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作 者:杨勇[1,2] 汤吉海[1] 陈献[1] 费兆阳[1,3] 崔咪芬[1] 乔旭[1,3]
机构地区:[1]南京工业大学化学化工学院,江苏南京210009 [2]淮阴工学院生命科学与化学工程学院,江苏淮安223001 [3]材料化学工程国家重点实验室南京工业大学,江苏南京210009
出 处:《石油化工》2014年第11期1253-1258,共6页Petrochemical Technology
摘 要:采用沉淀-浸渍法制备了Ti O2/Si O2催化剂,并将其用于催化碳酸二甲酯(DMC)与碳酸二苯酯(DPC)逆歧化制备甲基苯基碳酸酯(MPC)。研究了载体种类、Ti O2负载量、反应温度、反应时间、原料配比和催化剂用量等因素对逆歧化反应的影响,并对催化剂进行了XRD,BET,NH3-TPD等技术的表征。实验结果表明,Ti O2在载体Si O2表面分散较好,催化剂具有较大的比表面积和孔体积,利于反应物和产物的扩散,催化性能较好。当Ti O2负载量为15%(w)时,催化剂表面的弱酸量最多,催化活性最高。在DPC用量0.35 mol、n(DMC)∶n(DPC)=3、15%Ti O2/Si O2催化剂用量5%(相对于DPC质量)、反应温度160℃、反应时间2 h、搅拌转速500 r/min的最佳工艺条件下,DPC转化率和MPC收率分别为81.5%和78.6%。TiO2/SiO2 catalysts were prepared through precipitation-impregnation and used to catalyze the reverse disproportionation reaction of dimethyl carbonate (DMC) with diphenyl carbonate (DPC) to methyl phenyl carbonate (MPC). The catalysts were characterized by means of XRD, BET and NH3-TPD. The effects of supports, TiO2 loading, reaction temperature, reaction time, n(DMC) : n (DPC) and catalyst dosage on the reverse disproportionation reaction were studied. The results indicated that the catalysts with good dispersivity of TiO2 on the SiO2 support, large specific surface area and large pore volume were obtained, which were beneficial to the diffusion of the reactants and product. When the TiO2 loading was 15% (w), the best catalyst performance was achieved due to the highest weak acid amount on the catalyst surface. Under the optimal conditions of DPC dosage 0.35 mol, n(DMC) : n(DPC) 3, w(15%YiO2/SiO2) 5% (based on the mass ofDPC) , reaction temperature 160 ℃, reaction time 2 h and stirring speed 500 r/min, the conversion of DPC and the yield of MPC reached 81.5% and 78.6%, respectively.
关 键 词:二氧化钛/二氧化硅催化剂 碳酸二甲酯 碳酸二苯酯 甲基苯基碳酸酯 逆歧化反应
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