液相外延层层浸渍组装金属-有机框架薄膜及其物理性能

王大为; 谷志刚; 张健

doi:10.7498/aps.69.20200274

摘要

金属-有机框架(MOF)作为一种通过配位键将金属节点和有机配体连接而成的新型无机-有机杂化多孔有序晶体材料, 因其具有比表面积大、稳定性好、结构多样以及功能可调等优点, 受到人们的广泛关注. MOF薄膜的制备和功能化拓展了其应用领域. 本文重点介绍了用液相外延层层浸渍法组装表面配位金属-有机框架薄膜(SURMOF), 并总结了部分SURMOF在光学、电学等方面的物理性能, 以及对SURMOF的应用前景进行了展望.

关键词:

Abstract

Metal-organic framework (MOF) is a new kind of inorganic-organic hybrid porous ordered crystal material, which is connected by metal nodes and organic ligands through coordination bond. Because of its large specific surface area, high stability, diverse structure and adjustable function, MOF has received wide attention. The improvements in preparation and functionalization of MOF thin films expand their application fields. In this paper, the method for assembly of surface coordinated metal-organic framework thin films (SURMOF) by liquid phase expitaxial layer-by-layer dipping method is introduced, and the physical properties of some SURMOFs in optics, electricity and other aspects are summarized, and the application prospect of SURMOF is prospected as well.

Keywords:

metal-organic framework /
thin film /
liquid phase expitaxial layer by layer /
physical properties

作者及机构信息

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

通信作者: 谷志刚, zggu@fjirsm.ac.cn

基金项目: 国家级-国家自然科学基金(21872148)

Authors and contacts

State Key Laboratory of Structural Chemistry, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, Fuzhou 350002, China

Corresponding author: Gu Zhi-Gang, zggu@fjirsm.ac.cn

文章全文 : translate this paragraph

参考文献

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施引文献

图 1 MOF (顶排)和次级构筑单元(中排)以及配体(下排)的结构模型^[1]

Fig. 1. Structural model of MOF (top row) and the representative secondary building units (middle row), as well as ligands (down row)^[1]

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图 2 液相外延法层层组装制备SURMOF示意图^[12]

Fig. 2. Schematic diagram of liquid phase epitaxial layer by layer assembly of SURMOF ^[12].

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图 3 机械液相外延层层浸渍法制备 SURMOF装置示意图(P0, 样品架的起始和最终位置; P1—P7, 浸泡溶液; 1, 聚四氟乙烯工作台; 2, 容器盖; 3, 夹持器; 4, 样品夹; 5, 样品; 6, 位置控制器; 7, 超声波清洗器; 8, 清洗池; 9, 容器盖的位置; 10, 泵和清洗容器; 11, 计算机)^[33]

Fig. 3. Schematic diagram of SURMOF prepared by liquid phase epitaxy layer by layer dipping method (P0, starting and final position for the sample holder; P1− P7, containers for immersion solutions; 1, Teflon working table; 2, container lid; 3, gripper; 4, sample holder; 5, sample; 6, position controller; 7, ultrasonic bath; 8, shower; 9, parking position of container lid; 10, pump and solution bottle for showering; 11, computer)^[33].

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图 4 在羟基和羧基修饰的基底上通过液相外延法逐层生长不同取向MOF膜的示意图^[35]

Fig. 4. Schematic diagram of MOF grown on the hydroxyl and carboxyl-terminated substrate via liquid phase epitaxy layer by layer method^[35]

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图 5 HKUST-1薄膜的SEM图像^[36]

Fig. 5. SEM image of HKUST-1 thin film^[36]

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图 6 (a)制备的OFET实物图; (b) HKUST-1薄膜修饰SiO₂介电层界面的OFET结构示意图; (c)半导体聚合物PTB7-Th的化学结构; (d) SURMOF HKUST-1的制备示意图及HKUST-1结构图; (e) HKUST-1/SiO₂/Si结构OFET器件的输出特性; (f) HKUST-1/SiO₂/Si结构OFET器件的传输特性^[40]

Fig. 6. (a) Sample diagram of field effect transistor (OFET); (b) sketch diagram of HKUST-1 film modified SiO₂ dielectric layer in the OFETs; (c) structure of semiconductor polymer PTB7-Th; (d) schematic diagram of liquid phase epitaxy layer by layer preparation of HKUST-1 and the structure; (e) the output characteristics of HKUST-1/SiO₂/Si based OFETs; (f) the transmission characteristics of HKUST-1/SiO₂/Si based OFETs^[40].

