臺灣博碩士論文加值系統

石材工業產生大量廢棄物的問題不僅影響環境，且還影響資源維護及廢棄物管理問題。本研究所使用之大理石污泥和石灰石污泥被認為是具環境吸引力及再利用的基本特徵。目前正在進行一項研究，將這種副產品與工業應用互相結合。因此，本研究的目的是將石灰石污泥和大理石污泥藉由水熱技術轉化為奈米HA晶體，並有效控制HA晶體的尺寸和形態，應用於水介質中去除Pb和Cu的吸附劑。經水熱合成之氫氧基磷灰石由XRD分析顯示，結晶度為98.48-99.54%，顯示出其具良好結晶性能。由SEM及TEM分析，可觀察到其呈現棒狀型態，並且交錯堆疊，形成許多微孔結構，晶體長度約為114-201 nm。此外，藉由氮氣吸脫附曲線得知氫氧基磷灰石具有H3磁滯迴線的典型IUPAC IV型等溫線，顯示N2於中孔產生毛細管冷凝，其平均孔徑為10.25-20.45 nm。藉由BET得知表面積和總孔體積為74.69-115.04 m2/g和0.5339 cm3/g。以Langmuir等溫吸附模型相較於其他模型具較佳相關性，其相關性R2為0.98-0.99。經Langmuir擬合之結果得知，其所合成氫氧基磷灰石最大吸附量為245.87 mg/g，對於人工廢水之去除率高達99%。熱力學分析顯示該過程是熱力學自發和吸熱過程。動力學研究顯示，吸附過程遵循偽二階模型，總吸附速率受膜擴散作為主導機制。

The problem of the large amounts of waste products deriving from stone industrial affects not only the environmental impact but also the resources maintenance and the problem of waste management. This study presents the essential features of an environmentally attractive reuse of what is currently considered limestone sludge and marble sludge. A research is currently carried out in order to join this by-product with possible industrial. Accordingly, the aim of this study is to convert limestone sludge and marble sludge into nanocrystalline HA and to achieve control over the size and morphology of the HA crystals by hydrothermal technique, and utilize as an adsorbent for the removal of Pb and Cu from aqueous media. X-ray diffraction analysis confirmed that all powders were composed of a hydroxyapatite phase. The powders were of crystallinity (Xc =98.48-99.54%) The surface morphologies of the hydroxyapatite were examined via SEM and TEM analysis. That consist of aggregates of rod-shaped nanoparticles with a narrow size distribution. That the actual size of the precipitated crystals were 114-201 nm in length. The hydroxyapatite was classified as a typical IUPAC type-IV isotherm with an H3 hysteresis loop, indicating a mesoporous structure based on capillary condensation of N2 in mesopores, which was also confirmed by the measured average pore diameter of 10.25-20.45 nm. The BET surface area and total pore volume of the HAP were estimated to be 74.69-115.04 m2/g and 0.5339 cm3/g. Langmuir isotherm model (R2=0.98-0.99) seems to be the most accurate model and provides a better description for the equilibrium data compared to the other models. According to the Langmuir fitting, the theoretical maximum adsorption capacity was found to be 245.45 mg/g, and more than 99% of Artificial wastewater can be removed by the Hydroxyapatite. Thermodynamic analysis indicated that the process is thermodynamically spontaneous and endothermic process. Kinetic studies revealed that the adsorption process follows the pseudo-second-order model and that the overall adsorption rate is controlled by film diffusion as the dominant mechanism.

摘要 I
Abstract II
誌謝 III
目錄 IV
圖目錄 V
表目錄 VIII
第一章 前言 1
1-1研究緣起 1
1-2研究目的與內容 2
第二章 文獻回顧 3
2-1石灰石污泥之來源特性與處置再利用 3
2-2大理石污泥之來源特性與處置再利用 14
2-3氫氧基磷灰石之結構性質及應用 19
2-4磷酸鹽之性質與高溫特性 26
2-5吸附理論 29
第三章 實驗材料設備與方法 36
3-1實驗流程 36
3-2實驗材料 37
3-3研究設備 38
第四章 結果與討論 46
4-1材料基本物化特性分析 46
4-2不同Ca/P莫耳比及不同水熱溫度分析 52
4-3合成氫氧基磷灰石之微觀結構 70
4-4水熱合成氫氧基磷灰石之孔洞分析 80
4-5合成氫氧基磷灰石之NMR圖譜分析 88
4-6水熱合成氫氧基磷灰石之吸附動力曲線分析 94
4-7合成之氫氧基磷灰石等溫吸附分析 108
4-8吸附熱力學 129
第五章 結論與建議 134
5-1結論 134
5-2建議 135
參考文獻 136

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