Solid-additive-regulated Non-equilibrium Film Formation Enables Highly-efficient Green-solvent-printed Binary Organic Solar Cells and Solar Modules

Shan-Hua Zhang; Rui Sun; Zi-Cheng Xing; Jia-Wang Qiu; Lin-Yong Xu; Yu-Hao Liu; Tian-Rui Qu; Xin-Rong Yang; Jie Min

doi:10.1007/s10118-026-3838-8

您当前的位置：

首页 >

文章列表页 >

Solid-additive-regulated Non-equilibrium Film Formation Enables Highly-efficient Green-solvent-printed Binary Organic Solar Cells and Solar Modules

RESEARCH ARTICLE | 更新时间：2026-11-03

- Solid-additive-regulated Non-equilibrium Film Formation Enables Highly-efficient Green-solvent-printed Binary Organic Solar Cells and Solar Modules
- Solid-additive-regulated Non-equilibrium Film Formation Enables Highly-efficient Green-solvent-printed Binary Organic Solar Cells and Solar Modules
- Chinese Journal of Polymer Science 2026年44卷页码：1-12
- 作者机构：
  
  a.The Institute for Advanced Studies, School of Electrical Engineering and Automation, Wuhan University, Wuhan 430072, China
  b.Key Laboratory for Preparation and Application of Ordered Structural Materials of Guangdong Province, Shantou University, Shantou 515063, China
  c.Anhui Province Key Laboratory for Control and Application of Optoelectronic Information Materials, Anhui Normal University, Wuhu 241002, China
- 作者简介：
  
  sun.rui@whu.edu.cn (R.S.)
  min.jie@whu.edu.cn (J.M.)
- 基金信息：
  
  This work was financially supported by the National Natural Science Foundation of China (NSFC) (Nos. 22279094 and 22409149), Anhui Province Key Laboratory for Control and Application of Optoelectronic Information Materials (No. OIM-2024-01), and Key Laboratory for Preparation and Application of Ordered Structural Materials of Guangdong Province. The authors extend their gratitude to the technical staff from Scientific Compass www.shiyanjia.com for providing invaluable assistance with the FTIR analysis. We thank the Core Facility of Wuhan University for the AFM and TEM measurements. The authors thank the resonant soft X-ray scattering beamline (Jinhua) BL05U-B of Hefei Light Source, jointly constructed by the Zhejiang Institute of Optoelectronics and the National Synchrotron Radiation Laboratory of the University of Science and Technology of China.;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/s10118-026-3838-8.The data that support the findings of this study are available from the corresponding author upon reasonable request.
- DOI：10.1007/s10118-026-3838-8
  中图分类号：
- 收稿：2026-06-16，
  
  录用：2026-08-10，
  
  网络首发：2026-11-02，
  
  纸质出版：2026-09
- 稿件说明：
移动端阅览
Zhang, S. H.; Sun, R.; Xing, Z. C.; Qiu, J. W.; Xu, L. Y.; Liu, Y. H.; Qu, T. R.; Yang, X. R.; Min, J. Solid-additive-regulated non-equilibrium film formation enables highly-efficient green-solvent-printed binary organic solar cells and solar modules. Chinese J. Polym. Sci. https://doi.org/10.1007/s10118-026-3838-8

Shan-Hua Zhang, Rui Sun, Zi-Cheng Xing, et al. Solid-additive-regulated Non-equilibrium Film Formation Enables Highly-efficient Green-solvent-printed Binary Organic Solar Cells and Solar Modules[J/OL]. Chinese Journal of Polymer Science, 2026, 441-12.
Zhang, S. H.; Sun, R.; Xing, Z. C.; Qiu, J. W.; Xu, L. Y.; Liu, Y. H.; Qu, T. R.; Yang, X. R.; Min, J. Solid-additive-regulated non-equilibrium film formation enables highly-efficient green-solvent-printed binary organic solar cells and solar modules. Chinese J. Polym. Sci. https://doi.org/10.1007/s10118-026-3838-8 DOI：

Shan-Hua Zhang, Rui Sun, Zi-Cheng Xing, et al. Solid-additive-regulated Non-equilibrium Film Formation Enables Highly-efficient Green-solvent-printed Binary Organic Solar Cells and Solar Modules[J/OL]. Chinese Journal of Polymer Science, 2026, 441-12. DOI： 10.1007/s10118-026-3838-8.

