V_2O_5/TiO_2-ZrO_2催化剂上甲醇选择氧化制甲缩醛  

Selective oxidation of methanol to dimethoxymethane over V_2O_5/TiO_2-ZrO_2 catalyst

作　　者：武建兵[1,2] 王辉[1] 秦张峰[1] 吴志伟[1,2] 黄礼春[1,2] 赵启[1,2] 王建国[1] 

机构地区：[1]中国科学院山西煤炭化学研究所煤转化国家重点实验室,山西太原030001 [2]中国科学院研究生院,北京100049

出　　处：《燃料化学学报》2011年第1期64-68,共5页Journal of Fuel Chemistry and Technology

基　　金：国家自然科学基金(10979068);国家重点基础研究发展规划(973计划;2006CB202504;2010CB234603);中国科学院知识创新方向项目(KJCX2.YW.H16)

摘　　要：采用共沉淀法制备TiO2-ZrO2复合氧化物载体、等体积浸渍法制备V2O5/TiO2-ZrO2催化剂,对催化剂在温和条件下甲醇选择氧化生成甲缩醛（DMM）反应进行研究。结果表明,与单一氧化物载体TiO2或ZrO2负载的钒基催化剂相比,V2O5/TiO2-ZrO2对甲醇选择氧化具有较好的催化性能。XRD、NH3-TPD和H2-TPR表明,ZrO2的加入有利于增加催化剂表面的酸性位,并改善钒物种的氧化还原性,使催化剂具有较好的甲醇选择氧化性能。钒的负载量对催化剂表面钒物种的存在形式和颗粒大小有较大的影响,进而影响催化剂的表面酸性和氧化还原性;V2O5质量分数5%~10%的催化剂甲醇氧化性能最好。The composite TiO2-ZrO2 support was prepared through co-precipitation of Ti（SO4）2 and Zr（SO4）2 solution and V2O5/TiO2-ZrO2 catalysts with different vanadium loadings were obtained by incipient impregnation with ammonium metavanadate solution.The catalytic performance of V2O5/TiO2-ZrO2 in the selective oxidation of methanol to dimethoxymethane（DMM） was investigated under mild reaction conditions.The V2O5/TiO2-ZrO2 catalyst performs better in the selective oxidation of methanol than V2O5 supported on the single oxide TiO2 or ZrO2.XRD,NH3-TPD,and H2-TPR characterization results indicated that the incorporation of highly dispersed ZrO2 in V2O5/TiO2-ZrO2 may enhance the surface acidity and the redox ability of vanadium species,which is favorable for the selective oxidation of methanol.The V2O5 loading influences the dispersion and structure of vanadium species that are related to the catalyst performance;a V2O5 content of 5%~10% is adequate to get V2O5/TiO2-ZrO2 of high performance for the selective oxidation of methanol to DMM.

关 键 词：甲醇 选择氧化 甲缩醛 V2O5 TIO2 ZRO2 

分 类 号：O643.3[理学—物理化学] TQ519[理学—化学]