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二氧化硅改性分子筛催化生物质基多元醇制备对二甲苯
引用本文:王声飞,范明慧,何雨婷,李全新.二氧化硅改性分子筛催化生物质基多元醇制备对二甲苯[J].化学物理学报,2019,32(4):513-520.
作者姓名:王声飞  范明慧  何雨婷  李全新
作者单位:中国科学技术大学化学物理系,中国科学院城市污染物转化重点实验室,安徽省生物质洁净能源重点实验室,合肥 230026,中国科学技术大学化学物理系,中国科学院城市污染物转化重点实验室,安徽省生物质洁净能源重点实验室,合肥 230026,中国科学技术大学化学物理系,中国科学院城市污染物转化重点实验室,安徽省生物质洁净能源重点实验室,合肥 230026,中国科学技术大学化学物理系,中国科学院城市污染物转化重点实验室,安徽省生物质洁净能源重点实验室,合肥 230026
摘    要:本文证明了在二氧化硅改性的分子筛催化作用下,生物质基多元醇(如山梨醇、木糖醇、赤藓糖醇、甘油和乙二醇)可以经过催化裂解、烷基化和异构化等反应,生成高附加值的化学品(对二甲苯).与HZSM-5分子筛催化剂相比,二氧化硅改性的分子筛降低了分子筛催化剂的外表面酸和孔径,从而显著的提高对甲苯的选择性和产率.本文详细讨论了催化剂、甲醇添加剂、反应温度和不同类型多元醇原料对对二甲苯选择性和产率的影响.甲醇的添加促进多元醇催化裂解中的烷基化反应,提高了二甲苯的产率.在15%SiO_2/HZSM-5催化剂作用下,对二甲苯的产率最高可达到10.9 C-mol%,对二甲苯在二甲苯中选择性达到91.1%.本文通过研究相关重要反应和催化剂特性,揭示了生物质基多元醇催化裂解制备对二甲苯的反应路径.

关 键 词:生物质基多元醇,对二甲苯,催化转化,二氧化硅改性的分子筛
收稿时间:2019/1/26 0:00:00

Catalytic Conversion of Biomass-Derived Polyols into Para-xylene over SiO2-Modified Zeolites
Sheng-fei Wang,Ming-hui Fan,Yu-ting He and Quan-xin Li.Catalytic Conversion of Biomass-Derived Polyols into Para-xylene over SiO2-Modified Zeolites[J].Chinese Journal of Chemical Physics,2019,32(4):513-520.
Authors:Sheng-fei Wang  Ming-hui Fan  Yu-ting He and Quan-xin Li
Affiliation:Department of Chemical Physics, CAS Key Laboratory of Urban Pollutant Conversion, Chinese Academy of Sciences, Anhui Key Laboratory of Biomass Clean Energy, University of Science and Technology of China, Hefei 230026, China,Department of Chemical Physics, CAS Key Laboratory of Urban Pollutant Conversion, Chinese Academy of Sciences, Anhui Key Laboratory of Biomass Clean Energy, University of Science and Technology of China, Hefei 230026, China,Department of Chemical Physics, CAS Key Laboratory of Urban Pollutant Conversion, Chinese Academy of Sciences, Anhui Key Laboratory of Biomass Clean Energy, University of Science and Technology of China, Hefei 230026, China and Department of Chemical Physics, CAS Key Laboratory of Urban Pollutant Conversion, Chinese Academy of Sciences, Anhui Key Laboratory of Biomass Clean Energy, University of Science and Technology of China, Hefei 230026, China
Abstract:This work proved that biomass-based polyols (sorbitol, xylitol, erythritol, glycerol and ethanediol) were able to be converted into high-value chemical (p-xylene) by catalytic cracking of polyols, alkylation of aromatics, and the isomerization of xylenes over the SiO2-modified zeolites. Compared to the conventional HZSM-5 zeolite, the SiO2-containing zeolites considerably increased the selectivity and yield of p-xylene due to the reduction of external surface acidity and the narrowing of pore entrance. The influences of the methanol additive, reaction temperature, and types of polyols on the selectivity and yield of p-xylene were investigated in detail. Catalytic cracking of polyols with methanol significantly enhanced the production of p-xylene by the alkylation of toluene with methanol. The highest p-xylene yield of 10.9 C-mol% with a p-xylene/xylenes ratio of 91.1% was obtained over the 15wt%SiO2/HZSM-5 catalyst. The reaction pathway for the formation of p-xylene was addressed according to the study of the key reactions and the characterization of catalysts.
Keywords:Biomass-derived polyols  Para-xylene  Catalytic conversion  SiO2-modified HZSM-5
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