An enthalpy–entropy competition strategy enables moisture-stable and scalable perovskite photovoltaics – nature.com

Thank you for visiting nature.com. You are using a browser version with limited support for CSS. To obtain the best experience, we recommend you use a more up to date browser (or turn off compatibility mode in Internet Explorer). In the meantime, to ensure continued support, we are displaying the site without styles and JavaScript.
Advertisement
Nature Synthesis (2026)
123 Accesses
2 Altmetric
Metrics details
Scalable fabrication of perovskite solar modules is hindered by processing inconsistencies and moisture-induced degradation. Although classic coordination solvents form thermodynamically stable intermediate phases with lead iodide (PbI2) under inert gas atmospheres, they are highly hygroscopic in ambient conditions. Moreover, due to minimal entropy change, this phase is difficult to remove during annealing, leading to micropores and unwanted phases. Here we introduce an enthalpy–entropy competition strategy for scalable, humidity-tolerant perovskite printing, in which dimethyl sulfoxide/N-methylpyrrolidone is replaced by N-butylpyrrolidone. N-butylpyrrolidone forms strong carbonyl–PbI2 coordination at ambient temperatures (enthalpy-driven), yet readily dissociates on heating (entropy-driven), facilitating easier formamidinium iodide embedding and intermediate-phase protection. The strategy yields perovskite solar modules with certified power conversion efficiencies of 23.97% in a 100-cm2 rigid module and 19.71% in a flexible counterpart. Encapsulated devices retain 80% of initial performance after 1,440 hours under the double 85 condition (85 °C, 85% relative humidity), demonstrating outstanding operational durability.
This is a preview of subscription content, access via your institution
Subscribe to this journal
Receive 12 digital issues and online access to articles
$119.00 per year
only $9.92 per issue
Buy this article
USD 39.95
Prices may be subject to local taxes which are calculated during checkout
All the data in the paper were derived from our group experiments and are therefore available. These data are published alongside the paper. Source data are provided with this paper.
Best Research-Cell Efficiency Chart. National Laboratory of the Rockies https://www.nlr.gov/pv/cell-efficiency (2026).
Li, S. et al. High-efficiency and thermally stable FACsPbI3 perovskite photovoltaics. Nature 635, 82–88 (2024).
Article  CAS  PubMed  Google Scholar 
Cai, Q. et al. Enhancing electron transport for efficiency-recorded HTL-free inverted perovskite solar cells by molecular complementary passivation. Joule 9, 101880 (2025).
Article  CAS  Google Scholar 
Luo, C. et al. Engineering bonding sites enables uniform and robust self-assembled monolayer for stable perovskite solar cells. Nat. Mater. 24, 1265–1272 (2025).
Article  CAS  PubMed  Google Scholar 
Liu, D. et al. Strain relaxation in halide perovskites via 2D/3D perovskite heterojunction formation. Sci. Adv. 11, eadu3459 (2025).
Article  CAS  PubMed  PubMed Central  Google Scholar 
Li, J. et al. Homogeneous coverage of the low-dimensional perovskite passivation layer for formamidinium-caesium perovskite solar modules. Nat. Energy 9, 1540–1550 (2024).
Article  CAS  Google Scholar 
Chu, Z. et al. Synergistic macroscopic-microscopic regulation: dual constraints of the island effect and coffee-ring effect in printing efficient flexible perovskite photovoltaics. Adv. Funct. Mater. 35, 2424191 (2025).
Article  CAS  Google Scholar 
Fan, B. et al. A bionic interface to suppress the coffee-ring effect for reliable and flexible perovskite modules with a near-90% yield rate. Adv. Mater. 34, 2201840 (2022).
Article  CAS  Google Scholar 
Zhao, X. et al. Operationally stable perovskite solar modules enabled by vapor-phase fluoride treatment. Science 385, 433–438 (2024).
Article  CAS  PubMed  Google Scholar 
Li, D. et al. Selection of functional spacer cations for efficient 2D/3D perovskite solar cells. CCS Chem. 5, 781–801 (2023).
