA, Chen, BH, Sabbah, A, Lin, KH, Chiu, WS, Lin, SJ, Chu, CY, Lu, CH, Yang, SD, Mohamed, MG, Kuo, SW, Hung, CH, Chen, LC, Chen, KH & Chou, HH 2024, 'Overcoming small-bandgap charge recombination in visible and NIR-light-driven hydrogen evolution by engineering the polymer photocatalyst structure', Nature Communications, vol. 15, no. 1, 707. https://doi.org/10.1038/s41467-024-45085-6

TY - JOUR

T1 - Overcoming small-bandgap charge recombination in visible and NIR-light-driven hydrogen evolution by engineering the polymer photocatalyst structure

AU - Elsayed, Mohamed Hammad

AU - Abdellah, Mohamed

AU - Alhakemy, Ahmed Zaki

AU - Mekhemer, Islam M.A.

AU - Aboubakr, Ahmed Esmail A.

AU - Chen, Bo Han

AU - Sabbah, Amr

AU - Lin, Kun Han

AU - Chiu, Wen Sheng

AU - Lin, Sheng Jie

AU - Chu, Che Yi

AU - Lu, Chih Hsuan

AU - Yang, Shang Da

AU - Mohamed, Mohamed Gamal

AU - Kuo, Shiao Wei

AU - Hung, Chen Hsiung

AU - Chen, Li Chyong

AU - Chen, Kuei Hsien

AU - Chou, Ho Hsiu

PY - 2024/12

Y1 - 2024/12

N2 - 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%).

AB - 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%).

U2 - 10.1038/s41467-024-45085-6

DO - 10.1038/s41467-024-45085-6

M3 - Article

C2 - 38267492

AN - SCOPUS:85183006589

SN - 2041-1723

VL - 15

JO - Nature Communications

JF - Nature Communications

IS - 1

M1 - 707

ER -

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

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