含鈀中孔洞碳材於生質柴油高值化之催化研究

Catalytic Study on Palladium-Incorporated Mesoporous Carbon Materials for Upgrading of Biodiesel Fuel

潘俊宏(Jyun-Hong Pan)

指導教授 ： 楊家銘

國立清華大學/理學院/化學系所/碩士(2020年)

摘要

作為一種再生能源，生質柴油可以與石化柴油混合作為燃料，現已應用於歐洲、美洲、東南亞等地區的柴油車輛。生質柴油的使用可減少碳排放，然而在應用上仍存在成分調控問題，例如：由植物油或魚油製造的生質柴油，其組成具有高比例的多元不飽和脂肪酸甲酯，此成分碳鏈上的碳碳共軛雙鍵易被氧化，這會導致生質柴油儲存穩定性低、損壞車輛的引擎和排氣系統……等等問題，因此生質柴油的部分雙鍵氫化反應是重要的研究課題。本研究的目的在於製備負載鈀金屬的中孔洞碳材（Pd-OMC），並將之應用於催化商用棕櫚油衍生之生質柴油的部分氫化反應。Pd-OMC的合成以中孔洞二氧化矽平板狀SBA-15作為硬模板，改變碳化溫度和鈀負載量以調控Pd-OMC的結構表現，探討催化活性，並進一步探討改變催化反應溫度、反應壓力與金屬及生質柴油重量比對Pd-OMC催化此反應活性的影響。我們發現，碳化溫度為900 oC且鈀金屬負載量為1 wt% 的Pd-OMC對於此反應有最佳的活性，所轉化的產物為具有良好的氧化穩定性和冷流性質的單元不飽和脂肪酸甲酯，在90%的多元不飽和脂肪酸甲酯轉化率下，也具有最高單元不飽和脂肪酸甲酯選擇性。

關鍵字

生質柴油高值化 ； 部分氫化 ； 鈀催化劑 ； 有序中孔洞碳材

並列摘要

Biodiesel fuel (BDF) is one of renewable energy resources, and it has been blended with petroleum-based diesel and applied for diesel cars in Europe, America, and Southeast Asia. Ideally, the use of BDF in the transport sector can reduce CO2 emission. However, there are several technical problems for the usage of BDF. For example, BDFs produced from vegetable oils or fish fats contain high amounts of polyunsaturated fatty acid methyl esters (FAMEs), and the conjugated C=C double bonds on the carbon chains of FAMEs have low oxidation stability and degrade easily at the ambient condition. It leads to low storage stability, possible damage of engine and exhaust system of vehicles and other issues. A solution is partial hydrogenation of the C=C double bonds of FAMEs catalyzed by noble metals. In this report, palladium-incorporated ordered mesoporous carbons (Pd-OMC) were prepared and applied for partial hydrogenation of commercial palm oil-derived BDF (denoted as palm-BDF). Pd-OMC catalysts were prepared by the hard template method with different carbonization temperatures and Pd loadings using platelet SBA-15 as a template to control the pore structure and Pd distribution of Pd-OMC. The effects of reaction temperature (40 to 100 oC), reaction pressure (0.1 to 0.8 MPa) and metal/oil mass ratio on catalytic performance of Pd-OMC catalysts in partial hydrogenation of Palm-BDF were studied. The Pd-OMC with a carbonization temperature of 900 oC and Pd loading of 1 wt% gave the highest activity and selectivity in converting polyunsaturated FAMEs to monounsaturated FAMEs with good oxidation stability and cold flow properties even at a polyunsaturated FAMEs conversion of 90%.

並列關鍵字

Biodiesel fuel upgrading ； Partial hydrogenation ； Palladium catalyst ； Ordered mesoporous carbon

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