Article  CAS  Google Scholar 
Xu, Y. et al. Printable oil-NiOX hole transport layer enables efficient n-i-p perovskite solar cells with a high thermal stability. Sci. China Chem. 67, 2335–2340 (2024).
Article  CAS  Google Scholar 
Wang, H. et al. Impurity-healing interface engineering for efficient perovskite submodules. Nature 634, 1091–1095 (2024).
Article  CAS  PubMed  Google Scholar 
Xing, Z. et al. Multi-environment phase stabilization by lattice reinforcement for efficient perovskite solar cells. Sci. China Mater. 66, 2573–2581 (2023).
Article  CAS  Google Scholar 
Yan, K. et al. Hybrid halide perovskite solar cell precursors: colloidal chemistry and coordination engineering behind device processing for high efficiency. J. Am. Chem. Soc. 137, 4460–4468 (2015).
Article  CAS  PubMed  Google Scholar 
Yaghoobi Nia, N. et al. Solution-based heteroepitaxial growth of stable mixed cation/anion hybrid perovskite thin film under ambient condition via a scalable crystal engineering approach. Nano Energy 69, 104441 (2020).
Article  CAS  Google Scholar 
Bu, T. et al. Lead halide-templated crystallization of methylamine-free perovskite for efficient photovoltaic modules. Science 372, 1327–1332 (2021).
Article  CAS  PubMed  Google Scholar 
Zou, Y. et al. A crystal capping layer for formation of black-phase FAPbI3 perovskite in humid air. Science 385, 161–167 (2024).
Article  CAS  PubMed  Google Scholar 
Wang, L. et al. A Eu3+-Eu2+ ion redox shuttle imparts operational durability to Pb-I perovskite solar cells. Science 363, 265–270 (2019).
Article  CAS  PubMed  Google Scholar 
Steele, J. A. et al. Direct laser writing of δ- to α-phase transformation in formamidinium lead iodide. ACS Nano 11, 8072–8083 (2017).
Article  CAS  PubMed  PubMed Central  Google Scholar 
Hidalgo, J. et al. Synergistic role of water and oxygen leads to degradation in formamidinium-based halide perovskites. J. Am. Chem. Soc. 145, 24549–24557 (2023).
CAS  PubMed  PubMed Central  Google Scholar 
Kim, H. et al. Optimal interfacial engineering with different length of alkylammonium halide for efficient and stable perovskite solar cells. Adv. Energy Mater. 9, 1902740 (2019).
Article  CAS  Google Scholar 
Chen, L. et al. Intrinsic phase stability and inherent bandgap of formamidinium lead triiodide perovskite single crystals. Angew. Chem. Int. Ed. 134, e202212700 (2022).
Article  Google Scholar 
Feng, W. et al. Near-stoichiometric and homogenized perovskite films for solar cells with minimized performance variation. Angew. Chem. Int. Ed. 135, e202300265 (2023).
Article  Google Scholar 
Yan, L. et al. Fabrication of perovskite solar cells in ambient air by blocking perovskite hydration with guanabenz acetate salt. Nat. Energy 8, 1158–1167 (2023).
Article  CAS  Google Scholar 
Wan, Z. et al. Efficient perovskite solar modules with an ultra-long processing window enabled by cooling stabilized intermediate phases. Energy Environ. Sci. 17, 6302–6313 (2024).
Article  CAS  Google Scholar 
Liu, P. et al. Ambient scalable fabrication of high-performance flexible perovskite solar cells. Energy Environ. Sci. 17, 7069–7080 (2024).
Article  CAS  Google Scholar 
Jeon, N. J. et al. Solvent engineering for high-performance inorganic-organic hybrid perovskite solar cells. Nat. Mater. 13, 897–903 (2014).
Article  CAS  PubMed  Google Scholar 
Chao, L. et al. Solvent engineering of the precursor solution toward large-area production of perovskite solar cells. Adv. Mater. 33, 2005410 (2021).
Article  CAS  Google Scholar 
Duan, C. et al. Scalable fabrication of wide-bandgap perovskites using green solvents for tandem solar cells. Nat. Energy 10, 318–328 (2024).
