Molecular Insights into Water Vapor Adsorption and Interfacial Moisture Stability of Hybrid Perovskites for Robust Optoelectronics
Molecular Insights into Water Vapor Adsorption and Interfacial Moisture Stability of Hybrid Perovskites for Robust Optoelectronics
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杂化钙钛矿水蒸气吸附和界面水分稳定性的分子洞察，用于鲁棒光电器件
DOI：
10.1016/j.ijheatmasstransfer.2021.121334
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发表时间：
2021-08
影响因子：
5.2
通讯作者：
Zhao Changying
中科院分区：
文献类型：
--
作者：
Lin Shangchao;Chen Chao;Zhao Lingling;Wang Mingchao;Wang Jingfan;Zhou Huanhuan;Zhao Changying
了解界面传质过程，如混合钙钛矿的水蒸气吸附引起的降解，对于提高其光电器件在潮湿环境中的耐久性和性能至关重要。本文采用巨正则蒙特卡罗（GCMC）和分子动力学（MD）模拟方法研究了不同相对湿度（RH）条件下，[MAI] 0和[PbI 2] 0表面封端的MAPbI 3上的蒸汽吸附.得到的蒸气吸附等温线匹配的Brunauer-Emmett-Teller（BET）吸附模型与吸附热为0.510和0.609 eV，分别为[MAI] 0和[PbI 2]0的水单层。在[MAI]0（RH ≥ 30%）上形成水单分子层与[PbI 2]0（RH ≥ 10%）相比具有较低的亲水性一致，这反映在预测的较大水接触角上。基于预测的水表面覆盖率在不同的RH，水分引起的表面降解动力学进行了研究，使用MD模拟和过渡态理论。由于水溶剂化的类似离子去除途径，湿度对降解能垒的影响较小，但通过攻击表面离子的尝试频率强烈影响离子解离速率。[MAI] 0比[PbI 2]0更易受水的影响，尽管其亲水性较低，这意味着长期暴露的MAPbI 3大多被[PbI 2]0终止。在300 K和30 ~ 80%RH条件下，平均降解物质损失速率为5.8 ~ 13.1 μm/s，与实验结果一致。最后，我们提供了一个图片的水扩散为基础的降解机制，并阐明有趣的氢键功能在蒸汽MAPbI 3接口。这项研究提供了对固有的蒸气-钙钛矿相互作用的定量见解，并解决了金属卤化物钙钛矿中的水分不稳定机制，以合理设计防水，长期稳定和高效的光电器件。
Understanding interfacial mass transfer processes, such as the water vapor adsorption-induced degradation of hybrid perovskites, is vital for improving the durability and performance of their optoelectronic devices in the ambient atmosphere with humidity. In this paper, vapor adsorption on prototypical MAPbI3, terminated by [MAI]0and [PbI2]0surface, at different relative humidity (RH) levels is studied using grand canonical Monte Carlo (GCMC) and molecular dynamics (MD) simulations. The resulting vapor adsorption isotherms match the Brunauer-Emmett-Teller (BET) adsorption model with heats of adsorption of 0.510 and 0.609 eV, respectively, for water monolayers on [MAI]0and [PbI2]0. The formation of water monolayer on [MAI]0(for RH ≥ 30%) is consistent with its lower hydrophilicity compared to [PbI2]0(for RH ≥ 10%), reflected from the larger water contact angle predicted. Based on predicted water surface coverages at various RHs, the moisture-induced surface degradation kinetics is studied using MD simulations and transition-state theory. Humidity has a minor impact on the degradation energy barriers due to the similar ion removal pathway by water solvation, but strongly affects the ion dissociation rates through the frequency of attempts to attack surface ions. [MAI]0is more vulnerable against water than [PbI2]0, despite its lower hydrophilicity, implying that long-term exposed MAPbI3are mostly terminated by [PbI2]0. Furtherly, averaged degradation material loss rates of 5.8 ~ 13.1 μm/s are estimated at 30 ~ 80% RH levels and 300 K, which is consistent with experiment observations. Finally, we offer a picture for the water-diffusion-based degradation mechanism and elucidate interesting hydrogen-bonding features at the vapor-MAPbI3interface. This research provides quantitative insights into the inherent vapor-perovskite interactions and addresses the moisture instability mechanisms in metal halide perovskites towards the rational design of water-resistant, long term stable and efficient optoelectronic devices.
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有机金属卤化物钙钛矿中氧和水引起的能量降解
影响因子：
9.5
作者：
Yang Jianming;Yuan Zhongcheng;Liu Xianjie;Braun Slawomir;Li Yanqing;Tang Jianxin;Gao Feng;Duan Chungang;Fahlman Mats;Bao Qinye
通讯作者：
Bao Qinye
影响因子：
5.7
作者：
Hailegnaw, Bekele;Kirmayer, Saar;Cahen, David
通讯作者：
Cahen, David
DOI：
10.1021/j100498a015
发表时间：
1978-05
期刊：
The Journal of Physical Chemistry
影响因子：
--
作者：
M. Nagao;K. Yunoki;H. Muraishi;T. Morimoto
通讯作者：
M. Nagao;K. Yunoki;H. Muraishi;T. Morimoto
中等湿度延迟有机-无机杂化钙钛矿中的电子-空穴复合：时域从头算模拟使实验合理化
影响因子：
5.7
作者：
Long, Run;Fang, Weihai;Prezhdo, Oleg. V.
通讯作者：
Prezhdo, Oleg. V.
影响因子：
3.7
作者：
Shi Liu;R. Cohen
通讯作者：
Shi Liu;R. Cohen