本研究以氣相奈米粒子電移動度分析儀 (differential mobility analyzer，DMA) 及傅立葉轉換紅外線光譜儀 (Fourier transform infrared spectroscope，FTIR) 兩種分析儀器為基礎，建立一定量定性分析技術與方法，藉由量測混成式奈米粒子的電移動度粒徑分佈、數量濃度及成分組成等性質來進行混成式奈米材料之開發及其膠體與界面化學之研究，透過這些資訊可進一步探討配體與奈米粒子間的吸脫附現象與優化作為生醫及能環領域應用之相關製備條件。
首先，在本研究的第一部分中，我們利用靜電自組裝法製備玻尿酸-金奈米粒子混成式奈米材料，並成功結合DMA及FTIR建立一套定量定性分析技術與方法來開發玻尿酸-金奈米粒子，並鑑定玻尿酸在牛血清蛋白-金奈米粒子表面的界面化學之效應。我們藉由建立感應耦合電漿質譜儀 (inductively coupled plasma-mass spectrometer，ICP-MS) 與電噴灑式氣相奈米粒子電移動度分析儀 (electrospray- differential mobility analyzer，ES-DMA)之整合技術，可以成功分析玻尿酸、牛血清蛋白及金奈米粒子之物理尺寸、數量與質量濃度以及聚集程度，而在pH 3環境下，當玻尿酸濃度小於5 × 10-3 μmol/L時，玻尿酸在牛血清蛋白-金奈米粒子之表面吸附密度與玻尿酸濃度呈正相關，且平衡吸附常數大約為4 × 105 L/mol。接著，玻尿酸受到酸鹼度與酵素誘導影響在牛血清蛋白-金奈米粒子表面脫落現象也成功的藉由ES-DMA以及衰減全反射式傅立葉轉換紅外線光譜儀 (attenuated total reflectance-Fourier transform infrared spectroscope，ATR-FTIR) 鑑定。在沒有添加酵素，環境酸鹼度從pH 3調至pH 7時，玻尿酸的脫落速率常數至少增加了3.7倍，而當加入酵素後，玻尿酸的脫落速率常數更進一步增加了2.0倍以上。研究成果顯示經由定量分析證明，透過改變水相中奈米膠體材料之表面化學性質以合成玻尿酸功能性奈米材料，對於各種玻尿酸衍生物應用在生醫領域有很大的幫助。
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在本研究的第二部分，我們以氣溶膠合成法為基礎，結合DMA及FTIR之分析技術與方法來開發銀碳混成式奈米粒子團簇 (Ag-C-NPC)，並即時地定量分析其界面化學之效應，並探討Ag-C-NPC應用於電容去離子技術時的性能表現。首先，我們成功的以氣相誘導自組裝法製備Ag-C-NPC，使銀奈米粒子均勻地裝飾在碳奈米粒子團簇上，而其粒徑大小、數量濃度及結構中的成分比例等界面化學性質，都可以藉由DMA及程序升溫傅立葉紅外光譜儀 (temperature-programmed Fourier transform infrared spectroscope，TP-FTIR) 即時鑑定，並透過調整前驅物濃度來控制Ag-C-NPC之特性。研究結果顯示，在碳奈米粒子團簇中添加銀奈米粒子，改善了以碳基材作為CDI電極材料時的離子吸附容量與充放電循環可逆性，達到了相當高的去鹽能力，相當於每克電極重可以去除17.5毫克溶液中的鹽。本研究驗證了結合氣溶膠合成法與即時性定量分析系統開發Ag-C-NPC並提升CDI性能表現之概念，透過此鑑定技術所得到之界面化學資訊，可以調控Ag-C-NPC之材料性質以優化其作為CDI電極時之離子吸附容量及循環穩定性。
本研究建立了一個可調控且快速的合成方法，並結合DMA及FTIR建立一套分析技術與方法開發混成式奈米材料，得到其尺寸大小、表面結構、數量與質量濃度、配體吸脫附現象及成分組成等特性，透過此鑑定技術充分了解混成式奈米材料界面化學效應之機制，對於開發混成式奈米材料與研究其配方化學以及在生醫與能環領域應用之優化都有很大的幫助。

In this work, we demonstrate a real-time characterization method using differential mobility analyses coupled to Fourier-transform infrared spectroscopy (DMA/FTIR) for the development of hybrid nanomaterials for biomedical and energy & environmental applications. The interfacial phenomena of hybrid nanomaterials, including mobility size distribution, number concentrations and chemical composition can be characterized by DMA/FTIR for the performance optimization.
