從水和廢水中去除磷酸鹽是控制優養化的關鍵步驟，而吸附技術是其中最有效的處理過程。本研究合成了一系列不同鍛燒溫度 (300至1000℃)下的檸檬酸改質氧化鑭 (c-La2O3)，並透過X射線繞射、N2吸附-脫附、動態光散射 (DLS)、熱重分析、X 射線光電子能譜 (XPS)、傅立葉轉換紅外光譜和高解析度穿透式電子顯微鏡 (HR-TEM)進行偵測。與原始La2O3相比，c-La2O3表現出更好的磷酸鹽吸附性質。吸附容量與pH值和鍛燒溫度成反比。在吸附動力學中，c-La2O3符合擬二級動力學模型，R2大於0.96，顯示c-La2O3與磷酸鹽之間的反應為化學吸附。 Langmuir模型可以更好地描述c-La2O3的吸附等溫曲線，顯示吸附過程是單層吸附。在pH 5條件下，300°C鍛燒的無晶形c-La2O3 (c-La-300)具有最高的比表面積，並擁有最高的最大吸附容量141 mg/g，與之相比c-La-800為79 mg/g，而原始La2O3為 43 mg/g。熱力學研究顯示，吸附反應為自發吸熱過程 (∆H0 = 1.02 kJ/mol, ∆S0 = 21 J/(mol K))。此外，在吸附過程中，氫氧根離子會釋放到溶液中，提高溶液的pH值，這可以透過H2PO4-、HPO42-或PO43-和c-La-300表面之羥基間的配位基交換描述。

關鍵字：優養化、氧化鑭、磷酸鹽、檸檬酸、單層吸附、化學吸附、擬二級動力學模式、朗繆爾模型

The removal of phosphate from water and wastewater is the key step to control eutrophication, and adsorption technology is one of the most effective treatment processes. In this study, a series of citric acid modified lanthanum oxides (c-La) under different calcination temperatures (300 to 1000 C) were synthesized and characterized by X-ray diffraction, N2 adsorption-desorption, dynamic light scattering (DLS), thermogravimetric analysis, Fourier transform infrared spectroscopy, and high-resolution transmission electron microscopy (HR-TEM). The c-La exhibited a better phosphate adsorption performance, as compared with pristine La2O3. The adsorption capacity was inversely correlated with pH and calcination temperature. In adsorption kinetics, c-La was fitted well in pseudo-second-order kinetic model with R2 larger than 0.96, suggesting that the reaction between c-La and phosphate is chemisorption. The adsorption isotherms of c-La could be better represented by Langmuir model, indicating that the adsorption process is a monolayer homogenous adsorption. At pH 5, the amorphous c-La sintered at 300C (c-La-300) had the highest specific surface area, and showed the greatest maximum adsorption capacity at 141 mg/g, comparing with the crystalline c-La sintered at 800C (c-La-800) at 79 mg/g and pristine La2O3 at 43 mg/g. The thermodynamic study indicated that the adsorption reaction was a spontaneous endothermic process with H = 3.52 kJ/mol and S = 21 J/(mol K). Furthermore, the hydroxyl ions would be released to the solution during adsorption process and increase the pH value of the solution, which could be described by the ligand exchange of hydroxyl groups on the surface of adsorbent between H2PO4-, HPO42-, or PO43-.

Keywords: Eutrophication; Lanthanum oxide; Phosphate; Citric acid; Chemisorption; Pseudo-second-order kinetic model; Langmuir model; Monolayer adsorption

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