本論文係有關於聚丙烯酸(PAA)被覆的磁性奈米粒子在廢水處理及強酸型磁性奈米吸附劑的製備與應用之研究。首先探討PAA被覆的磁性奈米粒子在染料廢水褪色上的應用；其次利用化學修飾方法，進一步修飾PAA被覆的磁性奈米粒子，使表面具備磺酸根，並應用在重金屬離子的分離與回收；最後以硫化鈉處理負載有重金屬離子的磁性奈米吸附劑，可製備出雙功能的複合奈米粒子。

關於PAA被覆的磁性奈米粒子在染料廢水褪色上的研究，係在25℃下，以鹼性染料亞甲基藍(methylene blue，MB)作為研究範例。實驗結果顯示，磁性奈米吸附劑對鹼性染料亞甲基藍(methylene blue)的吸附及脫附具有很高的效率，其吸附行為遵守Langmuir恆溫吸附模式，最大吸附容量(qm)和Langmuir平衡常數(KL)分別為19.9 mg•g-1 與10.1 mL•mg-1；吸附量隨溶液的pH值增加而增加，當pH>7時，吸附量趨於一穩定值。另外，此吸附過程為一吸熱程序，其焓的變化量為30.9 kJ•mol-1；磁性奈米吸附劑所吸附的MB可利用含醋酸的甲醇溶液加以脫附。值得一提的是，由於沒有內部擴散阻力的問題，MB的吸附與脫附程序皆可於2分鐘內完成。

關於強酸型磁性奈米吸附劑的製備，係先製備表面被覆PAA的磁性奈米粒子，再藉由碳二醯胺的活化將胺基苯磺酸共價鍵結在氧化鐵奈米粒子上。穿透式電子顯微鏡(TEM)與動態光散射分析儀(DLS)之分析顯示，磺酸化之磁性奈米粒子具有單分散性，其平均粒徑為13.5 nm，平均水力直徑為21 nm。由X射線繞射儀(XRD)分析得知，磁性奈米粒子為四氧化三鐵之尖晶石結構，且不因固定化與磺酸化的程序而改變。此外，由磁性與界面電位分析儀量測得知，所得磁性奈米粒子具有超順磁性，其等電點為2.45。而由傅立葉轉換紅外線光譜儀(FTIR)之分析可確認表面被覆PAA的氧化鐵奈米粒子已被磺酸化。

關於強酸型磁性奈米吸附劑在水溶液中吸附重金屬離子的研究，係在30℃下，以二價鈷離子作為研究範例。實驗結果顯示，強酸型磁性奈米吸附劑對Co2+的吸附具有很高的效率，其吸附行為遵守Langmuir恆溫吸附模式，最大吸附容量(qm)和Langmuir平衡常數(KL)分別為0.513 mmol•g -1與1.60 L•mmol-1；吸附量隨溶液的pH值增加而增加，當pH>4時，吸附量趨於一穩定值。另外，此吸附過程為一吸熱程序，其焓的變化量為3.65 kJ•mol-1。值得一提的是，Co2+的吸附程序可於2分鐘內完成。

關於強酸型磁性奈米吸附劑製備雙功能複合奈米粒子的研究，係先利用強酸型磁性奈米吸附劑吸附鎘離子，再以硫化鈉使鎘離子沈澱，便可在磁性奈米粒子表面形成硫化鎘量子點。實驗結果顯示，強酸型磁性奈米吸附劑對Cd2+的吸附，其吸附行為遵守Langmuir恆溫吸附模式，最大吸附容量(qm)和Langmuir平衡常數(KL)分別為0.503 mmol•g-1與1.05 L•mmol-1。穿透式電子顯微鏡(TEM)與高解析穿透式電子顯微鏡(HRTEM)之分析顯示，強酸型磁性奈米吸附劑的型態與大小，並沒有受到鎘離子之吸附與沈澱反應的影響；而吸附劑表面形成的CdS奈米晶體之大小約為1 nm。此外，X射線能量散射分析儀(EDX)也證實吸附劑表面有Cd及S的存在。由X射線繞射儀分析得知，磁性奈米粒子為四氧化三鐵之尖晶石結構，並不因鎘離子之吸附與沈澱反應而改變。此外，紫外光/可見光光譜儀(UV/Vis)與光致發光光譜儀(PL)分析皆顯示硫化鎘量子點的生成。

