具有电化学分子选择性的金属有机骨架薄膜的制备
发布时间：2018-08-26 09:54
【摘要】：近年来,MOF材料由于其大的比表面积、规则可调的孔径和可拆剪的化学性质等特点而被广泛关注,在气体分离存储、化学传感、催化、药物传输等方面表现出巨大的应用潜能。然而有关MOF材料电化学应用的研究报道相对比较少,将MOF膜层集成到电极表面实现电化学分子选择性催化和传感是拓展这方面研究的一个重要方向。在本论文中,我们选择了已经被报道比较稳定的ZIF-8和UiO-66作为研究对象,探讨了它们在电化学分子选择性催化和传感应用方面的可能性。相关的研究主要从以下三个方面展开：(1)采用室温醇相合成方法在FTO上制备了致密、无缺陷的ZIF-8薄膜,并分别用SEM和XRD对膜层的形貌和结构进行了表征。然而,我们发现所得到的膜层即使在接近中性的水溶液中也不能稳定存在。因此,尽管通过室温醇相合成方法可以成功地将ZIF-8集成到电极表面,但所得到体系的稳定性并不能满足电化学应用的要求。(2)通过表面化学对基底表面进行修饰,使基底表面具有不同的官能团(如-OH、-NH2、 PVP、-COOH、PDA、BDC),然后对UiO-66薄膜在这些基底上的生长条件进行了摸索。研究结果表明在-COOH修饰的玻璃基底和FTO上可以生长出致密、平整的UiO-66和NH2-Ui0-66薄膜。同时,通过调节反应物浓度和利用二次生长法可以对膜层厚度进行调控。(3)利用PDMS填充法、超临界C02干燥法、表面活性剂辅助干燥法对UiO-66薄膜进行了后处理,以[Fe(phen)3]2+、[Fe(CN)6]3-、[Ru(NH3)6]3+为探针分子对所得到的UiO-66/FTO体系进行了电化学检测。研究结果表明三种后处理方法均可以有效地减少膜层缺陷或降低其影响,其中PDMS填充法和超临界C02干燥法处理后的UiO-66薄膜展现出绝对的电化学分子选择性。
[Abstract]:In recent years, due to its large specific surface area, regular adjustable pore size and detachable chemical properties, MOF materials have attracted extensive attention. They have shown great application potential in gas separation and storage, chemical sensing, catalysis, drug transport and so on. However, there are few reports on the electrochemical application of MOF materials. It is an important research direction to integrate the MOF film layer onto the electrode surface to realize the electrochemical molecular selective catalysis and sensing. In this thesis, we have selected ZIF-8 and UiO-66, which have been reported as relatively stable, as the research objects, and discussed their potential applications in electrochemical molecular selective catalysis and sensing. The related studies were carried out in the following three aspects: (1) dense and defect-free ZIF-8 thin films were prepared on FTO by the synthesis of alcohols at room temperature, and the morphology and structure of the films were characterized by SEM and XRD, respectively. However, we found that the film could not exist stably even in near neutral aqueous solution. Therefore, although ZIF-8 can be successfully integrated into the electrode surface by the method of synthesis of alcohols at room temperature, the stability of the obtained system does not meet the requirements of electrochemical application. (2) the substrate surface is modified by surface chemistry. Different functional groups (such as -OH- NH _ 2, PVP,-COOH,PDA,BDC) were found on the substrate surface, and then the growth conditions of UiO-66 films on these substrates were explored. The results show that dense, flat UiO-66 and NH2-Ui0-66 thin films can be grown on the glass substrates and FTO modified by -COOH. At the same time, the thickness of the film can be controlled by adjusting the reactant concentration and using the secondary growth method. (3) the UiO-66 film was treated by PDMS filling method, supercritical C02 drying method and surfactant assisted drying method. Using [Fe (phen) _ 3] _ 2, [Fe (CN) _ 6] _ 3-and [Ru (NH3) _ 6] _ 3 as probe molecules, the obtained UiO-66/FTO system was detected by electrochemical method. The results show that the three post-treatment methods can effectively reduce the defects or the influence of the film. The UiO-66 films treated by PDMS filling method and supercritical C02 drying method show absolute electrochemical molecular selectivity.
【学位授予单位】：苏州大学
【学位级别】：硕士
【学位授予年份】：2015
【分类号】：TB383.2
本文编号：2204495
[Abstract]:In recent years, due to its large specific surface area, regular adjustable pore size and detachable chemical properties, MOF materials have attracted extensive attention. They have shown great application potential in gas separation and storage, chemical sensing, catalysis, drug transport and so on. However, there are few reports on the electrochemical application of MOF materials. It is an important research direction to integrate the MOF film layer onto the electrode surface to realize the electrochemical molecular selective catalysis and sensing. In this thesis, we have selected ZIF-8 and UiO-66, which have been reported as relatively stable, as the research objects, and discussed their potential applications in electrochemical molecular selective catalysis and sensing. The related studies were carried out in the following three aspects: (1) dense and defect-free ZIF-8 thin films were prepared on FTO by the synthesis of alcohols at room temperature, and the morphology and structure of the films were characterized by SEM and XRD, respectively. However, we found that the film could not exist stably even in near neutral aqueous solution. Therefore, although ZIF-8 can be successfully integrated into the electrode surface by the method of synthesis of alcohols at room temperature, the stability of the obtained system does not meet the requirements of electrochemical application. (2) the substrate surface is modified by surface chemistry. Different functional groups (such as -OH- NH _ 2, PVP,-COOH,PDA,BDC) were found on the substrate surface, and then the growth conditions of UiO-66 films on these substrates were explored. The results show that dense, flat UiO-66 and NH2-Ui0-66 thin films can be grown on the glass substrates and FTO modified by -COOH. At the same time, the thickness of the film can be controlled by adjusting the reactant concentration and using the secondary growth method. (3) the UiO-66 film was treated by PDMS filling method, supercritical C02 drying method and surfactant assisted drying method. Using [Fe (phen) _ 3] _ 2, [Fe (CN) _ 6] _ 3-and [Ru (NH3) _ 6] _ 3 as probe molecules, the obtained UiO-66/FTO system was detected by electrochemical method. The results show that the three post-treatment methods can effectively reduce the defects or the influence of the film. The UiO-66 films treated by PDMS filling method and supercritical C02 drying method show absolute electrochemical molecular selectivity.
【学位授予单位】：苏州大学
【学位级别】：硕士
【学位授予年份】：2015
【分类号】：TB383.2
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