摘要

Abstract

The commercialization of organic solar cells (OSCs) requires a transition from laboratory-scale spin-coating to high-throughput

environmentally friendly printing technologies. However

rapid crystallization and non-equilibrium molecular assembly during green-solvent processing often induce disordered morphologies and severe efficiency losses. Here

we introduce two nonhalogenated solid additives

2-methoxynaphthalene (2-MN) and 2

7-dimethoxynaphthalene (2

7-MN)

to regulate crystallization kinetics and film formation in blade-coated OSCs processed from the green solvent

-xylene. Benefiting from its symmetric molecular structure and stronger intermolecular interactions

7-MN effectively prolongs the liquid-solid transition and suppresses premature aggregation

enabling the formation of a highly ordered bi-continuous interpenetrating network with optimized charge-transport pathways. As a result

green-solvent-processed OSCs achieve a champion power conversion efficiency of 20.19% with an exceptional fill factor of 81.52%. Notably

the morphology control enabled by 2

7-MN remains robust under high-speed coating (30 m·min

–1

)

maintaining efficiencies approaching 19%. Importantly

large-area modules (15.84 and

76.95 cm

) deliver impressive efficiencies of 16.80% and 15.71%

respectively

which are the highest values reported in green-solvent-processed OSCs so far. This work establishes solid-additive engineering as an effective strategy for controlling non-equilibrium film formation toward scalable and sustainable organic photovoltaics.

关键词

Keywords

references

Xie, D.; Wu, B.; Wu, Q.; Deng, B.; Li, J.; Chen, Z.; Zhu, J.; Xia, R.; Pan, L.; Liu, K.; Jiang, Q.; Feng, H.; Yuan, X.; Zhang, Y.; Jiang, Q.; Liu, D.; Xu, T.; Li, H.; Huang, F.; Cao, Y.; Duan, C. Scalable polymer for large-area semitransparent organic photovoltaics. Joule 2025 , 9 , 102173..

Lu, X.; Xie, C.; Liu, Y.; Zheng, H.; Feng, K.; Xiong, Z.; Wei, W.; Zhou, Y. Increase in the efficiency and stability of large-area flexible organic photovoltaic modules via improved electrical contact. Nat. Energy 2024 , 9 , 793−802..

Jinno, H.; Fukuda, K.; Xu, X.; Park, S.; Suzuki, Y.; Koizumi, M.; Yokota, T.; Osaka, I.; Takimiya, K.; Someya, T. Stretchable and waterproof elastomer-coated organic photovoltaics for washable electronic textile applications. Nat. Energy 2017 , 2 , 780−785..

Corzo, D.; Rosas-Villalva, D.; C, A.; Tostado-Blázquez, G.; Alexandre, E. B.; Hernandez, L. H.; Han, J.; Xu, H.; Babics, M.; De Wolf, S.; Baran, D. High-performing organic electronics using terpene green solvents from renewable feedstocks. Nat. Energy 2023 , 8 , 62−73..

Shi, H. Y.; Xing, L.; Chen, M. X.; Chen, Z. Y.; Deng, M. W.; Xu, L. Y.; Wu, X. H.; Yang, X. R.; Shao, Y. M.; Papkovskaya, E. D.; Luponosov, Y.; Sun, R.; Min, J. Pendant Y-series acceptors with well-controlled morphology enabled high performance and stability all-polymer solar cells. Chinese J. Polym. Sci. 2025 , 43 , 1516−1526..

Burgués-Ceballos, I.; Lucera, L.; Tiwana, P.; Ocytko, K.; Tan, L. W.; Kowalski, S.; Snow, J.; Pron, A.; Bürckstümmer, H.; Blouin, N.; Morse, G. Transparent organic photovoltaics: a strategic niche to advance commercialization. Joule 2021 , 5 , 2261−2272..

