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作 者:林玲[1] 王惠璇[1] 刘承[1] 黄加乐[1] 李清彪[1]
机构地区:[1]厦门大学化学化工学院化学工程与生物工程系醇醚酯化工清洁生产国家工程实验室化学生物学福建省重点实验室,福建厦门361005
出 处:《化学反应工程与工艺》2011年第2期144-150,共7页Chemical Reaction Engineering and Technology
基 金:国家自然科学基金重点项目(21036004):国家自然科学基金面上项目(20976146);福建省科技计划重点项目(2009H0041);教育部博土点基金项目(20100121110032)
摘 要:采用芳樟叶浸出液,通过原位还原和等体积浸渍的方法制备负载型纳米银催化剂,并以对硝基苯酚(4-NP)加氢反应为模型反应,考察催化剂载体,焙烧条件等对负载型纳米银催化剂性能的影响,并采用扫描电镜(SEM),热重分析(TG)和红外光谱(FT-IR)等表征手段对催化剂进行表征。结果表明,以TiO_2为载体制备的纳米银催化剂具有较好的催化活性;植物还原法制备的催化剂表面纳米银颗粒较小((7.3±2.4)nm),催化效果较好。当体系中Ag与4-NP的物质的量之比为1:230时,完全反应时间小于或等于10 min。对催化剂进行一定条件的焙烧处理,能在一定程度上提高催化剂的活性和重复使用性,将催化剂于400℃下焙烧1h,催化活性最佳:将催化剂于400℃下焙烧2h,催化剂重复使用性最好。对芳樟叶浸出液与银的作用机理进行初步研究,表明劳樟叶浸出液中的杂环化合物能通过羰基与银络合,从而起到防止催化剂表面纳米银颗粒团聚的作用。The supported nano-silver catalyst(Ag/TiO2) was prepared by in situ reduction and incipient wetness impregnation method using the aqueous extract of cinnamomum camphora leaf, and the effects of carriers and calcination conditions on performance of the catalyst were investigated by 4-nitrophenol(4-NP) hydrogenation. The catalyst was characterized by means of scanning electron microscope(SEM), thermogravimetric analysis(TG) and Fourier transform infrared spectrophotometer(FT-lR). The results showed that the biosynthesized Ag/TiOz catalyst, with Ag nanoparticle size (7.3±2.4) nm, demonstrated excellent performance in catalyzing hydrogenation of 4-NP, and when the molar ratio of Ag to 4-NP was 1:230, the time for complete conversion of 4-NP to Aminophenol (4-AP) was less than or equal to 10 min. The catalytic activity and reusability of the catalyst could be improved through calcination. The catalyst calcined at 400 ℃ for I h in air exhibited better catalytic activity and calcined at 400℃ for 2 h exhibited better reusability. The action mechanism of Ag and cinnamomum camphora leaf extract was studied and the results showed that the heterocyclic compounds in the extract could complex with Ag through carbonyl groups, which prevented the Ag nanoparticles on the surface of catalyst gathering.
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