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Understanding the Effect of Crystalline Structural Transformation for Lead-Free Inorganic Halide Perovskites.
Advanced Materials ( IF 29.4 ) Pub Date : 2020-06-28 , DOI: 10.1002/adma.202002137
Ming Shi 1, 2 , Guanna Li 3 , Wenming Tian 4 , Shengye Jin 4 , Xiaoping Tao 1 , Yiming Jiang 1, 2 , Evgeny A Pidko 3 , Rengui Li 1 , Can Li 1
Affiliation  

Lead‐free inorganic halide perovskites have triggered appealing interests in various energy‐related applications including solar cells and photocatalysis. However, why perovskite‐structured materials exhibit excellent photoelectric properties and how the unique crystalline structures affect the charge behaviors are still not well elucidated but essentially desired. Herein, taking inorganic halide perovskite Cs3Bi2Br9 as a prototype, the significant derivation process of silver atoms incorporation to induce the structural transformation from Cs3Bi2Br9 to Cs2AgBiBr6, which brings about dramatic differences in photoelectric properties is unraveled. It is demonstrated that the silver incorporation results in the co‐operated orbitals hybridization, which makes the electronic distributions in conduction and valence bands of Cs2AgBiBr6 more dispersible, eliminating the strong localization of electron–hole pairs. As consequences of the electronic structures derivation, exhilarating changes in photoelectric properties like band structure, exciton binding energy, and charge carrier dynamics are verified experimentally and theoretically. Using photocatalytic hydrogen evolution activity under visible light as a typical evaluation, such crystalline structure transformation contributes to a more than 100‐fold enhancement in photocatalytic performances compared with pristine Cs3Bi2Br9, verifying the significant effect of structural derivations on the exhibited performances. The findings will provide evidences for understanding the origin of photoelectric properties for perovskites semiconductors in solar energy conversion.

中文翻译:

了解无铅无机卤化物钙钛矿晶体结构转变的影响。

无铅无机卤化物钙钛矿在各种与能源有关的应用中引起了人们的兴趣,包括太阳能电池和光催化。然而,为什么钙钛矿结构的材料为什么会表现出优异的光电性能,以及独特的晶体结构如何影响电荷行为仍未得到很好的阐明,但实际上是人们所希望的。在此,以无机卤化物钙钛矿Cs 3 Bi 2 Br 9为原型,通过大量引入银原子来诱导从Cs 3 Bi 2 Br 9到Cs 2 AgBiBr 6的结构转变。揭示了在光电性能上带来巨大差异的方法。结果表明,银的掺入导致协同的轨道杂交,这使Cs 2 AgBiBr 6的导带和价带电子分布更加分散,消除了电子-空穴对的强局部化。作为电子结构衍生的结果,通过实验和理论验证了诸如带结构,激子结合能和电荷载流子动力学之类的光电特性的令人振奋的变化。与可见的Cs 3 Bi 2 Br 9相比,使用可见光下的光催化氢析出活性作为典型评估,这种晶体结构转变可将光催化性能提高100倍以上。,验证了结构派生对所展示性能的重大影响。这些发现将为理解钙钛矿半导体在太阳能转换中的光电性质的起源提供证据。
更新日期:2020-08-04
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