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Support effects in the selective gas phase hydrogenation ofp-chloronitrobenzene over gold
Gold Bulletin ( IF 2.1 ) Pub Date : 2009-06-01 , DOI: 10.1007/bf03214922
Fernando Cárdenas-Lizana , Santiago Gómez-Quero , Noémie Perret , Mark A. Keane

The catalytic continuous gas phase hydrogenation of p-chloronitrobenzene (P=1 atm;T=423 K) has been investigated over a series of oxide (Al2O3, TiO2, Fe2O3 and CeO2) supported Au (1 mol %) catalysts. The application of two catalyst synthesis routes,i.e. impregnation (IMP) and deposition-precipitation (DP), has been considered where the DP route generated smaller mean Au particle sizes (1.5-2.8 nm) compared with the IMP preparation (3.5-9.0 nm). The catalysts have been characterised in terms H2 chemisorption and BET area measurements where the formation of metallic Au post-activation has been verified by diffuse reflectance UV-Vis, XRD and HRTEM analyses.p-Chloroaniline was generated as the sole reaction product over all the Au catalysts with no evidence of C-Cl and/or C-NO2 bond scission and/or aromatic ring reduction. The specific hydrogenation rate increased with decreasing Au particle size (from 9 to 3 nm), regardless of the nature of the support. This response extends to a reference Au/TiO2 catalyst provided by the World Gold Council. A decrease in specific rate is in evidence for smaller particles (< 2 nm) and can be attributed to a quantum size effect. The results presented establish the basis for the design and development of a versatile catalytic system for the clean continuous production of high value amino compounds under mild reaction conditions.

中文翻译:

对氯硝基苯在金上选择性气相加氢的支持作用

已经在一系列氧化物(Al2O3、TiO2、Fe2O3 和 CeO2)负载的 Au(1 mol%)催化剂上研究了对氯硝基苯(P=1 atm;T=423 K)的催化连续气相氢化。已经考虑了两种催化剂合成路线的应用,即浸渍 (IMP) 和沉积-沉淀 (DP),其中 DP 路线产生的平均金粒径 (1.5-2.8 nm) 与 IMP 制备 (3.5-9.0 nm) 相比)。催化剂已在 H2 化学吸附和 BET 面积测量方面进行了表征,其中金属 Au 后活化的形成已通过漫反射 UV-Vis、XRD 和 HRTEM 分析进行验证。 p-氯苯胺作为唯一的反应产物产生。没有证据表明 C-Cl 和/或 C-NO2 键断裂和/或芳环还原的 Au 催化剂。无论载体的性质如何,比氢化率随着 Au 粒径的减小(从 9 到 3 nm)而增加。此响应扩展到世界黄金协会提供的参考 Au/TiO2 催化剂。对于较小的粒子 (< 2 nm),比速率的降低是显而易见的,这可归因于量子尺寸效应。所呈现的结果为设计和开发用于在温和反应条件下清洁连续生产高价值氨基化合物的多功能催化系统奠定了基础。2 nm) 并且可以归因于量子尺寸效应。所呈现的结果为设计和开发用于在温和反应条件下清洁连续生产高价值氨基化合物的多功能催化系统奠定了基础。2 nm) 并且可以归因于量子尺寸效应。所呈现的结果为设计和开发用于在温和反应条件下清洁连续生产高价值氨基化合物的多功能催化系统奠定了基础。
更新日期:2009-06-01
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