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※

doi:10.6023/A21120573

化学学报 ›› 2022, Vol. 80 ›› Issue (4): 460-466.DOI: 10.6023/A21120573 上一篇下一篇

所属专题：中国科学院青年创新促进会合辑

研究论文

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^※

梁广玲^a^,^b^,^c, 叶晓亮^b^,^c, 王观娥^a^,^b^,^c^,^*(), 徐刚^b^,^c

a 福建师范大学化学与材料学院福州 350007
b 中国科学院福建物质结构研究所结构化学国家重点实验室福州 350002
c 中国科学院大学北京 100049

投稿日期:2021-12-22 发布日期:2022-02-15
通讯作者: 王观娥
作者简介:
^※ 庆祝中国科学院青年创新促进会十年华诞.
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^※

Guang-ling Liang^a^,^b^,^c, Xiao-liang Ye^b^,^c, Guan-E Wang^a^,^b^,^c(), Gang Xu^b^,^c

a College of Chemistry and Materials Science, Fujian Normal University, Fuzhou 350007
b State Key Laboratory of Structural Chemistry, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, Fuzhou 350002
c University of Chinese Academy of Sciences, Beijing 100049

Received:2021-12-22 Published:2022-02-15
Contact: Guan-E Wang
About author:
^※ Dedicated to the 10th anniversary of the Youth Innovation Promotion Association, CAS.
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)

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1. Supporting Information-A21120573.pdf(859KB)

摘要/Abstract

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.

关键词: 无机-有机杂化, 结构调控, 光电响应, 湿度传感

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.

Key words: inorganic-organic hybrid, structure control, photoelectric response, humidity sensing

引用此文

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.

Guang-ling Liang, Xiao-liang Ye, Guan-E Wang, Gang Xu. In situ Alkylation Regulation of the Structure and Properties of Inorganic-Organic Hybrid Perovskite-Like Materials^※[J]. Acta Chimica Sinica, 2022, 80(4): 460-466.

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图/表 5

图1. (a) Pb5I166–最小不对称单元的配位模式、(b)由Pb5I166–组成的二维层状结构、(c) [(Me3)ODA(Me3)]3Pb5I16的三维堆积、(d) Pb2I62–最小不对称单元的配位模式、(e)由Pb2I62–组成的一维链状结构及(f) [H(Et2)ODA(Et2)H]Pb2I6•H2O的三维堆积(为清楚起见, 省略了H原子)

Figure 1. (a) Coordination mode of the smallest asymmetric unit of Pb5I166–, (b) 2D layered structure consisted of Pb5I166–, (c) 3D stacking of [(Me3)ODA(Me3)]3Pb5I16, (d) coordination mode of the smallest asymmetric unit of Pb2I62–, (e) 1D chain structure comprised of Pb2I62– and (f) 3D stacking of [H(Et2)ODA(Et2)H]Pb2I6•H2O (for clarity, the H atom is omitted)

图2. (a)化合物1和(b)化合物2的模拟和实验PXRD图谱以及它们在室温下于不同溶剂中浸泡2 h后的PXRD图谱

Figure 2. Simulated and experimental PXRD patterns of (a) compound 1 and (b) compound 2, and their PXRD patterns after immersing in different solvents at room temperature for 2 h

图3. (a)化合物1和(b)化合物2在30~130 ℃范围内的I-V曲线、(c)化合物1和化合物2温度依赖的电导率图(ln σ-1000/T)和(d)化合物1和化合物2的光学带隙

Figure 3. I-V Curves of (a) compound 1 and (b) compound 2 in the range of 30~130 ℃, (c) temperature-dependent conductivity results of compound 1 and compound 2 (ln σ-1000/T) and (d) the optical band gap of compound 1 and compound 2

图4. (a)化合物1和化合物2对不同波长光(400~700 nm)的光电流响应及(b)化合物1在550 nm波长下的光电流循环稳定性

Figure 4. (a) Photocurrent response of compound 1 and compound 2 to light with different wavelengths (400~700 nm) and (b) cyclic stability of the photocurrent of compound 1 at 550 nm

图5. 室温下, 基于化合物2的传感器的湿度响应特性 (a) 10%~100% RH下的响应-恢复曲线; (b) 响应值-RH%曲线图; (c) 70% RH下连续4个循环的响应-恢复曲线; (d) 使用直流瞬时极性反转获得的传感器在40%~100% RH下的电流-时间曲线

Figure 5. Humidity response characteristics of the sensor based on compound 2 at room temperature (a) response-recovery curve at 10%~100% RH; (b) response-RH% plot; (c) response-recovery curve for four consecutive cycles at 70% RH; (d) current-time curves of the sensor at 40%~100% RH obtained by using DC instantaneous reverse polarity experiments

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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^※

In situ Alkylation Regulation of the Structure and Properties of Inorganic-Organic Hybrid Perovskite-Like Materials^※

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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※

In situ Alkylation Regulation of the Structure and Properties of Inorganic-Organic Hybrid Perovskite-Like Materials※

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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^※

In situ Alkylation Regulation of the Structure and Properties of Inorganic-Organic Hybrid Perovskite-Like Materials^※