溶胶-凝胶法制备ZSM-5-Al<sub>2</sub> o>3</sub>-TiO<sub>2</sub>-复合材料负载Pt/NiMo硫化物催化剂对大豆油的脱氢环裂解

IF 0.2 Q4 ENERGY & FUELS Journal of The Japan Institute of Energy Pub Date : 2023-10-20 DOI:10.3775/jie.102.110
Yuuya HAYASHI, Tadanori HASHIMOTO, Atsushi ISHIHARA
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引用次数: 0

摘要

采用zsm -5- al2o3 - tio2 -复合负载Pt、Ni、Mo硫化物催化剂,在1.0 MPa氢气条件下,在420 ~ 580℃范围内对大豆油进行脱氢环裂解反应。Pt/NM/Z(24)75Ti(500sg) (N=Ni, M=Mo, Z=ZSM-5, 24=SiO2/Al2O3, 75=重量比,Ti=TiO2, 500=煅烧温度,sg=溶胶-凝胶法)和Pt/NM/Z(24)75Ti(600sg)在该反应中表现出比单一使用Al2O3和TiO2的捏合法制备的催化剂更高的活性和更高的芳香收率。其中,捏合法制备的Pt/NM/Z(24)30Al30Ti和溶胶-凝胶法制备的Pt/NM/Z(24)75Al(600sg)的芳烃产率最高,达到15%。结果表明,TiO2在复合载体上的加入会促进硫化钼与TiO2的相互作用,激活氢,导致甘油三酯酯基的裂解和烃碎片的环化。采用溶胶-凝胶法制备时,不仅含有TiO2,而且含有Al2O3的催化剂均表现出较高的芳烃产率。Pt/NM/Z(24)75Ti(500sg)和Pt/NM/Z(24)75Ti(600sg)抑制了气态产物的生成,而Pt/NM/Z(24)30Al30Ti和Pt/NM/Z(24)75Al(600sg)增加了气态产物的生成,说明芳烃的生成机理可能不同。前者通过长链烃片段的直接环化生成芳烃,而后者通过气化生成C2-C4烯烃并由烯烃的Diels-Alder反应连续环化生成芳烃。
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Dehydrocyclization-cracking of Soybean Oil Using Pt/NiMo Sulfide Catalysts Supported on Hierarchical ZSM-5-Al<sub>2</sub>O<sub>3</sub>-TiO<sub>2</sub>-composite Prepared by Sol-gel Method
Hierarchical ZSM-5-Al2O3-TiO2-composite supported Pt, Ni and Mo sulfides catalysts were used for the dehydrocyclization-cracking of soybean oil at 1.0 MPa of hydrogen in the range 420-580 °C. Pt/NM/Z(24)75Ti(500sg) (N=Ni, M=Mo, Z=ZSM-5, 24=SiO2/Al2O3, 75=weight ratio, Ti=TiO2, 500=cal-cination temp. °C, sg=sol-gel method) and Pt/NM/Z(24)75Ti(600sg) prepared by the sol-gel method exhibited the higher activity in this reaction and the higher aromatics yields than the catalysts with single use of Al2O3 and TiO2 prepared by the kneading method. Further, Pt/NM/Z(24)30Al30Ti prepared by the kneading method and Pt/NM/Z(24)75Al(600sg) prepared by the sol-gel method exhibited the highest aromatics yield of 15% among the catalysts tested. The result indicated that the addition of TiO2 to the composite support would promote the interaction between molybdenum sulfide and TiO2, activate hydrogen and lead to enhanced cracking of ester group of triglyceride and cyclization of hydrocarbon fragments. When the sol-gel method was used, the catalysts with not only TiO2 but also Al2O3 exhibited the higher aromatics yields. Pt/NM/Z(24)75Ti(500sg) and Pt/NM/Z(24)75Ti(600sg) inhibited the formation of gaseous products while Pt/NM/Z(24)30Al30Ti and Pt/NM/Z(24)75Al(600sg) increased gaseous products, suggesting that the mechanism of aromatics formation might be different, and that the former would produce aromatics through the direct cyclization of longer-chained hydrocarbon fragments while the latter would produce them through gasification to C2-C4 olefins and the successive cyclization by the Diels-Alder reaction of olefins.
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