Ru-Rh/AC催化对苯二酚选择性加氢制备1,4-环己二醇
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摘要
采用浸渍法制备了负载在活性炭(AC)上的Ru-Rh/AC双金属催化剂,通过ICP-AES,TEM,XRD方法对Ru-Rh/AC催化剂进行了表征;将Ru-Rh/AC催化剂用于对苯二酚选择性加氢制备1,4-环己二醇的反应,系统考察了溶剂、反应温度、反应压力和催化剂用量对该反应的影响。表征结果显示,活性组分在AC载体表面形成了高分散的粒径为2～5 nm的合金颗粒。实验结果表明,优化的反应条件为:以异丙醇为溶剂、催化剂中Ru-Rh金属与对苯二酚摩尔比为0.005、反应温度80℃、反应压力1.0 MPa。在此条件下反应1 h,对苯二酚转化率为100%,目的产物1,4-环己二醇的选择性为95.5%。Ru-Rh/AC双金属催化剂具有较好的稳定性。
Ruthenium-rhodium/active carbon(Ru-Rh/AC) catalyst was prepared by an impregnation method,characterized by means of ICP-AES,TEM and XRD,and used in the liquid phase selective hydrogenation of hydroquinone to 1,4-cyclohexanediol.The results showed that 2-5 nm Ru-Rh nanoparticles were dispersed well on the surface of the active carbon.The effects of solvents,catalyst dosage,reaction temperature and pressure on the activity and selectivity of the Ru-Rh/AC catalyst were investigated.Under the optimized reaction conditions:isopropanol as the solvent,n(RuRh)∶n(hydroquinone) 0.005,80 ℃,1.0 MPa and 1 h,the selectivity to 1,4-cycloheanediol and the conversion of hydroquinone researched 95.5% and 100%,respectively.The Ru-Rh/AC catalyst has good stability.
Ruthenium-rhodium/active carbon(Ru-Rh/AC) catalyst was prepared by an impregnation method,characterized by means of ICP-AES,TEM and XRD,and used in the liquid phase selective hydrogenation of hydroquinone to 1,4-cyclohexanediol.The results showed that 2-5 nm Ru-Rh nanoparticles were dispersed well on the surface of the active carbon.The effects of solvents,catalyst dosage,reaction temperature and pressure on the activity and selectivity of the Ru-Rh/AC catalyst were investigated.Under the optimized reaction conditions:isopropanol as the solvent,n(RuRh)∶n(hydroquinone) 0.005,80 ℃,1.0 MPa and 1 h,the selectivity to 1,4-cycloheanediol and the conversion of hydroquinone researched 95.5% and 100%,respectively.The Ru-Rh/AC catalyst has good stability.
引文
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[4]医药和液晶材料单体——1,4-环己二醇[J].试剂与精细化学品,2006(2):13.
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[8]闫世润,乔明华,范康年.非晶态合金催化剂的研究进展[J].石油化工,2007,36(3):213-220.
[9]Wu Mingli,Chen Donghwang,Huang Tingchia.Synthesis ofAu/Pd Bimetallic Nanoparticles in Reverse Micelles[J].Lang-muir,2001,17(13):3877-3883.
[10]Yamashita H,Yoshikawa M,Funabiki T,et al.Catalysis byAmorphous Metal Alloys[J].J Chem Soc,Faraday Trans,1986,82(6):1771-1780.
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[12]Greeley J,Mavrikakis M.Near-Surface Alloys for HydrogenFuel Cell Applications[J].Catal Today,2006,111(1):52-58.
[13]中国有色金属工业总公司昆明贵金属研究所.粗铑及含铑量高的合金废料的溶解与提纯:中国,1031567[P].1989-03-08.
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[15]Smith H A,Stump B L.A Study of the Catalytic Hydrogena-tion of Hydroxybenzenes over Platinum and Rhodium Catalysts[J].J Am Chem Soc,1961,83(12):2739-2743.
[16]Bovkun T T,Sasson Y,Blum J.Conversion of Chlorophe-nols into Cyclohexane by a Recyclable Pd-Rh Catalyst[J].JMol Catal A:Chem,2005,242(1):68-73.