Article  Google Scholar 
Wang, Y. et al. Solvent-assisted reaction for spontaneous defect passivation in perovskite solar cells. Nat. Photonics 19, 985–991 (2025).
Article  CAS  Google Scholar 
Meng, H. et al. Inhibition of halide oxidation and deprotonation of organic cations with dimethylammonium formate for air-processed p–i–n perovskite solar cells. Nat. Energy 9, 536–547 (2024).
Article  CAS  Google Scholar 
Qin, M. et al. Manipulating the mixed-perovskite crystallization pathway unveiled by in situ GIWAXS. Adv. Mater. 31, 1901284 (2019).
Article  Google Scholar 
Ma, C. et al. Unveiling facet-dependent degradation and facet engineering for stable perovskite solar cells. Science 379, 173–178 (2023).
Article  CAS  PubMed  Google Scholar 
Li, S. et al. Coherent growth of high-miller-index facets enhances perovskite solar cells. Nature 635, 874–881 (2024).
Article  PubMed  Google Scholar 
Li, H. et al. Optimizing the crystallization behavior and film morphology of donor–acceptor conjugated semiconducting polymers by side-chain–solvent interaction in nonpolar solvents. Macromolecules 54, 10557–10573 (2021).
Article  CAS  Google Scholar 
Gao, W. et al. Efficient all-small-molecule organic solar cells processed with non-halogen solvent. Nat. Commun. 15, 1946 (2024).
Article  CAS  PubMed  PubMed Central  Google Scholar 
Ma, R. et al. In-situ understanding on the formation of fibrillar morphology in green solvent processed all-polymer solar cells. Natl Sci. Rev. 11, nwae384 (2024).
Article  CAS  PubMed  PubMed Central  Google Scholar 
Liu, H. et al. Simultaneous mechanical and chemical synthesis of long-range-ordered perovskites. Nat. Synth. 4, 196–208 (2025).
Article  Google Scholar 
Han, C. et al. Program-modulated kinetics of perovskite-film growth by molecular ‘thruster’ for high-efficiency and stable perovskite solar cells. Angew. Chem. Int. Ed. 64, e202419726 (2025).
Article  CAS  Google Scholar 
Tong, J. et al. Carrier control in Sn-Pb perovskites via 2D cation engineering for all-perovskite tandem solar cells with improved efficiency and stability. Nat. Energy 7, 642–651 (2022).
Article  CAS  Google Scholar 
Stolterfoht, M. et al. Visualization and suppression of interfacial recombination for high-efficiency large-area pin perovskite solar cells. Nat. Energy 3, 847–854 (2018).
Article  CAS  Google Scholar 
Li, B. et al. Fundamental understanding of stability for halide perovskite photovoltaics: the importance of interfaces. Chem 10, 35–47 (2024).
Article  CAS  Google Scholar 
Zhan, L. et al. Anchorable polymers enabling ultra-thin and robust hole-transporting layers for high-efficiency inverted perovskite solar cells. Angew. Chem. Int. Ed. 137, e202422571 (2025).
Article  Google Scholar 
Download references
A portion of this work is based on the data obtained at Beijing Synchrotron Radiation Facility (BSRF) and SSRF. We thank the 1W1A-Diffuse X-ray Scattering Beamline of BSRF (https://cstr.cn/31109.02.BSRF.1W1A) and BL16B1, BL02U2 and BL03HB of SSRF for providing technical support and assistance in GIWAXS data collection.
We thank the following for support: National Key Research and Development Program of China (grant nos. 2024YFF1401100 and 2024YFB3815200), the National Natural Science Foundation of China (NSFC) (grant nos. 52527804, 52573277, 52403323 and 22461142139), the Natural Science Foundation of Jiangxi Province (grant no. 20242BAB24002), Hebei Province Central Guidance Fund for Local Science and Technology Development (grant no. 254Z4301G), Nanchang University Interdisciplinary Research Funding Program (grant no. 202505300006), Shenzhen Science and Technology Program (grant no. JCYJ20241202124937050) and the State Key Laboratory for Mechanical Behavior of Materials.