This dissertation concerns the application of polyacrylic acid (PAA)-coated magnetic nano-adsorbent in wastewater treatment and the preparation of sulfonated magnetic nanoparticles as a strong acid cation magnetic nano-adsorbent. The adsorption of methylene blue (MB) from an aqueous solution by PAA-bound iron oxide magnetic nanoparticles was studied. Then the PAA-coated magnetic nanoparticles were further sulfonated by sulfanilic acid via carbodiimide activation and used for the recovery of heavy metal ions from aqueous solution. Finally, a magnetic luminescent nanocomposite was obtained by the adsorption of metal ions on the sulfonated iron oxide nanoparticles and the subsequent precipitation with sodium sulfide.

The adsorption of methylene blue (MB) from an aqueous solution by PAA-bound iron oxide magnetic nanoparticles was studied. It was shown that the novel magnetic nano-adsorbent was quite efficient for the adsorption/desorption of MB. In the aqueous solution of MB at 25C, the adsorption data could be fitted by the Langmuir equation with a maximum adsorption amount of 0.199 mg•mg-1 and a Langmuir adsorption equilibrium constant of 10.1 mL•mg-1. The adsorption capacity increased with the increase in solution pH and reached a constant when pH > 7. The adsorption process was endothermic in nature with an enthalpy change (H) of 30.9 kJ•mol-1 at 10-40ºC. By using the methanol solution of acetic acid, the adsorbed MB could be desorbed. In addition, it was notable that both the adsorption and desorption of MB were quite fast and could be completed within 2 min due to the absence of internal diffusion resistance.

The strong acid cation magnetic nano-adsorbent was prepared by the sulfonation of PAA-coated magnetic nanoparticles via carbodiimide activation. Transmission electron microscopy (TEM) micrograph and dynamic light scattering (DLS) measurements showed that the sulfonated magnetic nanoparticles were mondisperse with a mean core diameter of 13.5 nm and a mean hydrodynamic diameter of 21 nm. X-ray diffraction (XRD) pattern indicated that the iron oxide nanoparticles were pure Fe3O4 with a spinel structure; it also revealed that the binding and sulfonation processes did not result in the phase change of Fe3O4 cores. In addition, the magnetic and zeta potential measurements showed that the sulfonated magnetic nanoparticles were superparamagnetic and the isoelectric point of the product was 2.45. The sulfonation of the PAA-coated magnetic nanoparticles was confirmed by FTIR analysis.

The adsorption of Co2+ ions from an aqueous solution by sulfonated magnetic nanoparticles was studied. It was shown that the novel magnetic nano-adsorbent was quite efficient for the adsorption of Co2+ ions. In the aqueous solution of Co2+ ions at 30C, the adsorption data could be fitted by the Langmuir equation with a maximum adsorption amount of 0.513 mmol•g-1 and a Langmuir adsorption equilibrium constant of 1.60 L•mmol-1. The adsorption capacity increased with the increase in solution pH and reached a constant when pH > 4. The adsorption process was endothermic in nature with an enthalpy change (H) of 3.65 kJ•mol-1 at 15-40ºC. In addition, it was notable that the adsorption of Co2+ ions were quite fast and could be completed within 2 min due to the absence of internal diffusion resistance.

The fabrication of magnetic luminescent nanocomposites via adsorption-precipitation of cadmium ions on sulfonated iron oxide nanoparticles was studied. In the aqueous solution of Cd2+ ions at 30C, the adsorption data could be fitted by the Langmuir equation with a maximum adsorption amount of 0.503 mmol•g-1 and a Langmuir adsorption equilibrium constant of 1.05 L•mmol-1. Transmission electron microscope micrograph of the magnetic luminescent nanocomposites showed that the morphologies were similar to that before the adsorption-precipitation of Cd2+ ions and the High resolution transmission electron microscope indicated the CdS nanocrystals of about 1 nm were formed on a sulfonated magnetic nanoparticle. In addition, the analysis of energy dispersive X-ray (EDX) spectrum revealed the presence of Cd and S on the particle surface. X-ray diffraction (XRD) pattern indicated that the iron oxide nanoparticles were pure Fe3O4 with a spinel structure; and the adsorption-precipitation processes do not result in the phase change of Fe3O4 cores. Both ultraviolet-visible (UV/Vis) and photoluminescence (PL) analyses confirmed the formation of magnetic luminescent nanocomposites.

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