本研究探討含銅層狀矽酸鹽觸媒衍生之銅觸媒與商化銅觸媒應用於己二酸催化為己二醇。合成搭載不同重量百分比之含銅層狀矽酸鹽與商化觸媒比較其物化性的差異對反應性之影響。觸媒的物化性鑑定包括:氮氣物理吸附(N2 physisorption)、X-ray繞射圖譜(XRD)、紅外光光譜分析(IR)、應耦合電漿原子發射光譜分析(ICP-AES)、穿透式電子顯微鏡(HR-TEM)、吡啶吸附紅外光譜分析(Pd-IR)、氫氣程溫還原反應(H2-TPR)、一氧化碳的化學吸附(CO chemisorption)、一氧化碳程溫脫附(CO-TPD)以及氨氣的程溫脫附反應 (NH3-TPD)。
本實驗以氨氣蒸發-水熱法來合成不同重量百分比的含銅層狀矽酸鹽，比較相同重量百分比之銅觸媒發現含銅層狀矽酸鹽衍生之觸媒具有較高的反應活性，可歸因於表面活性點較多與Cu+/Cu0比例較高。利用批次式反應器於240 oC及58 bar 氫氣壓力下進行己二酸加氫脫氧，發現觸媒物化性差異也反應在活性測試上；隨著擔載量的上升，其反應活性也隨之增加。經由產物分佈圖來建立己二酸轉化為己二醇之反應路徑圖，並探討己二酸加氫轉化之機制，利用Langmuir–Hinshelwood–Hougen–Watson (LHHW)模型來擬合，可求得己二酸的平衡速率常數略大於己內酯之平衡速率常數。由於己二酸為反應物，佔據了所有活性點，當己二酸接近百分之百轉化後，才有空出的活性點能與衍生之產物反應。

The aim of this study is to understand copper phyllosilicates derived silica-supported copper (10 wt%, 20 wt%, and 30 wt%) catalysts tested in direct hydrogenation of AA to HDOL. Different weight loading of copper phyllosilicates were used to compare the effects of differences in physicochemical properties on reactivity. Catalyst characterizations, including N2 physisorption, XRD, TEM, and H2-TPR were performed. Copper phyllosilicates catalysts were prepared by ammonia evaporation hydrothermal method. The turnover frequency calculated based on the HDOL production rate per Cu+ site of a Cu-based catalyst derived from phyllosilicate was higher than its counterpart synthesized by impregnation using similar Cu loadings (ca. 20 wt%). Moreover, catalyst reuse tests showed that phyllosilicate derived Cu/SiO2 had better recyclability than its impregnated counterpart, possibly due to stronger interaction between Cu and silica support of the former. Based on the product distribution, a plausible reaction network of hydrogenation of AA was proposed. Furthermore, kinetic analyses by resorting to a global reaction model and to the Langmuir–Hinshelwood–Hougen–Watson (LHHW) formalism were conducted. The latter is more appropriate than the former to portray the experimental results because the possible existence of competitive adsorption between AA and ε-caprolactone.

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