Abstract:
Ambient printing of perovskite solar cells (PSCs) faces severe challenges in controlling crystallization under humid conditions, leading to substantial performance losses compared to inertly processed devices. While ligand-assisted coordination is known to modulate crystal growth, a precise understanding of how specific chemical bonds influence crystallization dynamics during ambient printing remains elusive. Herein, we unveil a dual-functionalized bonding (DFB) mechanism enabled by aromatic formamidine ligands that concurrently coordinate with both the inorganic framework and organic cations during ambient printing. The key mechanistic insight lies in the ability of ligands to form simultaneous coordination bonds with [PbI6]4— octahedra and hydrogen bonds with formamidinium ions (FA+), which collectively delay nucleation, suppress the δ-phase formation, and widen the recrystallization window. By incorporating an electron-deficient triazole ring into the ligand backbone, we enhance this bifunctional binding effect, leading to superior crystallization control and defect suppression. The resulting perovskite films exhibit remarkable homogeneity, low trap density, and enhanced carrier diffusion. Consequently, ambient-printed devices achieve champion power conversion efficiencies of 25.57% for 0.09 cm2, 23.98% for 1.04 cm2, and 22.98% in 5 × 5 cm2 mini-modules. The optimized devices retain over 90% of their initial performance after 1,000 h of continuous operation. This work provides a profound mechanistic framework for molecular-level crystallization control in printed photovoltaics
https://doi.org/10.1002/anie.202520159
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Dounya Barrit,* Yalan Zhang, Tinghuan Yang, Ming-Chun Tang, Ruipeng Li, Detlef-M. Smilgies, Shengzhong (Frank) Liu, Thomas D. Anthopoulos,* Aram Amassian,* and Kui Zhao*, Solar RRL.
2020, 00668. -
Editorial: Polymer Solar Cells: Molecular Design and Microstructure Control
Jiangang Liu*, Ergang Wang,* and Kui Zhao,* Frontiers in Chemistry . 2020, 8, 697
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Ultrastable perovskite-zeolite composite enabled by encapsulation and in situ passivation
Peijun Wang; Bolun Wang; Yucheng Liu; Lin Li; Hua Zhao; Yonghua Chen; Jiyang Li; Shengzhong (Frank) Liu*; Kui Zhao*, Angew Chem Int Ed, 2020, 14, 23100-23106.
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Printable CsPbI3 Perovskite Solar Cells with PCE of 19% via an Additive Strategy
Xiaoming Chang, Junjie Fang, Yuanyuan Fan, Tao Luo,1 Hang Su, Yalan Zhang, Jing Lu, Leonidas Tsetseris, Thomas D. Anthopoulos,* Shengzhong (Frank) Liu,* Kui Zhao*, Adv. Mater. 2020, 2001243
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Ming-Chun Tang*, Yuanyuan Fan, Dounya Barrit, Ruipeng Li, Hoang X. Dang, Siyuan Zhang, Timothy Magnanelli, Nhan V. Nguyen, Edwin J. Heilweil, Christina A. Hacker, Detlef-M. Smilgies, Kui Zhao*, Aram Amassian* and Thomas D. Anthopoulos*, Solar RRL 2020, 00272.
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Yucheng Liu, Zhuo Xu, Zhou Yang, Yunxia Zhang, Jian Cui, Yihui He, Haochen Ye, Kui Zhao, Huaming Sun, Rui Lu, Ming Liu, Mercouri G.Kanatzidis, Shengzhong (Frank)Liu,* Matter 2020, 04, 017.
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Ming-Chun Tang‡, Yuanyuan Fan‡, Dounya Barrit, Ruipeng Li, Siyuan Zhang, Timothy Magnanelli, Nhan V. Nguyen, Edwin J. Heilweil, Christina A. Hacker, Detlef-M. Smilgies, Kui Zhao,* Aram Amassian,* and Thomas D. Anthopoulos,* , Solar RRL. 2020, 10.1002.
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Yue Shen,† Yucheng Liu,† Haochen Ye, Yiting Zheng, Qi Wei, Yingdong Xia, Yonghua Chen,* Kui Zhao,* Wei Huang, Shengzhong (Frank) Liu,*, Angew. Chem. Int. Ed. 2020, 59, 14896–14902.
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Ming-Chun Tang,‡ Yuanyuan Fan,‡ Dounya Barrit, Xiaoming Chang, Hoang X. Dang, Ruipeng Li, Kai Wang, Detlef-M. Smilgies, Shengzhong (Frank) Liu, Stefaan De Wolf, Thomas D. Anthopoulos,* Kui Zhao* and Aram Amassian*, J. Mater. Chem. A, 2020, 8, 1095.
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Dounya Barrit, Peirui Cheng, Kasra Darabi, Ming-Chun Tang, Detlef-M. Smilgies, Shengzhong (Frank) Liu, Thomas D. Anthopoulos,* Kui Zhao,* and Aram Amassian*, Adv. Funct. Mater. 2020, 30, 1907442.