Interpretation of Rubidium‐Based Perovskite Recipes toward Electronic Passivation and Ion‐Diffusion Mitigation
Interpretation of Rubidium‐Based Perovskite Recipes toward Electronic Passivation and Ion‐Diffusion Mitigation
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DOI：
10.1002/adma.202109998
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发表时间：
2022-02
影响因子：
29.4
通讯作者：
Chenzhe Xu;Xiwen Chen;Shokrgozar Ma;Mingyue Shi;Suicai Zhang;Zhaozhao Xiong;Wenqiang Fan;Haonan Si;Hualin Wu;Zheng Zhang;Qingliang Liao;Wanjian Yin;Z. Kang;Yue Zhang
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文献类型：
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作者：
Chenzhe Xu;Xiwen Chen;Shokrgozar Ma;Mingyue Shi;Suicai Zhang;Zhaozhao Xiong;Wenqiang Fan;Haonan Si;Hualin Wu;Zheng Zhang;Qingliang Liao;Wanjian Yin;Z. Kang;Yue Zhang
在有机-无机复合钙钛矿型太阳能电池中，Rb+离子的加入对提高电池的综合性能起着至关重要的作用。然而，这种成功源于RB+带来的不可替代的优势的来源仍然含糊不清。本文采用含晶界原子模型，对钙钛矿结构中Rb+的实际分布进行了精确的理论分析。利用基于同步加速器的掠入射X射线衍射仪，彻底确定了晶界和晶内的空间分布。在此基础上，阐述了卤素空位形成能的显著提高、载流子动力学的改善以及颗粒内部的电子钝化机理。通过增加能垒和抑制微电流，阐明了Rb+的加入在阻止晶界扩散途径、抑制卤化物相偏析以及最终提高本征稳定性方面的关键作用。因此，本文详细研究了Rb+离子浓度细微变化主导的占位效应对电子缺陷、离子迁移和相稳定性的影响，为高效级联策略和钙钛矿型复合工程的发展提供了新的思路。
Rubidium cation (Rb+) addition is witnessed to play a pivotal role in boosting the comprehensive performance of organic–inorganic hybrid perovskite solar cells. However, the origin of such success derived from irreplaceable superiorities brought by Rb+ remains ambiguous. Herein, grain‐boundary‐including atomic models are adopted for the accurate theoretical analysis of practical Rb+ distribution in perovskite structures. The spatial distribution, covering both the grain interiors and boundaries, is thoroughly identified by virtue of synchrotron‐based grazing‐incidence X‐ray diffraction. On this basis, the prominent elevation of the halogen vacancy formation energy, improved charge‐carrier dynamics, and the electronic passivation mechanism in the grain interior are expounded. As evidenced by the increased energy barrier and suppressed microcurrent, the critical role of Rb+ addition in blocking the diffusion pathway along grain boundaries, inhibiting halide phase segregation, and eventually enhancing intrinsic stability is elucidated. Hence, the linkage avalanche effect of occupied location dominated by subtle changes in Rb+ concentration on electronic defects, ion migration, and phase stability is completely investigated in detail, shedding a new light on the advancement of high‐efficiency cascade‐incorporating strategies and perovskite compositional engineering.