Optimally Miscible Polymer Bulk-Heterojunction-Particles for Nonsurfactant Photocatalytic Hydrogen Evolution

Wei Cheng Lin; Yu En Sun; Ying Rang Zhuang; Tse Fu Huang; Kuei Jhong Lin; Mohamed M. Elsenety; Jui Chen Yen; Hung Kai Hsu; Bo Han Chen; Chen Yu Chang; Je Wei Chang; Hsin Ni Huang; Bing Heng Li; Siriporn Jungsuttiwong; Toton Haldar; Shin Huei Wang; Wan Chi Lin; Tien Lin Wu; Chin Wen Chen; Chi Hua Yu; An Chung Su; Kun Han Lin; U. Ser Jeng; Shang Da Yang; Ho Hsiu Chou

doi:10.1021/jacs.4c13856

Optimally Miscible Polymer Bulk-Heterojunction-Particles for Nonsurfactant Photocatalytic Hydrogen Evolution

Wei Cheng Lin, Yu En Sun, Ying Rang Zhuang, Tse Fu Huang, Kuei Jhong Lin, Mohamed M. Elsenety, Jui Chen Yen, Hung Kai Hsu, Bo Han Chen, Chen Yu Chang, Je Wei Chang, Hsin Ni Huang, Bing Heng Li, Siriporn Jungsuttiwong, Toton Haldar, Shin Huei Wang, Wan Chi Lin, Tien Lin Wu, Chin Wen Chen, Chi Hua YuAn Chung Su, Kun Han Lin, U. Ser Jeng, Shang Da Yang, Ho Hsiu Chou

Department of Engineering Science

Research output: Contribution to journal › Article › peer-review

Abstract

Mini-emulsion and nanoprecipitation techniques relied on large amounts of surfactants, and unresolved miscibility issues of heterojunction materials limited their efficiency and applicability in the past. Through our molecular design and developed surfactant-free precipitation method, we successfully fabricated the best miscible bulk-heterojunction-particles (BHJP) ever achieved, using donor (PS) and acceptor (PSOS) polymers. The structural similarity ensures optimal miscibility, as supported by the interaction parameter of the PS/PSOS blend is positioned very close to the binodal curve. Experimental studies and molecular dynamics simulations further revealed that surfactants hinder electron output sites and reduce the concentration of sacrificial agents at the interface, slowing polaron formation. Multiscale experiments verified that these BHJP, approximately 12 nm in diameter, further form cross-linked fractal networks of several hundred nanometers. Transient absorption spectroscopy showed that BHJP facilitates polaron formation and electron transfer. Our BHJP demonstrated a superior hydrogen evolution rate (HER) compared to traditional methods. The most active BHJP achieved an HER of 251.2 mmol h^-1 g^-1 and an apparent quantum yield of 26.2% at 500 nm. This work not only introduces a practical method for preparing BHJP but also offers a new direction for the development of heterojunction materials.

Original language	English
Pages (from-to)	2537-2548
Number of pages	12
Journal	Journal of the American Chemical Society
Volume	147
Issue number	3
DOIs	https://doi.org/10.1021/jacs.4c13856
Publication status	Published - 2025 Jan 22

All Science Journal Classification (ASJC) codes

Catalysis
General Chemistry
Biochemistry
Colloid and Surface Chemistry

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10.1021/jacs.4c13856

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Lin, W. C., Sun, Y. E., Zhuang, Y. R., Huang, T. F., Lin, K. J., Elsenety, M. M., Yen, J. C., Hsu, H. K., Chen, B. H., Chang, C. Y., Chang, J. W., Huang, H. N., Li, B. H., Jungsuttiwong, S., Haldar, T., Wang, S. H., Lin, W. C., Wu, T. L., Chen, C. W., ... Chou, H. H. (2025). Optimally Miscible Polymer Bulk-Heterojunction-Particles for Nonsurfactant Photocatalytic Hydrogen Evolution. Journal of the American Chemical Society, 147(3), 2537-2548. https://doi.org/10.1021/jacs.4c13856

@article{a143aa2b63e04f83bfc06df943c59f29,

title = "Optimally Miscible Polymer Bulk-Heterojunction-Particles for Nonsurfactant Photocatalytic Hydrogen Evolution",

abstract = "Mini-emulsion and nanoprecipitation techniques relied on large amounts of surfactants, and unresolved miscibility issues of heterojunction materials limited their efficiency and applicability in the past. Through our molecular design and developed surfactant-free precipitation method, we successfully fabricated the best miscible bulk-heterojunction-particles (BHJP) ever achieved, using donor (PS) and acceptor (PSOS) polymers. The structural similarity ensures optimal miscibility, as supported by the interaction parameter of the PS/PSOS blend is positioned very close to the binodal curve. Experimental studies and molecular dynamics simulations further revealed that surfactants hinder electron output sites and reduce the concentration of sacrificial agents at the interface, slowing polaron formation. Multiscale experiments verified that these BHJP, approximately 12 nm in diameter, further form cross-linked fractal networks of several hundred nanometers. Transient absorption spectroscopy showed that BHJP facilitates polaron formation and electron transfer. Our BHJP demonstrated a superior hydrogen evolution rate (HER) compared to traditional methods. The most active BHJP achieved an HER of 251.2 mmol h-1 g-1 and an apparent quantum yield of 26.2% at 500 nm. This work not only introduces a practical method for preparing BHJP but also offers a new direction for the development of heterojunction materials.",

