Synthesis Of Mesoporous Carbon-based Solid Acid And Its Structrue-property Relationship In The Raw Oil

Mesoporous materials possesses special structure and several fascinating properties,showing promising potential applications for environment,medical science,energy,and so on.In comparison with the traditional mesoporous that is widely studied,there are still many issues of mesoporous carbon that need further investigation.The structure and morphology are not abundance enough,the methods of synthesis are lack of change.Significant efforts have been devoted to the sulfonation of mesoporous carbons,and their extensive applications in catalysis have been reported,its structure-property relationship in the raw oil esterification reaction are not understood very well.Therefore,this thesis using PF as raw material,the mesoporous carbon material was synthesized by EISA method.The specific surface area,pore order and pore size of the catalyst were obtained.It focuses on the synthesis,structures and structure-property relationship of mesoporous carbon-based solid acid catalysis is of great significance for enriching the contents of mesoporous carbon and catalyzed gas-phase esterification reaction.The major results were as follows:(1)A series of catalysts have been prepared with various hydrocarbons via one-pot.Compared with other carbon sources,anaerobic fermentation residues solid acid has the best catalytic performance.The maximal esterification rate was 65.37%with the catalyst produced at sulfofication temperature of 110 ?,the reaction time of 120min and 30%sulfuric acid concentration.The results shows that porous carbon-based solid acid exhibit amorphous carbon structure.Therefore,the graphitization degree and sulfonation degree of these catalysts increased with increasing sulfonation time.The pore size of solid acid was mainly microporous.The conversion rate was 76.32%under optimal conditions of 80?,2h,methanol/oil molar ratio 8:1 and 4wt%catalyst.(2)A series of catalysts have been prepared with various carbon resource,via different ways and various templates.The results show ordered mesoporous carbons were synthesized through Evaporation induced Self-assembly method using phenol formaldehyde resin as carbon resource and F127 or F127/P123 as template.Reaction conditions as follows:reaction temperature 110?,catalyst 3wt%,reaction time 90min.The catalyst conversion rate was the highest via EISA.The catalyst by hydrothermal synthesis,then the conversion rate of 91.50%.When the mixed template F127/P123 was mixed with 2:1,the activity of the catalyst was better than that of F127 alone,and the conversion was 95.10%.Therefore,EISA was the best method,and phenol resin was the best precursor.(3)The catalyst prepared at 75 ? had the best order,the specific surface areas were 677.97m~2/g,The corresponding pore sizes were 2.0.The longer the synthesis time,the better the orderliness of the catalyst.With the increase of heating rate,the order of catalyst is getting worse.The catalyst was prepared by changing the ratio of mixed template F127/P123,the best ratio was 2:1.(4)The optimum reaction conditions for the combination of gaseous esterification and the catalyst with specific surface area of 677.97m~2/g as follow:The conversion rate was 95.48%under optimal conditions of 110?,120min,3wt%catalyst.The catalytic activity of mesoporous carbon-based solid acid was significantly higher than anaerobic fermentation residue solid acid,and the conversion rate of mesoporous carbon-based solid acid catalyst reached 95.48%,while other was only 76.31%.Therefore,increase of mesopore channels was beneficial to the esterification reaction.From the analysis of the structure-activity relationship of the catalyst,the orderly structure of the catalyst has certain influence on the reaction rate and conversion rate.With the increase of the specific surface area,the conversion rate basically showed an upward trend.The effect of pore size on the conversion rate is not significant or basically unaffected.