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Vol. 14 (2022)

Resolving Mixed Intermediate Phases in Methylammonium-Free Sn–Pb Alloyed Perovskites for High-Performance Solar Cells

https://doi.org/10.1007/s40820-022-00918-1
Zhanfei Zhang
School of Materials Science and Engineering, Shanghai Jiao Tong University, Shanghai 20024, People’s Republic of China
Jianghu Liang
School of Materials Science and Engineering, Shanghai Jiao Tong University, Shanghai 20024, People’s Republic of China
Jianli Wang
School of Materials Science and Engineering, Shanghai Jiao Tong University, Shanghai 20024, People’s Republic of China
Yiting Zheng
School of Materials Science and Engineering, Shanghai Jiao Tong University, Shanghai 20024, People’s Republic of China
Xueyun Wu
School of Materials Science and Engineering, Shanghai Jiao Tong University, Shanghai 20024, People’s Republic of China
Congcong Tian
School of Materials Science and Engineering, Shanghai Jiao Tong University, Shanghai 20024, People’s Republic of China
Anxin Sun
School of Materials Science and Engineering, Shanghai Jiao Tong University, Shanghai 20024, People’s Republic of China
Zhenhua Chen
Shanghai Synchrotron Radiation Facility (SSRF), Shanghai Advanced Research Institute, Chinese Academy of Sciences, Shanghai 201800, People’s Republic of China
Chun‑Chao Chen
School of Materials Science and Engineering, Shanghai Jiao Tong University, Shanghai 20024, People’s Republic of China

Corresponding Author: Chun‑Chao Chen

c3chen@sjtu.edu.cn

Nano-Micro Letters, Vol. 14 (2022), Article Number: 165

Abstract

The complete elimination of methylammonium (MA) cations in Sn–Pb composites can extend their light and thermal stabilities. Unfortunately, MA-free Sn–Pb alloyed perovskite thin films suffer from wrinkled surfaces and poor crystallization, due to the coexistence of mixed intermediate phases. Here, we report an additive strategy for finely regulating the impurities in the intermediate phase of Cs0.25FA0.75Pb0.6Sn0.4I3 and, thereby, obtaining high-performance solar cells. We introduced d-homoserine lactone hydrochloride (D-HLH) to form hydrogen bonds and strong Pb–O/Sn–O bonds with perovskite precursors, thereby weakening the incomplete complexation effect between polar aprotic solvents (e.g., DMSO) and organic (FAI) or inorganic (CsI, PbI2, and SnI2) components, and balancing their nucleation processes. This treatment completely transformed mixed intermediate phases into pure preformed perovskite nuclei prior to thermal annealing. Besides, this D-HLH substantially inhibited the oxidation of Sn2+ species. This strategy generated a record efficiency of 21.61%, with a Voc of 0.88 V for an MA-free Sn–Pb device, and an efficiency of 23.82% for its tandem device. The unencapsulated devices displayed impressive thermal stability at 85 °C for 300 h and much improved continuous operation stability at MPP for 120 h.


Highlights:


1 The first study dedicated to solving the problem of mixed intermediate phases in methylammonium (MA)-free (FA-Cs) Sn–Pb alloyed perovskite systems, new performance records of 21.61% and 23.82% realized for its single-junction and tandem devices.
2 d-Homoserine lactone hydrochloride (D-HLH), employed as an additive, accelerates the transition from mixed intermediate phases into preformed perovskite nuclei.
3 The presence of D-HLH eliminated the negative effect of mixed intermediate phases and regulated the crystallization kinetics.

Keywords

Intermediate phase Homogeneous nucleation process MA-free tin–lead alloyed perovskite Light and thermal stability Tandem device
Zhang, Zhanfei, Jianghu Liang, Jianli Wang, Yiting Zheng, Xueyun Wu, Congcong Tian, Anxin Sun, Zhenhua Chen, and Chun‑Chao Chen. 2022. “Resolving Mixed Intermediate Phases in Methylammonium-Free Sn–Pb Alloyed Perovskites for High-Performance Solar Cells”. Nano-Micro Letters 14 (August):165. https://doi.org/10.1007/s40820-022-00918-1.
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