Chen, H.; Huang, Y.; Zhang, R.; Mou, H.; Ding, J.; Zhou, J.; Wang, Z.; Li, H.; Chen, W.; Zhu, J.; Cheng, Q.; Gu, H.; Wu, X.; Zhang, T.; Wang, Y.; Zhu, H.; Xie, Z.; Gao, F.; Li, Y.; Li, Y. Organic solar cells with 20.82% efficiency and high tolerance of active layer thickness through crystallization sequence manipulation. Nat. Mater. 2025 , 24 , 444−453..

Wang, Y.; Wen, J.; Zhong, Y.; Fu, L.; You, Z.; Li, H.; Han, G.; Han, W.; Liu, J.; Zhang, H.; Feng, Y.; Li, H.; Liu, W.; Zhang, J.; Han, K.; Liu, Y. Homology-guided zwitterionic interlayers for 21% efficiency non-fullerene organic solar cells. Adv. Mater. 2026 , 38 , e20669..

Fu, J.; Li, H.; Liu, H.; Huang, P.; Chen, H.; Fong, P. W. K.; Dela Peña, T. A.; Li, M.; Lu, X.; Cheng, P.; Xiao, Z.; Lu, S.; Li, G. Two-step crystallization modulated through acenaphthene enabling 21% binary organic solar cells and 83.2% fill factor. Nat. Energy 2025 , 10 , 1251−1261..

Basu, R.; Gumpert, F.; Lohbreier, J.; Morin, P. O.; Vohra, V.; Liu, Y.; Zhou, Y.; Brabec, C. J.; Egelhaaf, H. J.; Distler, A. Large-area organic photovoltaic modules with 14.5% certified world record efficiency. Joule 2024 , 8 , 970−978..

Carlé, J. E.; Helgesen, M.; Hagemann, O.; Hösel, M.; Heckler, I. M.; Bundgaard, E.; Gevorgyan, S. A.; Søndergaard, R. R.; Jørgensen, M.; García-Valverde, R.; Chaouki-Almagro, S.; Villarejo, J. A.; Krebs, F. C. Overcoming the scaling lag for polymer solar cells. Joule 2017 , 1 , 274−289..

Zhang, B.; Yang, F.; Li, Y. Recent progress in large-area organic solar cells. Small Sci. 2023 , 3 , 2300004..

Han, J.; Xu, H.; Corzo, D.; Sharma, A.; Baran, D. Pathways to commercially viable organic photovoltaic materials. Nat. Mater. 2026 , 25 , 725−736..

Zhou, M.; Xu, X.; Wang, D.; Song, J.; Qiao, J.; Zhang, R.; Wu, Y.; Wang, T.; Cui, J.; Hall, C. R.; Yin, H.; Du, X.; Qin, W.; Gao, K.; Chen, F.; Wei, Z.; Ashokkumar, M.; Smith, T. A.; Zhang, K.; Sun, Y.; Hao, X. Sonication-induced J-aggregation in nonhalogenated solvents boosts exciton delocalization for high-efficiency organic solar cells. Nat. Commun. 2025 , 16 , 10458..

Harillo-Baños, A.; Fan, Q.; Riera-Galindo, S.; Wang, E.; Inganäs, O.; Campoy-Quiles, M. High-throughput screening of blade-coated polymer: polymer solar cells: solvent determines achievable performance. ChemSusChem 2022 , 15 , e202101888..

Yang, S.; Chen, X.; Pan, Y.; Fang, J.; Han, Y.; Wang, Z.; Qian, F.; Qi, W.; Shui, K.; Zhang, Q.; Guo, F.; Sun, Y.; Ma, C. Q.; Luo, Q. High cell to module efficiency remaining ratio of ≈90% for the 100 cm 2 fully roll-to-roll gravure printed flexible organic solar cells from non-halogenated solvent. Adv. Mater. 2025 , 37 , 2500115..

Chen, H.; Zhang, R.; Chen, X.; Zeng, G.; Kobera, L.; Abbrent, S.; Zhang, B.; Chen, W.; Xu, G.; Oh, J.; Kang, S. H.; Chen, S.; Yang, C.; Brus, J.; Hou, J.; Gao, F.; Li, Y.; Li, Y. A guest-assisted molecular-organization approach for > 17% efficiency organic solar cells using environmental ly friendly solvents. Nat. Energy 2021 , 6 , 1045−1053..

