Molecular Weight Distribution Effects on the Structural and Mechanical Performance of Conjugated Polymers Incorporating Flexible Spacers: A Simulation Study

Hai-Yan Weng; Ji-Yuan Xing; Rui Shi; Zhong-Yuan Lu

doi:10.1007/s10118-026-3626-5

Your Location：

Home >

Browse articles >

Molecular Weight Distribution Effects on the Structural and Mechanical Performance of Conjugated Polymers Incorporating Flexible Spacers: A Simulation Study

RESEARCH ARTICLE | Updated：2026-07-01

- Molecular Weight Distribution Effects on the Structural and Mechanical Performance of Conjugated Polymers Incorporating Flexible Spacers: A Simulation Study
  Enhanced Publication
- Molecular Weight Distribution Effects on the Structural and Mechanical Performance of Conjugated Polymers Incorporating Flexible Spacers: A Simulation Study
- Chinese Journal of Polymer Science 2026年44卷第7期页码：2331-2340
- Affiliations：
  
  a.State Key Laboratory of Supramolecular Structure and Materials, Institute of Theoretical Chemistry, Jilin University, Changchun 130023, China
  b.State Key Laboratory of Electroanalytical Chemistry, Changchun Institute of Applied Chemistry, Chinese Academy of Sciences, Changchun 130023, China
- Author bio：
  
  shirui816@jlu.edu.cn (R.S.)
  luzhy@jlu.edu.cn (Z.Y.L.)
- Funds：
  
  This work was financially supported by the National Natural Science Foundation of China (No.22133002).;The authors declare no interest conflict.Electronic supplementary information (ESI) is available free of charge in the online version of this article at http://doi.org/10.1007/s10118-026-3626-5.The data that support the findings of this study are available from the corresponding author upon reasonable request. The author's contact information: luzhy@jlu.edu.cn.
- DOI：10.1007/s10118-026-3626-5
  中图分类号：
- 收稿：2026-02-15，
  
  录用：2026-03-12，
  
  网络首发：2026-05-28，
  
  纸质出版：2026-07-05
- Accepted：
Scan QR Code
Weng, H. Y.; Xing, J. Y.; Shi, R.; Lu, Z. Y. Molecular weight distribution effects on the structural and mechanical performance of conjugated polymers incorporating flexible spacers: a simulation study. Chinese J. Polym. Sci. 2026, 44, 2331–2340

Hai-Yan Weng, Ji-Yuan Xing, Rui Shi, et al. Molecular Weight Distribution Effects on the Structural and Mechanical Performance of Conjugated Polymers Incorporating Flexible Spacers: A Simulation Study[J]. Chinese Journal of Polymer Science, 2026, 44(7): 2331-2340.
Weng, H. Y.; Xing, J. Y.; Shi, R.; Lu, Z. Y. Molecular weight distribution effects on the structural and mechanical performance of conjugated polymers incorporating flexible spacers: a simulation study. Chinese J. Polym. Sci. 2026, 44, 2331–2340 DOI： 10.1007/s10118-026-3626-5.

Hai-Yan Weng, Ji-Yuan Xing, Rui Shi, et al. Molecular Weight Distribution Effects on the Structural and Mechanical Performance of Conjugated Polymers Incorporating Flexible Spacers: A Simulation Study[J]. Chinese Journal of Polymer Science, 2026, 44(7): 2331-2340. DOI： 10.1007/s10118-026-3626-5.

摘要

This work demonstrates that molecular weight distribution

quantified by the polydispersity index (PDI)

governs structure-property relationships in conjugated polymers incorporating flexible spacers. Increasing PDI promotes a loop-to-bridge conformational transition

transforming lamellar phase to perforated lamellar phase at intermediate rigid-segment lengths

switching deformation from destructive fibrillation to reconstructive strengthening

and enhancing both yield strength and strain.

Abstract

Conjugated polymers incorporating flexible spacers (CP-FSs) offer a promising route to mechanically robust active layers for flexible organic solar cells. However

the influence of molecular weight distribution (MWD)—a fundamental polymer characteristic—on structural and mechanical performance remains poorly understood due to synthetic challenges. Here

we employ dissipative particle dynamics and coarse-grained molecular dynamics simulations to elucidate how MWD

quantified by polydispersity index (PDI)

governs structure-property relationships in CP-FSs. Our results reveal that PDI acts as a molecular switch controlling phase morphology: increasing PDI drives transitions from lamellar to perforated lamellar structures at intermediate rigid segment lengths. At the molecular level

higher PDI significantly increases the fraction of bridging conformations (

$$ {\nu }_{\mathrm{bridge}} $$

https://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=111930340&type=

https://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=111930340&type=small

http://notExist.jpg

)

strengthening a load-bearing network. During tensile deformation

this enhanced load-bearing network suppresses destructive fibrillation and instead promotes reconstructive strengthening through dynamic loop-to-bridge transitions. These findings demonstrate that controlled MWD offers a composition-independent strategy for developing mechanically robust active layers

providing practical guidelines for flexible organic solar cell design.

