钼-钛复合氧化物催化碳酸二甲酯和乙酸苯酯合成碳酸二苯酯 |
Mo-Ti Composite Oxide Catalyst for Transesterification of Dimethyl Carbonate and Phenyl Acetate to Diphenyl Carbonate |
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摘要: 采用溶胶-凝胶法制备了用于碳酸二甲酯(DMC)与乙酸苯酯(PA)酯交换合成碳酸二苯酯(DPC)的钼-钛复合氧化物催化剂, 考察了Mo/Ti物质的量的配比、反应条件等因素对催化剂性能的影响。结合比表面积(BET法)、X-射线衍射等测试技术对催化剂进行了表征。结果发现, 在焙烧温度为500℃, nMo:nTi=5:2条件下制得的催化剂活性最高, 在优化的反应工艺条件(t=4 h, θ=180℃, wcat/wPA=0.08, nPA/nDMC=2)下, DMC的转化率为74.0%, 甲基苯基碳酸酯(MPC)及DPC的选择性分别为51.0%, 45.5%。比表面积测试结果表明, TiO2的添加, 增大了催化剂的比表面积, 有利于催化反应的进行。X-射线衍射测试结果表明, 钼-钛复合氧化物中, MoO3具有良好的结晶形态, 为α-MoO3, 没有发现TiO2、Mo-Ti复合氧化物新物种的结晶相, 说明TiO2、Mo-Ti复合氧化物新物相为无定型化合物, 并高度分散在整个复合氧化物体系中。 |
关键词: 钼-钛复合氧化物 碳酸二甲酯 乙酸苯酯 碳酸二苯酯 |
基金项目: 国家“十一五”科技支撑计划(2006BAE02B03);江苏省常州市工业科技攻关计划(CE2008091);重庆市教育委员会科学技术研究项目 (KJ110815);重庆理工大学科研启动基金(2010ZD29)资助项目。 |
Abstract: The Mo-Ti composite oxide catalyst was prepared by sol-gel method and used for the transesterification of dimethyl carbonate (DMC) and phenyl acetate (PA) to diphenyl carbonate (DPC). The effect of the molar ratio of Mo/Ti and reaction conditions on the catalytic performance was investigated. The catalyst with a Mo/Ti molar ratio of 2.5 shows the highest activity. When the reaction is carried out at 180℃, with a molar ratio of PA to DMC of 2:1, the reaction time of 4 h, a catalyst amount of 0.08 (weight ratio to PA), the conversion of DMC is 74.0%, and the selectivity of DPC and MPC is 45.5% and 51.0%, respectively. According to the surface and X-ray diffraction results, lager specific areas result in improved catalytic performance by the addition of TiO2. The Mo-Ti composite oxide is composed of α-MoO3 and highly dispersed amorphous titania and/or new crystal phase of Mo-Ti composite oxide. |
Keywords: molybdenum titanium composite oxide dimethyl carbonate phenyl acetate diphenyl carbonate |
投稿时间:2012-06-28 修订日期:2012-08-13 |
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曹平,杨先贵,辛阳,王公应.钼-钛复合氧化物催化碳酸二甲酯和乙酸苯酯合成碳酸二苯酯[J].无机化学学报,2013,29(4):747-752. |
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