Design And Application Of High Efficiency Metal Catalysts In Hydrogenolysis

Catalysis is the decrease in the activation energy due to the participation of asubstance called a catalyst and thereby increases the rate of chemical reaction withoutchange in the quality and quantity of catalyst during the reaction. Study and usecatalysts can greatly reduce the cost of product, improve product quality, protect theenvironment and make rational use of resources. The preparation of catalysts with anefficient activity and unique selectivity become one of the main directions of researchamong the scientists. This thesis devotes to the synthesis of highly effective catalystwith large surface area, high catalytic activity and selectivity by the nanomaterialspreparation technology.The first part of this thesis modulates the reaction conditions of hydrogenolysisof glycerol to1,2-PDO in the autoclave. Considering the limit of reaction scale, wedesign to largen the reaction scale for the second part. In the second part of the study,we design a series of Pt-based solid acid catalysts and investigated the reactionconditions for hydrogenolysis of glycerol to1-PO in the fixed-bed reactor. The lastpart of the study is the design of a series Pt-Ag bimetallic solid acid catalysts on thebasis of results of part two. The main content of the thesis is as follow:(1)We adopt co-precipitation to prepare a series of hydrotalcite-like compoundswith different Mg-Al ratio. Ru-Cu based catalysts are obtained by calcination andreduction and investigated the catalytic hydrogenolysis performances of glycerol. Onthe other hand, we optimized the operating conditions for the hydrogenolysis ofglycerol, such as reaction temperature, hydrogen pressure, catalyst loading, Ru-Curatio and so on. At the same time, the structure of the catalysts and the reactions werefurther studied by means of a variety of characterization methods.(2)A series Pt-based catalysts supported on different metal oxides(W03-Zr02,W03-Al203,W03-Ti02,W03-Si02) were prepared by sequentiallyincipient wetness impregnation and investigated the catalytic performance for thehydrogenolysis of glycerol to1-PO. Pt/WOi-ZrOz showed the best activity for thereaction and it has the largest active surface area and acid amount. The conversion ofglycerol can reach over99%and the selectivity to1-PO can reach over90%by using Pt/W03-Zr02as catalyst at the reaction temperature of160°C and the hydrogenpressure of2.5MPa. After reaction for160hours, the catalyst still showed goodactivity,(3) A series Pt-Ag bimetal catalysts supported on\VO3-ZrO2were prepared bysequentially incipient wetness impregnation on the basis of the results in part two andused as catalysts for the hydrogenolysis of glycerol to1,3-PDO. We investigated theeffect of WO3content, Pt loading，ratio of Pt to Ag，and the concentration of glycerolsolution on the catalytic performances. The highest activity was achieved at WO3content of39.2%, Pt loading of2wt%, and Pt:Ag=1:0.2. When the reactiontemperature is180°C, the hydrogen pressure is5.5MPa, and the concentration ofglycerol solution is80wt%，a conversion of glycerol more than52.7%and47%selectivity to1,3-PDO can be achieved within12h.