He, H.; Li, X.; Zhang, J.; Chen, Z.; Gong, Y.; Zhuo, H.; Wu, X.; Li, Y.; Wang, S.; Bi, Z.; Song, B.; Zhou, K.; Liang, T.; Ma, W.; Lu, G.; Ye, L.; Meng, L.; Zhang, B.; Li, Y.; Li, Y. Dynamic hydrogen-bonding enables high-performance and mechanically robust organic solar cells processed with non-halogenated solvent. Nat. Commun. 2025 , 16 , 787..

Song, J.; Zhang, C.; Li, C.; Qiao, J.; Yu, J.; Gao, J.; Wang, X.; Hao, X.; Tang, Z.; Lu, G.; Yang, R.; Yan, H.; Sun, Y. Non-halogenated solvent-processed organic solar cells with approaching 20 % efficiency and improved photostability. Angew. Chem. Int. Ed. 2024 , 63 , e202404297..

Wang, H.; Liu, S.; Li, H.; Li, M.; Wu, X.; Zhang, S.; Ye, L.; Hu, X.; Chen, Y. Green printing for scalable organic photovoltaic modules by controlling the gradient Marangoni flow. Adv. Mater. 2024 , 36 , 2313098..

Machui, F.; Lucera, L.; Spyropoulos, G. D.; Cordero, J.; Ali, A. S.; Kubis, P.; Ameri, T.; Voigt, M. M.; Brabec, C. J. Large area slot-die coated organic solarcells on flexible substrates with non-halogenated solution formulations. Sol. Energy Mater. Sol. Cells 2014 , 128 , 441−446..

Zhao, H.; Naveed, H. B.; Lin, B.; Zhou, X.; Yuan, J.; Zhou, K.; Wu, H.; Guo, R.; Scheel, M. A.; Chumakov, A.; Roth, S. V.; Tang, Z.; Müller-Buschbaum, P.; Ma, W. Hot hydrocarbon-solvent slot-die coating enables high-efficiency organic solar cells with temperature-dependent aggregation behavior. Adv. Mater. 2020 , 32 , 2002302..

Zhang, L.; Zhang, J.; Ma, Y.; Guo, X.; Huang, H.; Bi, Z.; Wang, Y.; Zhang, Y.; Xie, C.; Luo, W.; Hu, X.; Ma, W.; Yuan, Y. Improving efficiency and flexibility of non-halogenated solvent-processed dual-layer organic solar cells through solvent vapor annealing. Org. Electron. 2024 , 130 , 107075..

Song, J.; Li, Y.; Cai, Y.; Zhang, R.; Wang, S.; Xin, J.; Han, L.; Wei, D.; Ma, W.; Gao, F.; Sun, Y. Solid additive engineering enables high-efficiency and eco-friendly all-polymer solar cells. Matter 2022 , 5 , 4047−4059..

Liang, Q.; Li, H.; Xu, W.; Lu, J.; Ma, R.; Bai, Q.; Sun, X.; Chen, M.; Zhu, L.; Liu, Q.; Guo, Y.; Zhang, G.; Xue, Q.; Iwan, A.; Cheng, P.; Hu, H.; Wang, H.; Chen, J.; Niu, L.; Sun, H. Dual-asymmetric solid additive enables eco-friendly all-polymer solar cells with over 19% efficiency and excellent stability. Angew. Chem. Int. Ed. 2025 , 64 , e202425267..

Dahiya, H.; Kumar, D.; Sharma, G. D.; Karak, S. The emerging role of solid additives in advancing stability and performance of organic solar cells. Energy Technol. 2026 , 14 , e202502517..

Xu, X.; Yu, L.; Yan, H.; Li, R.; Peng, Q. Highly efficient non-fullerene organic solar cells enabled by a delayed processing method using a non-halogenated solvent. Energy Environ. Sci. 2020 , 13 , 4381−4388..

Wu, S.; Xu, H.; Wang, H.; Liu, X.; Tu, L.; Zhang, W.; Chen, Y.; Song, X.; Shi, Y. Isomerized dithienopyrazine-based solid additive enables organic solar cells with 20.5% efficiency. Angew. Chem. Int. Ed. 2026 , 65 , e6458866..

