NiCu/SiO₂和NiCuMo/SiO₂催化剂作用下松树乙醇木质素在超临界乙醇介质中的解聚

IF 0.5 Q4 CHEMISTRY, MULTIDISCIPLINARY Journal of Siberian Federal University. Chemistry Pub Date : 2020-06-01 DOI:10.17516/1998-2836-0179
А.В. Мирошникова, С.В. Барышников, Ю.Н. Маляр, В. А. Яковлев, О.П. Таран, Л. Дьякович, Борис Николаевич Кузнецов, A. Miroshnikova, S. V. Baryshnikov, Y. Malyar, V. Yakovlev, O. Taran, L. Djakovitch, B. Kuznetsov
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引用次数: 0

摘要

研究了在250 ~ 400℃范围内NiCu/ SiO2和NiCuMo/SiO2催化剂存在下,超临界乙醇中松乙醇木质素的热催化转化规律。采用元素分析和凝胶渗透色谱法(GPC)研究了乙醇木质素的组成和结构及其转化的液体和固体产物。气相色谱法测定气体产物的组成。在250℃的工艺温度下,催化剂对乙醇木质素的转化无显著影响。在含钼量为8.8 wt. %的NiCuMo/SiO₂催化剂存在下,反应温度为300℃时,液相产物的最大产率为83.5 wt. %。在350℃的温度下,NiCu/ SiO2和NiCuMo/SiO2催化剂使乙醇木质素几乎完全转化为液体和气体产物,固体产物的收率不超过1wt . %。在催化转化的液体产物中,由于木质素的脱氧和加氢反应及其解聚产物的催化强化,与初始乙醇木质素相比,O/C原子比降低,H/C原子比增加。根据300℃下乙醇木质素热催化转化液产物分子质量分布(MMD)曲线的GPC数据,在160和380 Da处存在峰值,可能分别与导环单体和二聚物有关。通过比较300℃下乙醇木质素解聚液体产物在NiCu/SiO₂和NiCuMo/SiO₂催化剂上的MMD可知,在催化剂中引入钼促进了单体愈创木酰产物的形成
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Depolymerization of Pine Ethanol Lignin in the Medium of Supercritical Ethanol in the Presence of Catalysts NiCu/SiO₂ and NiCuMo/SiO₂
The regularities of thermocatalytic transformation of pine ethanol lignin in supercritical ethanol in the presence of catalysts NiCu/SiO₂ and NiCuMo/SiO2 in the temperature range 250–400 °C were established. The composition and structure of ethanol lignin, liquid and solid products of its conversion were studied by methods of elemental analysis and gel-permeating chromatography (GPC). The composition of gaseous products – by method of gas chromatography. At the process temperature of 250 °C the catalysts do not have a significant effect on conversion of ethanol lignin. The maximal yield of liquid products (83.5 wt. %) was obtained at temperature 300 °C in the presence of catalyst NiCuMo/SiO₂ containing 8.8 wt. % of molybdenum. At temperature 350 °C NiCu/SiO₂ and NiCuMo/SiO2 catalysts contribute to the almost complete conversion of ethanol lignin into liquid and gaseous products, and the yield of solid products does not exceed 1 wt. %. In liquid products of catalytic conversion there is a decrease in the atomic ratio of O/C and the increase of H/C atomic ratio as compared to initial ethanol lignin due to catalytic intensification of reactions of deoxygenation and hydrogenation of lignin and products of its depolymerization. According to GPC data on the curves of molecular mass distribution (MMD) of liquid products of thermocatalytic conversion of ethanol lignin at 300 °C there are peaks with highs at 160 and 380 Da, probably related to guiacyle monomers and dimmers, respectively. From the comparison of MMD of liquid products obtained by ethanol lignin depolymerization at 300 °C over catalysts NiCu/SiO₂ and NiCuMo/SiO₂ it follows, that the introduction of molybdenum in the catalyst promotes the formation of monomeric guaiacyl products
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