【摘要】：近年來(lái),MOF材料由于其大的比表面積、規(guī)則可調(diào)的孔徑和可拆剪的化學(xué)性質(zhì)等特點(diǎn)而被廣泛關(guān)注,在氣體分離存儲(chǔ)、化學(xué)傳感、催化、藥物傳輸?shù)确矫姹憩F(xiàn)出巨大的應(yīng)用潛能。然而有關(guān)MOF材料電化學(xué)應(yīng)用的研究報(bào)道相對(duì)比較少,將MOF膜層集成到電極表面實(shí)現(xiàn)電化學(xué)分子選擇性催化和傳感是拓展這方面研究的一個(gè)重要方向。在本論文中,我們選擇了已經(jīng)被報(bào)道比較穩(wěn)定的ZIF-8和UiO-66作為研究對(duì)象,探討了它們?cè)陔娀瘜W(xué)分子選擇性催化和傳感應(yīng)用方面的可能性。相關(guān)的研究主要從以下三個(gè)方面展開(kāi)：(1)采用室溫醇相合成方法在FTO上制備了致密、無(wú)缺陷的ZIF-8薄膜,并分別用SEM和XRD對(duì)膜層的形貌和結(jié)構(gòu)進(jìn)行了表征。然而,我們發(fā)現(xiàn)所得到的膜層即使在接近中性的水溶液中也不能穩(wěn)定存在。因此,盡管通過(guò)室溫醇相合成方法可以成功地將ZIF-8集成到電極表面,但所得到體系的穩(wěn)定性并不能滿(mǎn)足電化學(xué)應(yīng)用的要求。(2)通過(guò)表面化學(xué)對(duì)基底表面進(jìn)行修飾,使基底表面具有不同的官能團(tuán)(如-OH、-NH2、 PVP、-COOH、PDA、BDC),然后對(duì)UiO-66薄膜在這些基底上的生長(zhǎng)條件進(jìn)行了摸索。研究結(jié)果表明在-COOH修飾的玻璃基底和FTO上可以生長(zhǎng)出致密、平整的UiO-66和NH2-Ui0-66薄膜。同時(shí),通過(guò)調(diào)節(jié)反應(yīng)物濃度和利用二次生長(zhǎng)法可以對(duì)膜層厚度進(jìn)行調(diào)控。(3)利用PDMS填充法、超臨界C02干燥法、表面活性劑輔助干燥法對(duì)UiO-66薄膜進(jìn)行了后處理,以[Fe(phen)3]2+、[Fe(CN)6]3-、[Ru(NH3)6]3+為探針?lè)肿訉?duì)所得到的UiO-66/FTO體系進(jìn)行了電化學(xué)檢測(cè)。研究結(jié)果表明三種后處理方法均可以有效地減少膜層缺陷或降低其影響,其中PDMS填充法和超臨界C02干燥法處理后的UiO-66薄膜展現(xiàn)出絕對(duì)的電化學(xué)分子選擇性。
[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.
【學(xué)位授予單位】：蘇州大學(xué)
【學(xué)位級(jí)別】：碩士
【學(xué)位授予年份】：2015
【分類(lèi)號(hào)】：TB383.2

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