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作 者:宋爽爽 蒋丽红[1] 王亚明[1] 郑燕娥 包宇辉 申晨 SONG Shuang-shuang;JIANG Li-hong;WANG Ya-ming;ZHENG Yan-e;BAO Yu-hui;SHEN Chen(Faculty Chemical Engineering,Kunming University of Science and Technology,Kunming 650500,Yunnan,China)
机构地区:[1]昆明理工大学化学工程学院
出 处:《精细化工》2019年第11期2234-2242,共9页Fine Chemicals
基 金:国家自然科学基金项目(21266012);国家自然科学基金联合重点支持项目(U1202265)
摘 要:采用溶胶-凝胶法制备复合载体TiO2-ZrO2,并通过金属诱导化学镀法制备负载型催化剂Ni-B/TiO2-ZrO2,以松香加氢为探针反应,通过单因素实验对载体制备过程、催化剂制备过程进行了优化,得到适宜的载体制备条件为:Zr/Ti物质的量比为0.6、焙烧温度为550℃、焙烧时间4 h;催化剂制备条件:制备温度为50℃、微波升温时间为3 min、n(Ni)∶n(B)=1∶2。结果表明:该条件下制备的催化剂用于松香加氢反应,枞酸型树脂酸转化率达99%以上,且可重复使用7次。以XRD、XPS、TEM、BET为表征手段,对催化剂失活前后的结构与性能进行了分析,结果表明:Ni-B以非晶态的形式负载在TiO2-ZrO2载体上,分散性较好,平均粒径约为25 nm。而失活催化剂上Ni^0、B^0含量均下降,出现活性组分流失、氧化等现象,这可能是导致催化剂失活的主要原因。A Ti O2-ZrO2 composite carrier was prepared by sol-gel method. Subsequently, a supported Ni-B/Ti O2-ZrO2 catalyst was prepared by metal induced electroless plating. The preparation processes of carrier and catalyst were optimized by single factor experiment. The suitable carrier preparation conditions were as follows: molar ratio of Zr/Ti 0.6, calcination temperature 550 ℃, and calcination time 4 h. The catalyst preparation conditions were as follows: microwave intervention temperature 50 ℃, microwave heating time 3 min, n(Ni)∶n(B)=1∶2. The catalyst prepared under these conditions was used for the hydrogenation of rosin, and the conversion rate of abietic resin acids was over 99%. In addition, the catalyst could be reused for 7 times. XRD, XPS, TEM and BET were employed to characterize the structure and properties of the catalyst before and after deactivation. The results showed that Ni-B was supported on the Ti O2-ZrO2 carrier in an amorphous state with good dispersion and average particle size of about 25 nm. However, the content of Ni^0 and B^0 on the deactivated catalyst decreased, and the active components were lost and oxidized, which might be the main cause of catalyst deactivation.
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