原位烷基化调控无机-有机杂化类钙钛矿材料的结构及其性能※
收稿日期: 2021-12-22
网络出版日期: 2022-02-15
基金资助
国家自然科学基金(91961115); 国家自然科学基金(21975254); 国家自然科学基金(21905280); 中国科学院青年创新促进会(2018342)
In situ Alkylation Regulation of the Structure and Properties of Inorganic-Organic Hybrid Perovskite-Like Materials※
Received date: 2021-12-22
Online published: 2022-02-15
Supported by
National Natural Science Foundation of China(91961115); National Natural Science Foundation of China(21975254); National Natural Science Foundation of China(21905280); Youth Innovation Promotion Association of Chinese Academy of Sciences(2018342)
无机-有机杂化类钙钛矿材料由于结构可调和独特的光电特性而引起了人们的广泛关注. 通过选用不同的烷基化溶剂, 一步水热法原位合成了两种新型的无机-有机杂化材料——二维(2D)结构的[(Me3)ODA(Me3)]3Pb5I16 (1)和一维(1D)结构的[H(Et2)ODA(Et2)H]Pb2I6•H2O (2) (ODA=4,4-二氨基二苯醚). 化合物1由2D的无机类钙钛矿层[Pb5I16]6–和有机阳离子[(Me3)ODA(Me3)]2+组成, 化合物2由1D无机类钙钛矿链[Pb2I6]2–、有机阳离子[(Et2)ODA(Et2)]2+和水分子组成. 实验表明, 两种不同维度的化合物虽然都具有典型的半导体性能, 但却表现出不同的化学稳定性以及光、电等物理特性. 其中, 化合物1对波长为400~700 nm的光呈现出明显的光电响应, 而化合物2在对水和有机溶剂表现出良好稳定性的同时, 还表现出优异的湿敏响应性能.
梁广玲 , 叶晓亮 , 王观娥 , 徐刚 . 原位烷基化调控无机-有机杂化类钙钛矿材料的结构及其性能※[J]. 化学学报, 2022 , 80(4) : 460 -466 . DOI: 10.6023/A21120573
Inorganic-organic hybrid perovskite-like materials have attracted widespread attention due to their tunable structure and unique optoelectronic properties. By simply changing the size of the organic cations, the structural dimensions of inorganic-organic hybrid perovskite-like materials can be adjusted. However, most of the research were carried out by selecting different types of organic cationic ligands, which is not conducive to the study of structure-activity relationship. Herein, by choosing different alkylation solvents, the control of dimensions and performance of inorganic-organic hybrid perovskite-like materials was realized when the reaction precursors were consistent. Two new inorganic-organic hybrid materials were synthesized in situ by a simple one-step hydrothermal method, that were two-dimensional (2D) [(Me3)ODA(Me3)]3Pb5I16 (1) and one-dimensional (1D) [H(Et2)ODA(Et2)H]Pb2I6•H2O (2) (ODA=4,4-diaminodiphenyl ether). Compound 1 is consisted by 2D inorganic perovskite-like network layers and [(Me3)ODA(Me3)]2+ organic dications, while compound 2 is composed by 1D inorganic perovskite-like chains, [H(Et2)ODA(Et2)H]2+ and water molecules. Compound 1 and 2 showed different structures and exhibited different stability, optoelectronics, and humidity sensitivity. The methylated compound 1 showed an obvious photoelectric response under visible light illumination (400~790 nm), and the ethylated compound 2 exhibited no photoelectric response. Compound 2 presented better stability to water and organic solvents compared to compound 1, which can be as an ideal candidate in fabricating smart and efficient sensors for humidity detection. The chemiresistive humidity sensor based on compound 2 showed an investigated response in the wide relative humidity (RH) (10%~100%) at room temperature. The sensor showed a high sensitivity in the range of 10%~100% RH and good cycle stability. It displayed 105-fold increase toward 100% RH. The sensing mechanism of the compound 2 based humidity sensor was further studied by direct current (DC) instantaneous reverse polarity method, which proved that the moisture responsiveness was dominated by electronic conduction, and the free transmission of electrons dominated the change of material's conductivity.
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