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作 者:王英斌 王康军 刘蝈蝈[1,2] 宋雨莹 秦王昕 张亚芳 WANG Yingbin;WANG Kangjun;LIU Guoguo;SONG Yuying;QIN Wangxin;ZHANG Yafang(School of Chemical Engineering,Shenyang University of Chemical Technology,Shenyang 110142,China;Key Laboratory on Resources Chemicals and Materials of Ministry of Education,Shenyang University of Chemical Technology,Shenyang 110142,China)
机构地区:[1]沈阳化工大学化学工程学院,辽宁沈阳110142 [2]沈阳化工大学资源化工与材料教育部重点实验室,辽宁沈阳110142
出 处:《沈阳化工大学学报》2023年第3期208-217,共10页Journal of Shenyang University of Chemical Technology
基 金:辽宁省兴辽英才青年拔尖项目(XLYC1907029);辽宁省教育厅项目(LJKZ0439,LJKQ2021068);沈阳化工大学“优青”托举计划项目(2019YQ001);辽宁省科技厅创新能力提升联合基金项目(2021-NLTS-12-01)。
摘 要:分别采用沉积沉淀法、溶胶凝胶法和蒸氨法制备Cu/SiO_(2)催化剂.利用N_(2)吸附-脱附、N_(2)O滴定、XRD、FT-IR、H_(2)-TPR和NH_(3)-TPD对催化剂的物理化学性质进行表征,并考察其己二酸二甲酯加氢合成1,6-己二醇的性能.结果表明:虽然溶胶凝胶法和蒸氨法因层状硅酸铜的存在具有较高的铜分散度和表面酸性等性质,但受制于较小孔径结构,反而是传统的沉积沉淀法制备的Cu/SiO_(2)催化剂因较大的孔径具有更高的反应活性.在反应温度200℃、反应压力5.0 MPa、液时空速0.6 h^(-1)和n(氢)/n(酯)=175的条件下该催化剂可稳定运行50 h,己二酸二甲酯的转化率可达99.8%,1,6-己二醇的选择性可达98.2%.Cu/SiO_(2)catalysts were prepared by deposition precipitation,sol-gel and ammonia evaporation method,respectively.The physicochemical structure properties of the catalyst were characterized by N_(2)adsorption-desorption,N_(2)O titration,XRD,FT-IR,H_(2)-TPR and NH_(3)-TPD,and the performance of hydrogenation of dimethyl adipate(DMA)to 1,6-hexanediol(HDO)was investigated.The results showed that although the sol-gel and ammonia evaporation method had high copper dispersion and surface acidity due to the the presence of copper phyllosilicate structure,they are restricted by the smaller pore structure.Instead,the Cu/SiO_(2)catalyst prepared by the traditional deposition precipitation method had higher reaction activitydue to the larger pore.Under the conditions of reaction temperature 200℃,reaction pressure of 5.0 MPa,liquid hourly space velocity of 0.6 h^(-1)and molar ratio of H_(2)to ester of 175,the reaction could be run stably for 50 h.The conversion rate of dimethyl adipate can reach 99.8%,and the 1,6-hexanediol selectivity can reach 98.2%.
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