The Role of Specific Interactions in the Formation of Perovskite Structures

IF 1.204 Q3 Energy Applied Solar Energy Pub Date : 2024-03-05 DOI:10.3103/s0003701x23601746

I. N. Nurgaliev, M. B. Marasulov, N. R. Ashurov

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Abstract

Using methylammonium lead iodide (MAPbI3) as an example, the process of complexation of molecular particles from solution at the initial stage of crystallization was studied using calculations based on the density functional theory (DFT). The calculations were carried out taking into account solvents widely used in experiments: dimethyl sulfoxide (DMSO) and N,N-dimethylformamide (DMF) and N-methyl-2-pyrrolidone (N-MP) to analyze the structure and energy of iodoplumbate complexes in the form of simple complex [PbI_mX_n]² ^{– m} and polymeric iodoplumbates ([PbI_mX_n]² ^{– m})_x. Reaction schemes for the formation of MAPbI₃ in DMSO and DMF solvents, as well as in DMF–DMSO and DMF–N–MP binary solvents, are proposed based on the calculated energies. Calculations showed the important role of NH–O hydrogen bonds in the formation of iodoplumbate monomers, as well as the imbalance of the energies of the complexes at several elementary stages of the reaction in various solvents (the formation of [PbI₄X_n]^2– is favorable; the formation of [PbI₅X_n]^3– is slowed down. Mixing a small amount of DMSO with DMF results in a better energy balance and, therefore, potentially better equilibrium in the overall crystallization process, and thus a better quality of the perovskite crystal structure.

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特定相互作用在形成包晶结构中的作用

摘要以甲基碘化铅铵（MAPbI3）为例，使用基于密度泛函理论（DFT）的计算方法研究了结晶初期分子颗粒从溶液中络合的过程。计算考虑了实验中广泛使用的溶剂：二甲基亚砜（DMSO）、N,N-二甲基甲酰胺（DMF）和 N-甲基-2-吡咯烷酮（N-MP），分析了简单复合物 [PbImXn]2 - m 和聚合碘铂酸盐（[PbImXn]2 - m）x 形式的碘铂酸盐复合物的结构和能量。根据计算得出的能量，提出了在 DMSO 和 DMF 溶剂中，以及在 DMF-DMSO 和 DMF-N-MP 二元溶剂中形成 MAPbI3 的反应方案。计算结果表明，NH-O 氢键在碘铂酸盐单体的形成过程中起着重要作用，而且在各种溶剂中，复合物在反应的几个基本阶段的能量不平衡（[PbI4Xn]2- 的形成有利；[PbI5Xn]3- 的形成缓慢。将少量二甲基亚砜与 DMF 混合会导致更好的能量平衡，因此，整个结晶过程可能会达到更好的平衡，从而提高包晶晶体结构的质量。

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来源期刊

Applied Solar Energy Energy-Renewable Energy, Sustainability and the Environment

CiteScore

2.50

自引率

0.00%

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期刊介绍： Applied Solar Energy is an international peer reviewed journal covers various topics of research and development studies on solar energy conversion and use: photovoltaics, thermophotovoltaics, water heaters, passive solar heating systems, drying of agricultural production, water desalination, solar radiation condensers, operation of Big Solar Oven, combined use of solar energy and traditional energy sources, new semiconductors for solar cells and thermophotovoltaic system photocells, engines for autonomous solar stations.