关键词

Keywords

references

Li, S.; Li, Z.; Wan, X.; Chen, Y. Recent progress in flexible organic solar cells. eScience 2023 , 3 , 100085..

Wang, D.; Liu, H.; Li, Y.; Zhou, G.; Zhan, L.; Zhu, H.; Lu, X.; Chen, H.; Li, C. Z. High-performance and eco-friendly semitransparent organic solar cells for greenhouse applications. Joule 2021 , 5 , 945−957..

Zhu, J.; Xia, J.; Li, Y.; Li, Y. Perspective on flexible organic solar cells for self-powered wearable applications. ACS Appl. Mater. Interfaces 2025 , 17 , 5595−5608..

Song, W.; Ye, Q.; Chen, Z.; Ge, J.; Xie, L.; Ge, Z. Advances in stretchable organic photovoltaics: flexible transparent electrodes and deformable active layer design. Adv. Mater. 2024 , 36 , 2311170..

Yang, F.; Huang, Y.; Li, Y.; Li, Y. Large-area flexible organic solar cells. npj Flex. Electron. 2021 , 5 , 30..

Yan, Y.; Duan, B.; Ru, M.; Gu, Q.; Li, S.; Zhao, W. Toward flexible and stretchable organic solar cells: a comprehensive review of transparent conductive electrodes, photoactive materials, and device performance. Adv. Energy Mater. 2025 , 15 , 2404233..

Park, J. S.; Kim, G. U.; Lee, S.; Lee, J. W.; Li, S.; Lee, J. Y.; Kim, B. J. Material design and device fabrication strategies for stretchable organic solar cells. Adv. Mater. 2022 , 34 , 2201623..

Mitchell, V.; Jones, D. Advances toward the effective use of block copolymers as organic photovoltaic active layers. Polym. Chem. 2018 , 9 , 795−814..

Zhou, H.; Yang, L.; You, W. Rational design of high performance conjugated polymers for organic solar cells. Macromolecules 2012 , 45 , 607−632..

Qiu, Z.; Hammer, B. A.; Müllen, K. Conjugated polymers–Problems and promises. Prog. Polym. Sci. 2020 , 100 , 101179..

Lee, Y.; Gomez, E. D. Challenges and opportunities in the development of conjugated block copolymers for photovoltaics. Macromolecules 2015 , 48 , 7385−7395..

Xie, R.; Colby, R. H.; Gomez, E. D. Connecting the mechanical and conductive properties of conjugated polymers. Adv. Electron. Mater. 2018 , 4 , 1700356..

Zuo, J.; Han, D.; Yao, H.; Kuvondikov, V.; Ye, L. Stretching the future: strategies and emerging trends in stretchable organic photovoltaic materials. Energy Environ. Sci. 2025 , 18 , 6344−6365..

Zheng, Y.; Zhang, S.; Tok, J. B. H.; Bao, Z. Molecular design of stretchable polymer semiconductors: current progress and future directions. J. Am. Chem. Soc. 2022 , 144 , 4699−4715..

Root, S. E.; Savagatrup, S.; Printz, A. D.; Rodriquez, D.; Lipomi, D. J. Mechanical propertie s of organic semiconductors for stretchable, highly flexible, and mechanically robust electronics. Chem. Rev. 2017 , 117 , 6467−6499..

Genene, Z.; Lee, J. W.; Lee, S. W.; Chen, Q.; Tan, Z.; Abdulahi, B. A.; Yu, D.; Kim, T. S.; Kim, B. J.; Wang, E. Polymer acceptors with flexible spacers afford efficient and mechanically robust all-polymer solar cells. Adv. Mater. 2022 , 34 , 2107361..

Chen, Q.; Han, Y. H.; Franco, L. R.; Marchiori, C. F.; Genene, Z.; Araujo, C. M.; Lee, J. W.; Phan, T. N. L.; Wu, J.; Yu, D. Effects of flexible conjugation-break spacers of non-conjugated polymer acceptors on photovoltaic and mechanical properties of all-polymer solar cells. Nano-Micro Lett. 2022 , 14 , 164..