Yao, H.; Qian, D.; Zhang, H.; Qin, Y.; Xu, B.; Cui, Y.; Yu, R.; Gao, F.; Hou, J. Critical role of molecular electrostatic potential on charge generation in organic solar cells. Chin. J. Chem. 2018 , 36 , 491−494..

Wang, X.; Wu, J.; Zhao, S.; Chen, M.; Shi, T.; Xie, X.; Bai, Q.; Xie, J.; Zhang, L.; Ma, D.; Chen, J. Elevating dielectric constant via additive en gineering: achieving 19.23% certified efficiency in thick-film binary organic solar cells. Joule 2025 , 9 , 102135..

Li, C.; Zhou, J.; Song, J.; Xu, J.; Zhang, H.; Zhang, X.; Guo, J.; Zhu, L.; Wei, D.; Han, G.; Min, J.; Zhang, Y.; Xie, Z.; Yi, Y.; Yan, H.; Gao, F.; Liu, F.; Sun, Y. Non-fullerene acceptors with branched side chains and improved molecular packing to exceed 18% efficiency in organic solar cells. Nat. Energy 2021 , 6 , 605−613..

Xu, L. Y.; Gao, Y.; Sun, R.; Xing, Z.; Xiao, B.; Yang, X.; Shao, Y.; Chang, B.; Wu, X.; Xiao, B.; Zhang, M.; Min, J. Controlled-disorder asymmetrical donors enable efficient all-small-molecule solar cells with excellent solution-processability. Angew. Chem. Int. Ed. 2026 , 65 , e19713..

Zheng, B.; Yue, Y.; Ni, J.; Zhou, X.; He, Y.; Gui, X.; Shen, H.; Jing, Y.; Zhao, J.; Zhang, J.; Zhang, Y.; Wang, J.; Jiang, L.; Huo, L. An efficient one-arrow-two-hawks strategy achieves high efficiency and stable batch variance for benzodifuran-based polymer solar cells. Adv. Funct. Mater. 2023 , 33 , 2300981..

Song, H.; Yue, Y.; Gui, X.; Sun, S.; Yang, Z.; Zheng, B.; Shen, H.; Wang, J.; Zhang, J.; Huo, L. Strategic engineering of H-/J-aggregation equilibrium in no n-fullerene acceptors toward high-performance organic photovoltaics. Energy Environ. Sci. 2026 , 19 , 1703−1714..

Sun, R.; Wu, Y.; Yang, X.; Gao, Y.; Chen, Z.; Li, K.; Qiao, J.; Wang, T.; Guo, J.; Liu, C.; Hao, X.; Zhu, H.; Min, J. Single-junction organic solar cells with 19.17% efficiency enabled by introducing one asymmetric guest acceptor. Adv. Mater. 2022 , 34 , 2110147..

Jiang, Y.; Sun, S.; Xu, R.; Liu, F.; Miao, X.; Ran, G.; Liu, K.; Yi, Y.; Zhang, W.; Zhu, X. Non-fullerene acceptor with asymmetric structure and phenyl-substituted alkyl side chain for 20.2% efficiency organic solar cells. Nat. Energy 2024 , 9 , 975−986..

Sun, R.; Wu, Q.; Guo, J.; Wang, T.; Wu, Y.; Qiu, B.; Luo, Z.; Yang, W.; Hu, Z.; Guo, J.; Shi, M.; Yang, C.; Huang, F.; Li, Y.; Min, J. A layer-by-layer architecture for printable organic solar cells overcoming the scaling lag of module efficiency. Joule 2020 , 4 , 407−419..

Shao, Y.; Sun, R.; Wang, W.; Yang, X.; Sun, C.; Li, Y.; Min, J. Low-cost organic photovoltaic materials with great application potentials enabled by developing isomerized non-fused ring acceptors. Sci. China Chem. 2023 , 66 , 1101−1110..

Gasparini, N.; Jiao, X.; Heumueller, T.; Baran, D.; Matt, G. J.; Fladischer, S.; Spiecker, E.; Ade, H.; Brabec, C. J.; Ameri, T. Designing ternary blend bulk heterojunction solar cells with reduced carrier recombination and a fill factor of 77%. Nat. Energy 2016 , 1 , 16118..