author = "Lin, {Wei Cheng} and Sun, {Yu En} and Zhuang, {Ying Rang} and Huang, {Tse Fu} and Lin, {Kuei Jhong} and Elsenety, {Mohamed M.} and Yen, {Jui Chen} and Hsu, {Hung Kai} and Chen, {Bo Han} and Chang, {Chen Yu} and Chang, {Je Wei} and Huang, {Hsin Ni} and Li, {Bing Heng} and Siriporn Jungsuttiwong and Toton Haldar and Wang, {Shin Huei} and Lin, {Wan Chi} and Wu, {Tien Lin} and Chen, {Chin Wen} and Yu, {Chi Hua} and Su, {An Chung} and Lin, {Kun Han} and Jeng, {U. Ser} and Yang, {Shang Da} and Chou, {Ho Hsiu}",

note = "Publisher Copyright: {\textcopyright} 2024 The Authors. Published by American Chemical Society.",

year = "2025",

month = jan,

day = "22",

doi = "10.1021/jacs.4c13856",

language = "English",

volume = "147",

pages = "2537--2548",

journal = "Journal of the American Chemical Society",

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Lin, WC, Sun, YE, Zhuang, YR, Huang, TF, Lin, KJ, Elsenety, MM, Yen, JC, Hsu, HK, Chen, BH, Chang, CY, Chang, JW, Huang, HN, Li, BH, Jungsuttiwong, S, Haldar, T, Wang, SH, Lin, WC, Wu, TL, Chen, CW, Yu, CH, Su, AC, Lin, KH, Jeng, US, Yang, SD & Chou, HH 2025, 'Optimally Miscible Polymer Bulk-Heterojunction-Particles for Nonsurfactant Photocatalytic Hydrogen Evolution', Journal of the American Chemical Society, vol. 147, no. 3, pp. 2537-2548. https://doi.org/10.1021/jacs.4c13856

TY - JOUR

T1 - Optimally Miscible Polymer Bulk-Heterojunction-Particles for Nonsurfactant Photocatalytic Hydrogen Evolution

AU - Lin, Wei Cheng

AU - Sun, Yu En

AU - Zhuang, Ying Rang

AU - Huang, Tse Fu

AU - Lin, Kuei Jhong

AU - Elsenety, Mohamed M.

AU - Yen, Jui Chen

AU - Hsu, Hung Kai

AU - Chen, Bo Han

AU - Chang, Chen Yu

AU - Chang, Je Wei

AU - Huang, Hsin Ni

AU - Li, Bing Heng

AU - Jungsuttiwong, Siriporn

AU - Haldar, Toton

AU - Wang, Shin Huei

AU - Lin, Wan Chi

AU - Wu, Tien Lin

AU - Chen, Chin Wen

AU - Yu, Chi Hua

AU - Su, An Chung

AU - Lin, Kun Han

AU - Jeng, U. Ser

AU - Yang, Shang Da

AU - Chou, Ho Hsiu

PY - 2025/1/22

Y1 - 2025/1/22

N2 - Mini-emulsion and nanoprecipitation techniques relied on large amounts of surfactants, and unresolved miscibility issues of heterojunction materials limited their efficiency and applicability in the past. Through our molecular design and developed surfactant-free precipitation method, we successfully fabricated the best miscible bulk-heterojunction-particles (BHJP) ever achieved, using donor (PS) and acceptor (PSOS) polymers. The structural similarity ensures optimal miscibility, as supported by the interaction parameter of the PS/PSOS blend is positioned very close to the binodal curve. Experimental studies and molecular dynamics simulations further revealed that surfactants hinder electron output sites and reduce the concentration of sacrificial agents at the interface, slowing polaron formation. Multiscale experiments verified that these BHJP, approximately 12 nm in diameter, further form cross-linked fractal networks of several hundred nanometers. Transient absorption spectroscopy showed that BHJP facilitates polaron formation and electron transfer. Our BHJP demonstrated a superior hydrogen evolution rate (HER) compared to traditional methods. The most active BHJP achieved an HER of 251.2 mmol h-1 g-1 and an apparent quantum yield of 26.2% at 500 nm. This work not only introduces a practical method for preparing BHJP but also offers a new direction for the development of heterojunction materials.

AB - Mini-emulsion and nanoprecipitation techniques relied on large amounts of surfactants, and unresolved miscibility issues of heterojunction materials limited their efficiency and applicability in the past. Through our molecular design and developed surfactant-free precipitation method, we successfully fabricated the best miscible bulk-heterojunction-particles (BHJP) ever achieved, using donor (PS) and acceptor (PSOS) polymers. The structural similarity ensures optimal miscibility, as supported by the interaction parameter of the PS/PSOS blend is positioned very close to the binodal curve. Experimental studies and molecular dynamics simulations further revealed that surfactants hinder electron output sites and reduce the concentration of sacrificial agents at the interface, slowing polaron formation. Multiscale experiments verified that these BHJP, approximately 12 nm in diameter, further form cross-linked fractal networks of several hundred nanometers. Transient absorption spectroscopy showed that BHJP facilitates polaron formation and electron transfer. Our BHJP demonstrated a superior hydrogen evolution rate (HER) compared to traditional methods. The most active BHJP achieved an HER of 251.2 mmol h-1 g-1 and an apparent quantum yield of 26.2% at 500 nm. This work not only introduces a practical method for preparing BHJP but also offers a new direction for the development of heterojunction materials.

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DO - 10.1021/jacs.4c13856

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SN - 0002-7863

VL - 147

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JO - Journal of the American Chemical Society

JF - Journal of the American Chemical Society

IS - 3

ER -

Optimally Miscible Polymer Bulk-Heterojunction-Particles for Nonsurfactant Photocatalytic Hydrogen Evolution

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