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Unveiling Solvent-Related Effect on Phase Transformations in CsBr–PbBr2 System: Coordination and Ratio of Precursors
Chemistry of Materials ( IF 7.2 ) Pub Date : 2018-08-16 00:00:00 , DOI: 10.1021/acs.chemmater.8b00537
Mei Liu 1 , Jiangtao Zhao 2 , Zhenlin Luo 2 , Zhihu Sun 2 , Nan Pan 1 , Huaiyi Ding 1 , Xiaoping Wang 1
Chemistry of Materials ( IF 7.2 ) Pub Date : 2018-08-16 00:00:00 , DOI: 10.1021/acs.chemmater.8b00537
Mei Liu 1 , Jiangtao Zhao 2 , Zhenlin Luo 2 , Zhihu Sun 2 , Nan Pan 1 , Huaiyi Ding 1 , Xiaoping Wang 1
Affiliation
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All-inorganic cesium lead halide perovskite nanocrystals have emerged as attractive optoelectronic nanomaterials owing to their stabilities and highly efficient photoluminescence. However, the inorganic perovskites of CsPbBr3 synthesized by the solution method often suffer from byproducts such as Cs4PbBr6 and CsPb2Br5. Herein, we have investigated thoroughly the solvent-related effect on the phase formation in CsBr–PbBr2 system through single crystal X-ray diffraction measurement. It is found that the prepared product is dominantly determined by the coordination number (CN) of Pb(II) and the ratio of precursors. By use of dimethyl sulfoxide (DMSO) or dimethylformamide (DMF) as the solvent, Pb2+ is found to be surrounded by six-coordination sites, and the products can be tuned from CsPbBr3 to Cs4PbBr6 by increasing the precursor ratio of CsBr to PbBr2. On the contrary, in the solvent of water, only Pb2+ eight-coordinated crystal of CsPb2Br5 can be produced, regardless of the ratio of CsBr to PbBr2. More importantly, with the investigation of the extended X-ray absorption fine structure (EXAFS) for Pb L-II edge in precursor solutions, we identify that the CNs of Pb(II) of resultants are the same as those of the corresponding plumbite oligomers in precursor solutions. In addition, the phase transitions from Cs4PbBr6 to CsPbBr3, amorphous state, and CsPb2Br5 triggered by water vapor have also been observed clearly. This work not only enriches our understanding of the phase formation of CsBr–PbBr2 system but also provides the knowledge of the degradation of halide perovskites in the environment of humidity.
中文翻译：
在CsBr–PbBr 2体系中揭示与溶剂相关的相变效应：前驱体的配位和比例
全无机卤化铯铅钙钛矿纳米晶体由于其稳定性和高效的光致发光而成为有吸引力的光电纳米材料。然而，通过溶液法合成的CsPbBr 3的无机钙钛矿经常遭受诸如Cs 4 PbBr 6和CsPb 2 Br 5的副产物的困扰。在此，我们已经彻底研究了溶剂相关的影响对CsBr–PbBr 2中相形成的影响系统通过单晶X射线衍射测量。发现所制备的产物主要由Pb（II）的配位数（CN）和前体的比例决定。通过使用二甲基亚砜（DMSO）或二甲基甲酰胺（DMF）作为溶剂，发现Pb 2+被六个配位位点包围，并且可以通过增加前体比例将产物从CsPbBr 3调谐到Cs 4 PbBr 6。从CsBr到PbBr 2。相反，在水的溶剂中，无论CsBr与PbBr 2的比例如何，都只能生成CsPb 2 Br 5的Pb 2+八配位晶体。。更重要的是，通过对前体溶液中Pb L-II边缘的扩展X射线吸收精细结构（EXAFS）的研究，我们确定了所得物Pb（II）的CNs与相应的铅咬低聚物的CNs相同。在前体溶液中。另外，还清楚地观察到了由水蒸气触发的从Cs 4 PbBr 6到CsPbBr 3的相变，非晶态和CsPb 2 Br 5。这项工作不仅丰富了我们对CsBr–PbBr 2体系形成的理解，而且提供了在潮湿环境中卤化钙钛矿降解的知识。
更新日期：2018-08-16
中文翻译：
在CsBr–PbBr 2体系中揭示与溶剂相关的相变效应：前驱体的配位和比例
全无机卤化铯铅钙钛矿纳米晶体由于其稳定性和高效的光致发光而成为有吸引力的光电纳米材料。然而，通过溶液法合成的CsPbBr 3的无机钙钛矿经常遭受诸如Cs 4 PbBr 6和CsPb 2 Br 5的副产物的困扰。在此，我们已经彻底研究了溶剂相关的影响对CsBr–PbBr 2中相形成的影响系统通过单晶X射线衍射测量。发现所制备的产物主要由Pb（II）的配位数（CN）和前体的比例决定。通过使用二甲基亚砜（DMSO）或二甲基甲酰胺（DMF）作为溶剂，发现Pb 2+被六个配位位点包围，并且可以通过增加前体比例将产物从CsPbBr 3调谐到Cs 4 PbBr 6。从CsBr到PbBr 2。相反，在水的溶剂中，无论CsBr与PbBr 2的比例如何，都只能生成CsPb 2 Br 5的Pb 2+八配位晶体。。更重要的是，通过对前体溶液中Pb L-II边缘的扩展X射线吸收精细结构（EXAFS）的研究，我们确定了所得物Pb（II）的CNs与相应的铅咬低聚物的CNs相同。在前体溶液中。另外，还清楚地观察到了由水蒸气触发的从Cs 4 PbBr 6到CsPbBr 3的相变，非晶态和CsPb 2 Br 5。这项工作不仅丰富了我们对CsBr–PbBr 2体系形成的理解，而且提供了在潮湿环境中卤化钙钛矿降解的知识。
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