These authors contributed equally: Zhaoyang Chu, Junliang Li, Jiaju Gao.
College of Chemistry and Chemical Engineering, Film Energy Chemistry for Jiangxi Provincial Key Laboratory, Institute of Polymers and Energy Chemistry, Nanchang University, Nanchang, China
Zhaoyang Chu, Junliang Li, Jiaju Gao, Sihao Li, Zongyi Gu, Yihuan Xie, Yaling Luo, Xiangchuan Meng, Xiaotian Hu & Yiwang Chen
College of Chemistry and Chemical Engineering, Key Laboratory of Fluorine and Silicon for Energy Materials and Chemistry of Ministry of Education, Jiangxi Normal University, Nanchang, China
Baojin Fan & Yiwang Chen
College of Chemistry and Materials, Gannan Normal University, Ganzhou, China
Zhi Xing & Yiwang Chen
College of Materials and Energy, Guang’an Institute of Technology, Guang’an, China
Hongxiang Li
Key Laboratory for Advanced Optoelectronic Integrated Chips of Jiangsu Province, Peking University Yangtze Delta Institute of Optoelectronics, Nantong, China
Xiaotian Hu & Yiwang Chen
PubMed Google Scholar
PubMed Google Scholar
PubMed Google Scholar
PubMed Google Scholar
PubMed Google Scholar
PubMed Google Scholar
PubMed Google Scholar
PubMed Google Scholar
PubMed Google Scholar
PubMed Google Scholar
PubMed Google Scholar
PubMed Google Scholar
PubMed Google Scholar
X.H. and Y.C. directed and supervised the project. Z.C. and X.H. conceived of and designed the experiments. Z.C. and X.H. completed the writing of the paper. Z.C., J.L., Y.X., Z.G. and J.G. fabricated the PSMs. Z.C., S.L., B.F. and Y.L. fabricated the PSCs. Z.C., J.L., J.G. and H.L. characterized the GIWAXS. Z.C., Z.X., Z.G. and X.M. characterized the various photoelectric properties. All authors contributed to discussions and finalizing the paper.
Correspondence to Xiaotian Hu or Yiwang Chen.
The authors declare no competing interests.
Nature Synthesis thanks Yonghua Chen, Jingrui Li and the other, anonymous, reviewer(s) for their contribution to the peer review of this work. Primary Handling Editor: Alexandra Groves, in collaboration with the Nature Synthesis team.
Publisher’s note Springer Nature remains neutral with regard to jurisdictional claims in published maps and institutional affiliations.
Supplementary Text, Figs. 1–32, Tables 1–8 and references.
Statistical source data for Supplementary Figs. 1, 2, 5–7, 12, 14–17, 20–26, 29, 30 and 32.
Statistical source data.
Statistical source data.
Statistical source data.
Statistical source data.
Springer Nature or its licensor (e.g. a society or other partner) holds exclusive rights to this article under a publishing agreement with the author(s) or other rightsholder(s); author self-archiving of the accepted manuscript version of this article is solely governed by the terms of such publishing agreement and applicable law.
Reprints and permissions
Chu, Z., Li, J., Gao, J. et al. An enthalpy–entropy competition strategy enables moisture-stable and scalable perovskite photovoltaics. Nat. Synth (2026). https://doi.org/10.1038/s44160-026-01142-0
Download citation
Received:
Accepted:
Published:
Version of record:
DOI: https://doi.org/10.1038/s44160-026-01142-0
Anyone you share the following link with will be able to read this content:
Sorry, a shareable link is not currently available for this article.

Provided by the Springer Nature SharedIt content-sharing initiative
Advertisement
Nature Synthesis (Nat. Synth)
ISSN 2731-0582 (online)
© 2026 Springer Nature Limited
Sign up for the Nature Briefing newsletter — what matters in science, free to your inbox daily.

source

This entry was posted in Renewables. Bookmark the permalink.

Leave a Reply