Preparation Of Cu(Ⅱ)-doped Functionalized Mesoporous Silicon Materials And Their Catalytic Oxidation Performance For Tetrali

Since the high specific surface area of mesoporous silicon materials and rich silicon hydroxyl groups,it has attracted extensive attention from researchers in recent years.As we know the hydroxyl group on its surface is easy to modify,it can synthesize a new type of catalyst,and it is not easy to gather in the solvent,which is easy to recycle.Research shows that functional mesoporous silicon materials effectively broaden their application scope in various fields.In this paper,the mesoporous silicon material is modified by different silane coupling agents,and the silicon-based copper-containing catalyst is synthesized by Cu（II）to explore its catalytic performance.The main research content is divided into the following three parts.（1）Through the one-step modification of silane coupling agent 3-aminopropyltriethoxysilane（APTES）,three functionalized silicon-based copper-containing catalysts with silica gel,MCM-41 and attapulgite（ATP）as carriers were synthesized,and the structure characterization and catalytic activity test were studied.Experiments show that the Silica Gel-NH₂-Cu has the best catalytic performance among the three catalysts.Through the exploration of the reaction conditions such as temperature,catalyst dosage,reaction time,molar ratio between substrate and oxidant,the optimal conditions for catalyst Silica Gel-NH₂-Cu for catalytic oxidation of tetralin are obtained:0.5 m L tetralin,100 mg catalyst,3 m L tert-butyl hydrogen peroxide（TBHP）,80°C,8 h.Under this condition,the conversion rate of tetralin and the selectivity of tetralone reached 94.64%and 90.10%respectively.The catalytic system still has good catalytic activity after 3 times of reuse.（2）Through the two-step modification of silane coupling agent triethylenetetramine（TETA）,three functionalized silicon-based copper-containing catalysts with silica gel,MCM-41 and attapulgite（ATP）as carriers were synthesized,and their structure was characterized and research on catalytic activity testing.Experiments show that the MCM-41-Cl@TETA-Cu has the best catalytic performance among the three catalysts.Through the exploration of the reaction conditions such as temperature,catalyst dosage,reaction time,molar ratio between substrate and oxidant,the optimal conditions for catalyst MCM-41-Cl@TETA-Cu for catalytic oxidation of tetralin are obtained:0.5 m L tetralin,100 mg catalyst,2.4 m L tert-butyl hydrogen peroxide（TBHP）,80°C,6 h.Under this condition,the conversion rate of tetralin and the selectivity of tetralone reached 80.58%and 58.72%respectively.After the catalyst MCM-41-Cl@TETA-Cu is reused for 3 times,the activity remains basically unchanged and has good stability.（3）Through the one-step modification of silane coupling agent（3-chloropropyl）trimethoxy silane（CPTMS）,three functionalized silicon-based copper-containing catalysts with silica gel,MCM-41 and attapulgite（ATP）as carriers were synthesized,and the structure characterization and catalytic activity test were studied.Experiments show that the ATP-Cl-Cu has the best catalytic performance among the three catalysts.Through the exploration of the reaction conditions such as temperature,catalyst dosage,reaction time,molar ratio between substrate and oxidant,the optimal conditions for catalyst ATP-Cl-Cu for catalytic oxidation of tetralin are obtained:0.5 m L tetralin,100mg catalyst,3 m L tert-butyl hydrogen peroxide（TBHP）,80°C,4 h.Under this condition,the conversion rate of tetralin and the selectivity of tetralone reached 87.15%and 60.85%respectively.After the catalytic system is reused for 3 times,the selectivity of tetralone is basically stable,indicating that the catalyst ATP-Cl-Cu has a certain stability.In a word,this paper uses three different silane coupling agents to modify the mesoporous silicon material,and through catalytic performance evaluation,the optimal catalysts under the modification of different silane coupling agents are selected,they are Silica Gel-NH₂-Cu,MCM-41-Cl@TETA-Cu and ATP-Cl-Cu,respectively,and optimizes the reaction conditions of three catalysts catalyzing tetralin oxide,which can provide an experimental basis for the design and preparation of low-cost and efficient chemical reaction mesoporous catalysts,and which has certain practical application value in the development of the green chemical industry.