4-Phenylthiosemicarbazide Molecular Additive Engineering for Wide-Bandgap Sn Halide Perovskite Solar Cells with a Record Efficiency Over 12.2%,Advanced Energy Materials

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4-Phenylthiosemicarbazide Molecular Additive Engineering for Wide-Bandgap Sn Halide Perovskite Solar Cells with a Record Efficiency Over 12.2%
Advanced Energy Materials ( IF 24.4 ) Pub Date : 2024-04-10 , DOI: 10.1002/aenm.202401188
Padmini Pandey ₁ , SungWon Cho ₂ , Jitendra Bahadur ₁ , Saemon Yoon ₂ , Chang‐Mok Oh ₃ , In‐Wook Hwang ₃ , Hochan Song ₄ , Hyosung Choi ₄ , Shuzi Hayase _{5,

6} , Jung Sang Cho ₇ , Dong‐Won Kang _{1,

2}

Affiliation

The utilization of wide bandgap (WBG) tin halide perovskites (Sn-HPs) offers an environmentally friendly alternative for multi-junction Sn-HP photovoltaics. Nonetheless, rapid crystallization leads to suboptimal film morphology and substantial creation of defect states, which undermine device efficiency. This study introduces 4-Phenylthiosemicarbazide (4PTSC) as an additive to achieve a densely packed Sn-HP film with fewer imperfections. The strong chemical coordination between SnI₂ and the functional groups S═C─N (Sn···S═C─N), NH₂, and phenyl conjugation enhances solution stability and supports the delay of perovskite crystallization through adduct formation. This process yields pinhole-free films with preferred grain growth. 4PTSC acts as a strong coordination complex and a reducing agent to passivate uncoordinated Sn²⁺ and halide ions and reduce the formation of SnI₄, thereby reducing defect formation. The π-conjugated phenyl ring in the 4PTSC facilitates the preferred crystal growth orientation of perovskite grains. Furthermore, the hydrophobic nature of 4PTSC mitigates Sn²⁺ oxidation by repelling moisture, enhancing stability. The open circuit voltage significantly increased from 0.78 to 0.94 V, resulting in achieving the champion efficiency of 12.22% (certified 11.70%), surpassing all previously reported efficiencies for WBG Sn halide perovskite solar cells. Additionally, the unencapsulated 4PTSC-1.0 device maintained outstanding stability over 1200 h under ambient atmospheric conditions.

中文翻译：

宽禁带卤化锡钙钛矿太阳能电池的 4-苯基氨基硫脲分子添加剂工程，效率超过 12.2%，创历史新高

宽带隙 (WBG) 卤化锡钙钛矿 (Sn-HP) 的利用为多结 Sn-HP 光伏发电提供了一种环保的替代方案。尽管如此，快速结晶会导致薄膜形态不理想，并大量产生缺陷态，从而降低器件效率。本研究引入 4-苯基氨基硫脲 (4PTSC) 作为添加剂，以实现缺陷较少的致密 Sn-HP 薄膜。 SnI ₂ 与官能团 S=C─N (Sn···S=C─N)、NH ₂ 和苯基共轭之间的强化学配位增强了溶液稳定性并支持通过加合物形成延迟钙钛矿结晶。该工艺生产出具有良好晶粒生长的无针孔薄膜。 4PTSC作为强配位络合物和还原剂，钝化未配位的Sn ²⁺ 和卤化物离子，减少SnI ₄ 的形成，从而减少缺陷形成。 4PTSC中的π-共轭苯环有利于钙钛矿晶粒的优选晶体生长方向。此外，4PTSC 的疏水性通过排斥水分来减轻 Sn ²⁺ 氧化，从而增强稳定性。开路电压从 0.78 V 显着增加至 0.94 V，实现了 12.22% 的冠军效率（认证为 11.70%），超过了之前报道的所有 WBG 锡卤化物钙钛矿太阳能电池的效率。此外，未封装的 4PTSC-1.0 器件在环境大气条件下可保持 1200 小时以上的出色稳定性。

更新日期：2024-04-10

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