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標題: 類水滑石化合物添加過渡金屬作為鹼性觸媒與轉酯化反應生成生質柴油之應用
Hydrotalcite-like compounds containing transition metals as solid base catalysts for transesterification and application for biodiesel production
作者: 王譽賓
Wang, Yu-Bin
關鍵字: Hydrotalcite compounds;水滑石化合物;Hydrotalcite-like compounds;transesterification;biodiesel;類水滑石化合物;轉酯化反應;生質柴油
出版社: 化學工程學系所
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本研究是利用共沉澱法製備出添加含過渡金屬(Ni2+、Fe3+)之類水滑石(Hydrotalcite-Like Compounds, HTLCs)的層狀氫氧雙層化合物(Layerd double hydroxide, LDH)鹼性觸媒,MgAlNi-HTLCs與MgAlFe-HTLCs,將MgAlNi-HTLCs與MgAlFe-HTLCs在固定Al的含量分成四種不同MgAl與過渡金屬的莫耳比,Mg16Al8.5Ni1、Mg12Al6.5Ni1、Mg8Al4.5Ni1、Mg4Al2.5Ni1;Mg15Al8Fe1、Mg12Al6.5Fe1、Mg9Al5Fe1、Mg6Al3.5Fe1、並將M2+/(M2++M3+)~0.33,藉以探討添加過渡金屬對轉酯化反應之影響。MgAlNi在773 K下鍛燒10 h、MgAlFe在873 K下鍛燒16 h後,將此兩種含過渡金屬(MgAlNi與MgAlFe )之類水滑石化合物鹼性觸媒作為大豆油與甲醇之轉酯化反應上生成生質柴油之應用,並以FE-SEM、BET、XRD、TGA、CO2-TPD、FT-IR來分析MgAlNi與MgAlFe類水滑石化合物鹼性觸媒的物理與化學特性。分析結果發現類水滑石化合物鹼性觸媒的鹼性強度與Mg2+的含量有關,Mg2+的含量越多則鹼性越強,轉化率越高。在轉化率的表現上,添加過渡金屬後所形成的MgAlNi與MgAlFe類水滑石化合物鹼性觸媒也較未添加過渡金屬的水滑石化合物觸媒(Mg3Al)來得高。在Mg16Al8.5Ni1、Mg15Al8Fe1此兩種莫耳比下之觸媒,反應溫度65℃、攪拌轉速1200 rpm、醇油比21:1、反應時間4 h、觸媒添加量3 wt%,可以達到87%與81%的脂肪酸甲酯轉化率,而觸媒經過NH4OH與甲醇清洗、烘乾再鍛燒後,在重複使用性上也可以重複使用3次仍然有83%與78%的脂肪酸甲酯轉化率。

In this study, Hydrotalcite-like compounds (HTLCs) containing transition metals Ni2+ and Fe3+ layerd double hydroxide (LDH) MgAlNi and MgAlFe base catalysts were synthsized by co-precipitation method. The Mg2+、Al3+、Ni2+ and Fe3+ molar ratio varied over the range from Mg16Al8.5Ni1、Mg12Al6.5Ni1、Mg8Al4.5Ni1、Mg4Al2.5Ni1 of the MgAlNi and Mg15Al8Fe1、Mg12Al6.5Fe1、Mg9Al5Fe1、Mg6Al3.5Fe1 of the MgAlFe catalysts at a constant Al amount in M2+/(M2++M3+) is about 0.33 in the Hydrotalcite-like compounds to evaluate the conversion of the transesterification. The MgAlNi-HTLCs calcined at 773 K for 10 h and MgAlFe-HTLCs calcined at 873 K for 16 h have performed as base catalysts for transesterification of soybean oil with methanol to produce biodiesel, and the catalysts were characterized by FE-SEM, BET, XRD, TGA, CO2-TPD, FT-IR to evaluate the physical and chemical properties of the catalysts. The results have indicated that the basicity of the catalysts were related to the Mg2+ content, and the basicity increases with increasing Mg2+ content. From GC analysis, the conversion of containing transition metals of MgAlNi-HTLCs and MgAlFe-HTLCs were higher than the hydrotalcite compound(Mg3Al) without transition metals. The optimum reaction conditions were obtained with a methanol/oil molar ratio of 21, 3% catalyst (w/w oil), and 1200 rpm stirring speed for 4 h at 338K, and results in the highest FAME conversion for 87% of Mg16Al8.5Ni1 and 81% of Mg15Al8Fe1. The performance of the two previous catalysts of the three times reaction cycles with washing by NH4OH and methanol and following the drying and calcination procedures maintains at 83% and 78% conversion, respectively.
其他識別: U0005-1001201211534800
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