Luo, X.; Freychet, G.; Gan, Z.; An, K.; Du, H.; Wang, C.; Li, N.; Zhong, W.; Ying, L. Intrinsically stretchable organic photovoltaic thin films enabled by optimized donor–acceptor pairing. Macromolecules 2023 , 56 , 8928−8938..

Ye, Q.; Chen, Z.; Yang, D.; Song, W.; Zhu, J.; Yang, S.; Ge, J.; Chen, F.; Ge, Z. Ductile oligomeric acceptor-modified flexible organic solar cells show excellent mechanical robustness and near 18% efficiency. Adv. Mater. 2023 , 35 , 2305562..

Wang, H.; Kou, H.; Pan, J.; Wang, X.; Liu, D.; Yang, R. Design high-performance stretchable light-harvesting polymers for organic solar cells via synergistic effect of flexible alkyl segment and hydrogen bond. Small 2025 , 21 , 2412767..

Rahmanudin, A.; Yao, L.; Sivula, K. Conjugation break spacers and flexible linkers as tools to engineer the properties of semiconducting polymers. Polym. J. 2018 , 50 , 725−736..

Ding, Z.; Liu, D.; Zhao, K.; Han, Y. Optimizing morphology to trade off charge transport and mechanical properties of stretchable conjugated polymer films. Macromolecules 2021 , 54 , 3907−3926..

Zhu, J.; Yan, C.; Wang, J.; Li, H.; Cheng, P. Control of molecular aggregation structures towards flexible organic photovoltaics. Mater. Horiz. 2025 , 12 , 6069−6081..

Lee, J. W.; Sun, C.; Lee, S. W.; Kim, G. U.; Li, S.; Wang, C.; Kim, T. S.; Kim, Y. H.; Kim, B. J. Sequentially regular polymer acceptors featuring flexible spacers for high-performance and mechanically robust all-polymer solar cel ls. Energy Environ. Sci. 2022 , 15 , 4672−4685..

Seo, S.; Lee, J. W.; Kim, D. J.; Lee, D.; Phan, T. N. L.; Park, J.; Tan, Z.; Cho, S.; Kim, T. S.; Kim, B. J. Poly (dimethylsiloxane)-block-PM6 polymer donors for high-performance and mechanically robust polymer solar cells. Adv. Mater. 2023 , 35 , 2300230..

Lee, J. W.; Jeong, D.; Kim, D. J.; Phan, T. N. L.; Park, J. S.; Kim, T. S.; Kim, B. J. Flexible-spacer incorporated polymer donors enable superior blend miscibility for high-performance and mechanically-robust polymer solar cells. Energy Environ. Sci. 2021 , 14 , 4067−4076..

Ding, Z.; Hua, J.; Gao, Z.; Wang, M.; Zhao, K.; Han, Y. Molecular weight optimization for intrinsically stretchable conjugated polymers: from film microstructure to strain-insensitive performance. J. Mater. Chem. C 2025 , 13 , 12612−12627..

Ismail Saqib, M.; Yin, X.; Liu, Z.; Zhao, M.; Cheng, M.; Li, Y.; Song, C.; Liang, Q.; Xin, J.; Miao, Z. The effects of polymer molecular weight on morphology and the device efficiency: progress and prospects for organic solar cells. Macromol. Chem. Phys. 2025 , 226 , 2500031..

Lee, H. G.; Lee, J. W.; Oh, E. S.; Lee, M. J.; Kim, T. S.; Lee, C.; Kim, B. J. The effect of rigid-block length in elastomer-containing photoactive block copolymers on the photovoltaic and mechanical properties of polymer solar cells. J. Mater. Chem. A 2024 , 12 , 19039−19051..

Liang, Z.; Neshchadin, A.; Zhang, Z.; Zhao, F. G.; Liu, X.; Yu, L. Stille polycondensation: a multifaceted approach towards the synthesis of polymers with semiconducting properties. Polym. Chem. 2023 , 14 , 4611−4625..

Tian, D.; Wang, J.; Huang, X.; Ding, Y.; Hu, A. Understanding broad polydispersity in step-growth polymerization via catalyst competition mechanism. Chinese J. Polym. Sci. 2024 , 42 , 1897−1904..

Shin, W.; Ko, W.; Jin, S. H.; Earmme, T.; Hwang, Y. J. Reproducible and rapid synthesis of a conjugated polymer by Stille polycondensation in flow: Effects of reaction parameters on molecular weight. Chem. Eng. J. 2021 , 412 , 128572..

Caddeo, C.; Ackermann, J.; Mattoni, A. A theoretical perspective on the thermodynamic stability of polymer blends for solar cells: From experiments to predictive modeling. Solar RRL 2022 , 6 , 2200172..

