Design Principles of Large Cation Incorporation in Halide Perovskites

被引:7
|
作者
Park, Heesoo [1 ]
Kumar, Syam [2 ]
Chawla, Sanjay [3 ]
El-Mellouhi, Fedwa [1 ]
机构
[1] Hamad Bin Khalifa Univ, Qatar Environm & Energy Res Inst, POB 34110, Doha, Qatar
[2] Inst Technol Sligo, Dept Hlth & Nutr Sci, Ash Lane, Sligo F91 YW50, Ireland
[3] Hamad Bin Khalifa Univ, Qatar Comp Res Inst, POB 34110, Doha, Qatar
来源
MOLECULES | 2021年 / 26卷 / 20期
关键词
halide perovskites; photocatalyst; density functional theory; large cation; fluorinated cation; octahedral deformation; mixed cation; non-covalent interaction; Bayesian optimization; GENERALIZED GRADIENT APPROXIMATION; TOTAL-ENERGY CALCULATIONS; LEAD IODIDE PEROVSKITES; HIGH-PERFORMANCE; ION DIFFUSION; STABILITY; EFFICIENT; METHYLAMMONIUM; FORMAMIDINIUM; SEGREGATION;
D O I
10.3390/molecules26206184
中图分类号
Q5 [生物化学]; Q7 [分子生物学];
学科分类号
071010 ; 081704 ;
摘要
Perovskites have stood out as excellent photoactive materials with high efficiencies and stabilities, achieved via cation mixing techniques. Overcoming challenges to the stabilization of Perovskite solar cells calls for the development of design principles of large cation incorporation in halide perovskite to accelerate the discovery of optimal stable compositions. Large fluorinated organic cations incorporation is an attractive method for enhancing the intrinsic stability of halide perovskites due to their high dipole moment and moisture-resistant nature. However, a fluorinated cation has a larger ionic size than its non-fluorinated counterpart, falling within the upper boundary of the mixed-cation incorporation. Here, we report on the intrinsic stability of mixed Methylammonium (MA) lead halides at different concentrations of large cation incorporation, namely, ehtylammonium (EA; [CH3CH2NH3](+)) and 2-fluoroethylammonium (FEA; [CH2FCH2NH3](+)). Density functional theory (DFT) calculations of the enthalpy of the mixing and analysis of the perovskite structural features enable us to narrow down the compositional search domain for EA and FEA cations around concentrations that preserve the perovskite structure while pointing towards the maximal stability. This work paves the way to developing design principles of a large cation mixture guided by data analysis of DFT data. Finally, we present the automated search of the minimum enthalpy of mixing by implementing Bayesian optimization over the compositional search domain. We introduce and validate an automated workflow designed to accelerate the compositional search, enabling researchers to cut down the computational expense and bias to search for optimal compositions.</p>
引用
收藏
页数:16
相关论文
共 50 条
  • [31] Organic Cation-Dependent Degradation Mechanism of Organotin Halide Perovskites
    Wang, Feng
    Ma, Jiale
    Xie, Fangyan
    Li, Linkai
    Chen, Jian
    Fan, Jun
    Zhao, Ni
    ADVANCED FUNCTIONAL MATERIALS, 2016, 26 (20) : 3417 - 3423
  • [32] Insight into the Role of Guanidinium and Cesium in Triple Cation Lead Halide Perovskites
    Ramos-Terron, Susana
    Illanes, Jose Francisco
    Bohoyo-Gil, Diego
    Camacho, Luis
    de Miguel, Gustavo
    SOLAR RRL, 2021, 5 (12):
  • [33] Thermal stability and decomposition kinetics of mixed-cation halide perovskites
    Chen, Zicong
    Yang, Zhenyu
    Du, Shijie
    Lin, Dabin
    Zhang, Fangteng
    Zeng, Youjun
    Liu, Guanyu
    Nie, Zhaogang
    Ma, Lin
    PHYSICAL CHEMISTRY CHEMICAL PHYSICS, 2023, 25 (48) : 32966 - 32971
  • [34] Role of the Alkali Metal Cation in the Early Stages of Crystallization of Halide Perovskites
    Flatken, Marion A.
    Radicchi, Eros
    Wendt, Robert
    Buzanich, Ana Guilherme
    Haerk, Eneli
    Pascual, Jorge
    Mathies, Florian
    Shargaieva, Oleksandra
    Prause, Albert
    Dallmann, Andre
    De Angelis, Filippo
    Hoell, Armin
    Abate, Antonio
    CHEMISTRY OF MATERIALS, 2022, 34 (03) : 1121 - 1131
  • [35] Recent Advances in the A-Site Cation Engineering of Lead Halide Perovskites
    Ma, Yunxiu
    Wang, Yu
    Fang, Yueyue
    Jiang, Yu
    Dai, Zhigao
    Miao, Jinshui
    ADVANCED OPTICAL MATERIALS, 2024, 12 (30):
  • [36] Mixed cation hybrid lead halide perovskites with enhanced performance and stability
    Xu, Feng
    Zhang, Taiyang
    Li, Ge
    Zhao, Yixin
    JOURNAL OF MATERIALS CHEMISTRY A, 2017, 5 (23) : 11450 - 11461
  • [37] Mitigation of Halide Segregation by Cation Composition Management in Wide Bandgap Perovskites
    Safdari, Majid
    Kim, Daehan
    Balvanz, Adam
    Kanatzidis, Mercouri G.
    ACS ENERGY LETTERS, 2024, 9 (07): : 3400 - 3408
  • [38] Design of Mixed-Cation Tri-Layered Pb-Free Halide Perovskites for Optoelectronic Applications
    Liu, Zhun
    Zhao, Xingang
    Zunge, Alex
    Zhang, Lijun
    ADVANCED ELECTRONIC MATERIALS, 2019, 5 (06)
  • [39] Rotational Energy Barriers and Relaxation Times of the Organic Cation in Cubic Methylammonium Lead/Tin Halide Perovskites from First Principles
    Kanno, Shohei
    Imamura, Yutaka
    Saeki, Akinori
    Hada, Masahiko
    JOURNAL OF PHYSICAL CHEMISTRY C, 2017, 121 (26): : 14051 - 14059
  • [40] Exploring Lysine Incorporation as a Strategy to Mitigate Postsynthetic Halide Exchange in Lead-Halide Hybrid Perovskites
    Lang, Arad
    Kurashvili, Mariam
    Sklar, Johanna
    Polishchuk, Iryna
    Fada'os, Awj
    Sessa, Ithai
    Buyan-Arivjikh, Altantulga
    Katsman, Alexander
    Feldmann, Jochen
    Pokroy, Boaz
    ACS APPLIED MATERIALS & INTERFACES, 2025, 17 (06) : 9485 - 9493