Electrohydrodynamic-Mediated Molecular Coordination for Stabilizing α-Phase Perovskite Solar Cells
Abstract Formamidinium-rich perovskite solar cells (PSCs) have achieved remarkable efficiencies, yet their phase purity is often compromised by the competitive nucleation of the nonperovskite δ-phase during rapid processing. Herein, we demonstrate an electrohydrodynamic (EHD)-mediated chemical strategy to bypass this kinetic trap using a multifunctional molecular, tetramethylthiourea (TeMTU). By precision tuning of the surface tension-Coulombic repulsion balance, TeMTU orchestrates the EHD-driven microdroplet evolution, effectively locking the in-flight precursor into a critically supersaturated state that fundamentally suppresses δ-phase nucleation. Beyond macroscopic fluid dynamics, molecular-level investigations reveal that TeMTU forms robust coordination complexes with the lead halide framework. This chemical intervention significantly elevates the activation energy barrier for the α-to-δ phase transition by 42%, as corroborated by Density Functional Theory and variable-cell double-ended surface walking analysis. The resulting α-phase FA-based films exhibit exceptional crystallinity and a minimized defect density, enabling electrospray-fabricated PSCs to achieve an impressive power conversion efficiency (PCE) of 26.24% (0.05 cm2) and 25.39% (1.0 cm2). Furthermore, the chemically stabilized lattice demonstrates operational durability, retaining 95% of its initial PCE after 3000 h of continuous maximum power point tracking at 65 °C.
Authors
- Chunnian He (ORCID: https://orcid.org/0000-0002-5768-6598)
- Xin Meng (ORCID: https://orcid.org/0000-0003-2228-0587)
- Yi Hou (ORCID: https://orcid.org/0000-0002-1532-816X)
- Zijing Dong (ORCID: https://orcid.org/0000-0001-5255-4441)
- Nengxu Li (ORCID: https://orcid.org/0000-0003-2430-8037)
- Zhuojie Shi (ORCID: https://orcid.org/0009-0006-1897-4585)
- Julian A. Steele (ORCID: https://orcid.org/0000-0001-7982-4413)
- Xianchang Yan
- Wan‐Jian Yin (ORCID: https://orcid.org/0000-0003-0932-2789)
- Yuduan Wang
- Zihao Zhu (ORCID: https://orcid.org/0000-0001-7793-3026)
- Zhenxiang Xing (ORCID: https://orcid.org/0009-0008-9779-210X)
- Eduardo Solano (ORCID: https://orcid.org/0000-0002-2348-2271)
- Xinyi Du (ORCID: https://orcid.org/0000-0002-5284-928X)
- Yoshiki Sugai
- Ling Kai Lee (ORCID: https://orcid.org/0009-0000-0463-6952)
- Jinxi Chen (ORCID: https://orcid.org/0000-0002-9531-9705)
- Rong Ji (ORCID: https://orcid.org/0000-0001-7245-9660)
- Yuzhong Chen (ORCID: https://orcid.org/0000-0001-7408-2684)
- Chao Luo (ORCID: https://orcid.org/0009-0001-5162-7992)
- Junxue Liu (ORCID: https://orcid.org/0000-0001-8349-1017)
- Ran Luo (ORCID: https://orcid.org/0009-0000-7967-6545)
- Yuhui Jiang
- Xi Wang
- Xiuxiu Niu
- Zhouyin Wei
- Xinyu Zhang
- Tao Wang
- Xiaohu Zhou
Institutions
- Tianjin University (CN)
- The University of Queensland (AU)
- National University of Singapore (SG)
- Soochow University (TW)
- ALBA Synchrotron (Spain) (ES)
- Hefei University (CN)
- Star Technology and Research (United States) (US)
- Hefei National Center for Physical Sciences at Nanoscale (CN)
- Spectra Research (United States) (US)
- Florida International University Tianjin Center (CN)
- Zhejiang University (CN)
Publication Details
- Journal
- Journal of the American Chemical Society
- Published
- 2026-09-24
- DOI
- https://doi.org/10.1021/jacs.6c05442
- Primary Topic
- Perovskite Materials and Applications
- Type
- article
- Field-Weighted Citation Impact
- 0.00