Li, Z.; Tolba, S. A.; Wang, Y.; Alesadi, A.; Xia, W. Modeling-driven materials by design for conjugated polymers: insights into optoelectronic, conformational, and thermomechanical properties. Chem. Commun. 2024 , 60 , 11625−11641..

Gao, H.; Yu, Z.; Zhang, X.; Yu, X.; Xing, J.; Zhu, Y.; Qian, H. J.; Lu, Z. Y. A mini review of the recent progress in coarse-grained simulation of polymer systems. Chin. J. Struct. Chem. 2024 , 43 , 100266..

Flory, P. J. Molecular size distribution in linear condensation polymers. J. Am. Chem. Soc. 1936 , 58 , 1877−1885..

Chu, X.; Xu, Z.; Cao, Y. C.; Li, W. Simulation study on the mechanical properties of lamella-forming ABABA linear multiblock copolymers. Macromolecules 2024 , 57 , 9536−9545..

Xu, Z.; Chu, X.; Li, W. Microscopic origins of the distinct mechanical response of ABA and ABC block copolymer nanostructures. ACS Macro Lett. 2024 , 13 , 240−246..

Chen, T.; Xu, Z.; Chu, X.; Peng, L.; Huang, X.; Li, W. A simulation study on the effect of tailoring molecular architectures on the mechanical behaviors of lamella-forming BABCB linear multiblock copolymers. Macromolecules 2025 , 58 , 6387−6398..

Stukowski, A. Visualization and analysis of atomistic simulation data with OVITO–the Open Visualization Tool. Model. Simul. Mater. Sci. Eng. 2009 , 18 , 015012..

Zhu, Y. L.; Liu, H.; Li, Z. W.; Qian, H. J.; Milano, G.; Lu, Z. Y. GALAMOST: GPU-accelerated large-scale molecular simulation toolkit. J. Comput. Chem. 2013 , 34 , 2197−2211..

[Xu, J.; Guo, S.; Zhen, M.; Yu, Z.; Zhu, Y.; Milano, G.; Lu, Z. PyGAMD: python graphics processing unit-accelerated molecular dynamics software. Mater. Genome Eng. Adv . 2025, e70019..

Matsen, M. W. Polydispersity-induced macrophase separation in diblockcopolymer melts. Phys. Rev. Lett. 2007 , 99 , 148304..

Kim, I.; Li, S. Recent progress on polydispersity effects on block copolymer phase behavior. Polym. Rev. 2019 , 59 , 561−587..

Li, S.; Li, K.; Xu, Q.; Wang, Y.; Yu, C.; Zhou, Y. Solution self-assembly behavior of rod-alt-coil alternating copolymers via simulations. Phys. Chem. Chem. Phys. 2019 , 21 , 25148−25157..

Matsen, M. Bridging and looping in multiblock copolymer melts. J. Chem. Phys. 1995 , 102 , 3884−3887..

Rasool, S.; Yeop, J.; Cho, H. W.; Lee, W.; Kim, J. W.; Yuk, D.; Kim, J. Y. Path to the fabrication of efficient, stable and commercially viable large-area organic solar cells. Mater. Futures 2023 , 2 , 032102..

Yu, W.; Zou, Y.; Zhang, S.; Liu, Z.; Wu, C.; Qu, B.; Chen, Z.; Xiao, L. Carbon-based perovskite solar cells with electron and hole-transporting/-blocking layers. Mater. Futures 2023 , 2 , 022101..

Zhang, L.; Wang, Y.; Meng, X.; Zhang, J.; Wu, P.; W ang, M.; Cao, F.; Chen, C.; Wang, Z.; Yang, F. The issues on the commercialization of perovskite solar cells. Mater. Futures 2024 , 3 , 022101..

浏览量

Downloads

CSCD

文章被引用时，请邮件提醒。

Submit

工具集

关联资源

Facile Preparation of Super-strong and Tough Poly(vinyl alcohol)/Carbon Nanotube Hydrogel Enabled by Triple Crosslinking Networks

Tough Polymeric Hydrogels Based on Amino Acid Derivative Mediated Dynamic Metal Coordination Bonds

Durable Anti-fogging and Abrasion-resistant Coatings Based on Polyoxometalates-Hydrophilic Resin Composites with Enhanced Cohesion and Adhesion

Sequence-encoded Conformation Pathways in Viscoelastic Microphase Separation of Multiblock Copolymers

Porous Organic Polymers for Photocatalytic Hydrogen Peroxide Production: Recent Advances and Future Perspectives