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图 7 (a)采用液相外延法将Ln(pdc)₃逐层负载到SURMOF孔道的示意图; (b) Ln(pdc)₃结构示意图; (c)紫外光(365 nm)照射石英玻璃生长的Ln(pdc)₃@HKUST-1薄膜和混合型Ln(pdc)₃@HKUST-1薄膜的照片; (d) Eu(pdc)₃@HKUST-1, Tb(pdc)₃@HKUST-1和Gd(pdc)₃@HKUST-1薄膜的发射光谱; (e)红色、绿色、蓝色发光的Ln(pdc)₃@HKUST-1薄膜以及混合白光发射薄膜的CIE色度坐标图^[43]

Fig. 7. (a) Schematic diagram of Ln(pdc)₃ encapsulated into SURMOF and grown in situ layer by layer using the liquid phase epitaxy method; (b) schematic diagram of Ln(pdc)₃ structure; (c) photographs of Ln(pdc)₃@HKUST-1 film on quartz glass under ultraviolet (365 nm) irradiation; (d) solid-phase photoluminescence emission spectra of Eu(pdc)₃@HKUST-1, Tb(pdc)₃@HKUST-1, Gd(pdc)₃@HKUST-1 films; (e) CIE chromaticity coordinate chart of red, green, blue and wite emitting Ln(pdc)₃@ HKUST-1 film^[43].

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图 8 (a)硅衬底上发射-敏化-发射(A-B-A)异质结构的截面SEM图; (b)不同有机连接体组成的A型、B型SURMOF异质结连接示意图; (c) Zn-ADB (A)和Zn-(Pd-DCP)(B)制备的SURMOF以及由它们构成异质结的XRD衍射图; (d)三重激发态分子传递光子上转换的示意图; (e)发射光谱示意图^[44]

Fig. 8. (a) SEM image of emission sensitization emission (A-B-A) heterostructure cross section on silicon substrate; (b) schematic diagram of A and B SURMOF heterojunction connection composed of different organic connectors; (c) the diffraction patterns of SURMOF prepared by Zn-ADB (A) and Zn-(Pd-DCP) (B); (d) the schematic diagram of photon upconversion of triplex excited state molecular transfer; (e) the schematic diagram of emission spectrum^[44].

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图 9 (a) MOF模板法制备CDs示意图; (b)石英玻璃、G@HKUST-1-200薄膜以及合成过程中的中间体材料照片; (c) CD@HKUST-1-200薄膜在350 nm激发波长的荧光发射谱图; (d) G@HKUST-1薄膜、CD@HKUST-1-200薄膜和HKUST-1模板制备的CDs水溶液的开孔Z-扫描数据(点)以及532 nm激发波长下的理论拟合数据(实线)^[45]

Fig. 9. (a) Schematic diagram of CDs prepared by MOF template method; (b) photos of the sample in the synthesis process; (c) photoluminescence of CD@HKUST-1-200 film; (d) open hole Z-scan data of CD@HKUST-1-200 film and HKUST-1 grown on quartz glass (point) and CDs aqueous solution made from G@HKUST-1 film with theoretical fitting data at 532 nm excitation wavelength^[45]

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图 10 (a)采用液相外延层层组装法在硅基底上逐层生长取向CoFe-PBA薄膜的示意图; (b)薄膜XRD对比和(c) [100]取向CoFe-PBA薄膜的SEM图(插图是CoFe-PBA薄膜在Si衬底上的模型图); (d)扫描速率为2 mV/s的线性扫描伏安曲线(已经过内阻校正); ① CoFe₂O₄薄膜、② RuO₂、③ CoFe₂O₄粉末、④ Fe-PBA薄膜、⑤ 泡沫镍-350; (e)为不同的电催化剂电流密度达到10 mA/cm²所需的过电位对比图; (f)塔费尔斜率对比图; (g)在1.5 V下的CoFe₂O₄薄膜和CoFe₂O₄粉末的电化学阻抗谱对比^[48]

Fig. 10. (a) Schematic diagram of layer by layer growth of oriented CoFe-PBA thin film on silicon substrate by LPE LBL method; (b) XRD comparison and (c) SEM image of oriented CoFe-PBA thin film in [100] plane (illustration shows the microstructure of CoFe PBA film on Si substrate); (d) linear sweep voltammetry curve with 2 mV/s scanning rate (IR corrected) of the sample; (e) the over potential required of different electrocatalyst to reach 10 mA/cm²; (f) the comparison of Tafel slope; (g) the comparison of electrochemical impedance spectra of CoFe₂O₄ film and CoFe₂O₄ powder at 1.5 V^[48]

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液相外延层层浸渍组装金属-有机框架薄膜及其物理性能