在Ce_(0.8)Cu_(0.2)O_(2)氧载体中添加不同质量S-1分子筛,并利用XRD、BET、XPS、SEM、TEM和CH4-TPR&CO_(2)-TPO等表征对氧载体的物化特性和反应性能进行了研究。考察了S-1分子筛添加量对Ce_(0.8)Cu_(0.2)O_(2)氧载体在化学链甲烷重...在Ce_(0.8)Cu_(0.2)O_(2)氧载体中添加不同质量S-1分子筛,并利用XRD、BET、XPS、SEM、TEM和CH4-TPR&CO_(2)-TPO等表征对氧载体的物化特性和反应性能进行了研究。考察了S-1分子筛添加量对Ce_(0.8)Cu_(0.2)O_(2)氧载体在化学链甲烷重整耦合CO_(2)还原反应中的性能的影响。与单纯的Ce_(0.8)Cu_(0.2)O_(2)氧载体相比,添加了0.3 g S-1分子筛后复合氧载体的比表面积明显增大,从15.44 m^(2)/g提高至73.27 m^(2)/g。同时热稳定性和结构稳定性也得到了很大的改善。添加了0.3 g S-1分子筛的复合氧载体CH4转化率由38.93%提升至56.03%,CO_(2)还原过程中CO产率由1.18 mmol/g增加至2.16 mmol/g。展开更多
1-Butylene epoxidation was catalyzed by microporous titanosilicate molecular sieves TS-1 synthesized by different methods and mesoporous titanosilicate molecular sieves Ti-HMS, using dilute hydrogen peroxide solution ...1-Butylene epoxidation was catalyzed by microporous titanosilicate molecular sieves TS-1 synthesized by different methods and mesoporous titanosilicate molecular sieves Ti-HMS, using dilute hydrogen peroxide solution as oxidant. The effect of the Si/Ti molar ratio of the catalyst TS-1 and Ti-HMS on their performance was investigated. Conventional TS-1 has smaller crystal size and higher activity than that of TS-1 synthesized by using TPABr as template or the method of gas-solid phase. The TS-1 synthesized by using TPABr as template exhibits the highest selectivity to 1, 2-epoxybutane (BO). With the increase of Ti content in molecular sieves, the conversion of H2O2 increases. The catalytic activity of mesoporous Ti-HMS is lower than that of TS-1, and large amount of H2O2 is decomposed in 1-butylene epoxidation. The primary reason for low activity of Ti-HMS in 1-butylene epoxidation is that Ti-HMS has poorer hydrophobicity property than TS-1.展开更多
文摘在Ce_(0.8)Cu_(0.2)O_(2)氧载体中添加不同质量S-1分子筛,并利用XRD、BET、XPS、SEM、TEM和CH4-TPR&CO_(2)-TPO等表征对氧载体的物化特性和反应性能进行了研究。考察了S-1分子筛添加量对Ce_(0.8)Cu_(0.2)O_(2)氧载体在化学链甲烷重整耦合CO_(2)还原反应中的性能的影响。与单纯的Ce_(0.8)Cu_(0.2)O_(2)氧载体相比,添加了0.3 g S-1分子筛后复合氧载体的比表面积明显增大,从15.44 m^(2)/g提高至73.27 m^(2)/g。同时热稳定性和结构稳定性也得到了很大的改善。添加了0.3 g S-1分子筛的复合氧载体CH4转化率由38.93%提升至56.03%,CO_(2)还原过程中CO产率由1.18 mmol/g增加至2.16 mmol/g。
文摘1-Butylene epoxidation was catalyzed by microporous titanosilicate molecular sieves TS-1 synthesized by different methods and mesoporous titanosilicate molecular sieves Ti-HMS, using dilute hydrogen peroxide solution as oxidant. The effect of the Si/Ti molar ratio of the catalyst TS-1 and Ti-HMS on their performance was investigated. Conventional TS-1 has smaller crystal size and higher activity than that of TS-1 synthesized by using TPABr as template or the method of gas-solid phase. The TS-1 synthesized by using TPABr as template exhibits the highest selectivity to 1, 2-epoxybutane (BO). With the increase of Ti content in molecular sieves, the conversion of H2O2 increases. The catalytic activity of mesoporous Ti-HMS is lower than that of TS-1, and large amount of H2O2 is decomposed in 1-butylene epoxidation. The primary reason for low activity of Ti-HMS in 1-butylene epoxidation is that Ti-HMS has poorer hydrophobicity property than TS-1.
基金supported by the National Natural Science Foundation of China(21403070 and 21373088)Innovation Program of Shanghai Municipal Education Commission(13zz038)+2 种基金Key Project of the Shanghai Committee of Science and Technology(12JC1403600)National Key Technology R&D Program(2012BAE05B02)Shanghai Leading Academic Discipline Project(B409)~~