In the first part of this work, a facile electrostatic-directed assembly method is used for the fabrication of hyaluronic acid (HA)-functionalized gold nanoparticle (AuNP). Here, the assembly-disassembly of hyaluronic acid (HA) with bovine serum albumin-conjugated gold nanoparticle (BSA-AuNP) was demonstrated using orthogonal characterization approaches: electrospray-differential mobility analysis (ES-DMA) and attenuated total reflection Fourier transform infrared spectroscopy (ATR-FTIR). Physical sizes, number and mass concentrations, and degrees of aggregation of HA, BSA and AuNP were successfully quantified using the ES-DMA hyphenated with inductively coupled plasma mass spectrometry (ICP-MS). Surface packing density of HA on the BSA-AuNP was shown to be proportional to the concentration of HA (CHA) when CHA ≤ 5 × 10-3 μmol/L, and the equilibrium binding constant of HA on the BSA-AuNP was identified as ≈ 4 × 105 L/mol at pH 3. The pH-sensitive and enzyme-induced detachments of HA from BSA-AuNP were both successfully characterized by using ES-DMA and ATR-FTIR. In the absence of enzymatic catalysis, the rate constant of HA detachment (k) was shown to increase by at least 3.7 times via adjusting the environmental acidity from pH 3 to pH 7. A significant enzyme-induced HA detachment was identified at pH 7, showing a remarkably increase of k by at least 2.0 times in the presence of enzyme. The work provides a proof of concept for assembly of
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HA-based hybrid colloidal nanomaterials through the tuning of surface chemistry in the aqueous phase with the ability of in-situ quantitative characterization, which has shown the promise for the development of a variety of HA-derivative biomedical applications (e.g., drug delivery).
In the second part of this work, an aerosol-based synthetic approach, in combination with a real-time characterization method using differential mobility analyses coupled to temperature-programmed Fourier transform infrared spectroscopy (DMA/TP-FTIR), was demonstrated for the development of silver-carbon hybrid nanoparticle cluster (Ag-C-NPC). Here, silver-decorated carbon nanoparticle clusters (Ag-C-NPCs) were fabricated via gas-phase evaporation-induced self-assembly (EISA), which are used as electrode material of capacitive deionization of salt-containing wastewater. Physical size, number concentration, and compositions of the Ag-C-NPC were shown to be tunable and successfully characterized directly in the aerosol state on a quantitative basis using the DMA/TP-FTIR. The enhancements of deionization capacity and the charging/discharging reversibility are achievable by the addition of Ag NP. A remarkably high salt adsorption capacity of the Ag-C-NPC was achievable (17.5 mg of salt per gram of electrode material). This work provides a proof of concept of using the aerosol-based synthesis with the support of in-situ characterization for the development of Ag-C nanocomposite clusters with high CDI performance. The method also shows promise for the tuning of the material properties of Ag-C-NPC for the optimization of the CDI capacity and cyclic stability useful for a variety of the water desalination applications (e.g., brackish water).
This work demonstrates a controlled and facile synthetic approach with the support of in-situ aerosol-phase characterization to develop hybrid nanomaterials. The mechanistic understanding correlated to their interfacial phenomena is useful for the
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formation of hybrid nanomaterials and the performance optimization in the biomedical and energy & environmental applications.

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