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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Kang Wang, Changji Gao, Zhuo Xu, Qingwen Tian,* Xiaojing Gu, Lu Zhang,
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Zicheng Ding, Dongle Liu, Kui Zhao,* and Yanchun Han*, Macromolecules , 2021, 54, 9, 3907–3926.
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Editorial: Organic Semiconductors: Investigating the Processing-Structure-Property Relationships
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Lead-free molecular one-dimensional perovskite for efficient X-ray detection
Haojin Li, Xin Song, Chuang Ma, Zhuo Xu, Nuo Bu, Tinghuan Yang, Qingyue Cui, Lili Gao, Zhou Yang, Fei Gao, Guangtao Zhao, Zhaolai Chen, Zicheng Ding*, Kui Zhao*, Shengzhong (Frank) Liu, 2022, 64(1): 209-213.
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Junjie Fang, Zicheng Ding,* Xiaoming Chang, Jing Lu, Tinghuan Yang, Jialun Wen, Yuanyuan Fan, Yalan Zhang, Tao Luo, Yonghua Chen,* Shengzhong (Frank) Liu* and Kui Zhao*, J. Mater. Chem. A, 2021,9, 13297-13305.
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Film Formation Control for High Performance Dion–Jacobson 2D Perovskite Solar Cells
Xu Zhang, Tinghuan Yang, Xiaodong Ren, Lu Zhang, Kui Zhao,* Shengzhong (Frank) Liu*, Adv. Energy Mater. 2021, 2002733.
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Perovskite Solar Cells toward Eco-Friendly Printing
Xiaoming Chang, Yuanyuan Fan, Kui Zhao,* Junjie Fang, Dongle Liu, Ming-Chun Tang, Dounya Barrit, Detlef-M. Smilgies, Ruipeng Li, Jing Lu, Jianbo Li, Tinghuan Yang, Aram Amassian, Zicheng Ding, Yonghua Chen, Shengzhong (Frank) Liu,* and Wei Huang,* Research, 2021, 9671892.