Kumar, A.; Bansode, U.; Ogale, S.; Rahman, A. Understanding the thermal degradation mechanism of perovskite solar cells via dielectric and noise measurements. Nanotechnology 2020 , 31 , 365403..

Hu, T.; Chen, L.; Miao, W.; Li, C.; Song, J.; Liao, Y.; Liang, J.; Xiong, J.; Wang, X.; Sun, Y.; Yan, H.; Yang, R. Benzothieno [1,2- b ] furan: an atomically symmetric-breaking volatile solid additive for high-performance thick-film planar heterojunction organic solar cells. Sci. China Chem. 2026 , 69 , 1273−1281..

[Sun, R.; Wang, T.; Fan, Q.; Wu, M.; Yang, X.; Wu, X.; Yu, Y.; Xia, X.; Cui, F.; Wan, J.; Lu, X.; Hao, X.; Jen, A. K.; Spiecker, E.; Min, J. 18.2%-efficient ternary all-polymer organic solar cells with improved stability enabled by a chlorinated guest polymer acceptor. Joule 2023 , 7 , 221−237..

Yao, S.; Yang, L.; Shi, S.; Zhou, Y.; Long, M.; Zhang, W.; Cai, S.; Huang, C.; Liu, T.; Zou, B. A two-in-one annealing enables dopant free block copolymer based organic solar cells with over 16% efficiency. Chin. J. Chem. 2023 , 41 , 672−678..

Xu, S.; He, Q.; Xue, X.; Deng, J.; Han, F.; Xie, F.; Jiao, X.; Zhou, L.; Zeng, R.; Wang, Z.; Zhang, M.; Zhu, L.; Jing, H.; Zhang, Y.; Liu, F. Construction of shamrock-shaped giant molecule acceptors for efficient organic solar cells. Angew. Chem. Int. Ed. 2025 , 64 , e202507616..

Chen, Z.; Zhang, S.; Sun, R.; Mei, L.; Yang, W.; Xing, Z.; Yang, X.; Xiao, B.; Wu, X.; Chen,X.; Min, J. Enhanced ε r / L D and improved acceptor crystal growth enable all-polymer solar cells with outstanding efficiency, stability, and processability from a chlorinated-dimer diluent additive. Energy Environ. Sci. 2026 , 19 , 946−957..

Wei, L.; Zhan, L.; Yang, Y.; Chen, T.; Yu, J.; Sun, X.; Hu, H.; Sun, R.; Min, J.; Li, Y.; Wu, J.; Che, J.; Zhang, G.; Zhang, J.; Li, Y.; Yin, S.; Chen, H. Precise morphology control via backbone-derived solid additive enables binary organic solar cells to achieve 20% efficiency and thick-film compatibility. Adv. Mater. 2026 , 38 , e18516..

Sun, R.; Wang, T.; Yang, X.; Wu, Y.; Wang, Y.; Wu, Q.; Zhang, M.; Brabec, C. J.; Li, Y.; Min, J. High-speed sequential deposition of photoactive layers for organic solar cell manufacturing. Nat. Energy 2022 , 7 , 1087−1099..

Shao, Y.; Gao, Y.; Sun, R.; Yang, X.; Zhang, M.; Liu, S.; Min, J. A high-performance organic photovoltaic system with versatile solution processability. Adv. Mater. 2024 , 36 , 2406329..

Dong, S.; Jia, T.; Zhang, K.; Jing, J.; Huang, F. Single-component non-halogen solvent-processed high-performance organic solar cell module with efficiency over 14%. Joule 2020 , 4 , 2004−2016..

浏览量

下载量

CSCD

文章被引用时，请邮件提醒。

提交

工具集

关联资源

Simultaneous In situ GIWAXS/GISAXS/UV-Vis Reveals the Multiscale Film-formation Kinetics of Blade-coated Organic Photovoltaic Active Layers

Chalcogen Atom Engineering of Conjugated Side Chains Enables Additive-free Organic Solar Cells with 20.58% Efficiency

Cyano-functionalized Halogenated Benzene Additives for Efficient and Stable Organic Solar Cells

An Efficient Catalytic System for Room-temperature Stille Polymerization

Modulating Molecular Electrostatic Potential Unlocks Efficient Exciton Dissociation in A-D-A-type Narrow Bandgap Acceptors-based Organic Solar Cells