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Nanostructured silica-supported gold: Effect of nanoparticle size distribution and electronic state on its catalytic properties in oxidation reactions
Catalysis Today ( IF 5.2 ) Pub Date : 2020-09-02 , DOI: 10.1016/j.cattod.2020.08.028
Y. Kotolevich , O. Martynyuk , J.C. García Ramos , J.E. Cabrera Ortega , R. Vélez , V. Maturano Rojas , A. Aguilar Tapia , S. Martinez-Gonzalez , H.J. Tiznado Vazquez , M. Farías , R. Zanella , A. Pestryakov , N. Bogdanchikova , V. Cortés Corberán

Gold nanocatalysts, active in several oxidation reactions, suffer of insufficient time-on-stream stability. The easiest way to solve this problem is modifying the support, due to metal-support interaction. This study compares modifying effects of MgO and La2O3 on textural, electronic, and catalytic properties of Au nanoparticles (NPs) supported on inert nanostructured SiO2 in CO oxidation and liquid phase 1-octanol oxidation. Modification of the silica support surface with La and Mg increased metal support interaction, leading to gold particles with primary size of 1 nm but with different stability: stable under different pretreatment conditions on Mg-modified samples but highly sensible to the pretreatments on La-modified samples. Both modifiers changed electronic properties of supported gold favoring formation and stabilization of Auδ+ states, which are probable gold active sites in catalytic redox processes. Modification with La and Mg oxides changed catalytic properties in CO oxidation before and after pretreatment in H2 at 300 °C for 1 h. Gold catalysts supported on La- and Mg-modified silica showed similar performance in 1-octanol oxidation with higher conversion than unmodified Au/SiO2. La and Mg showed better promoting effects of catalytic properties in this reaction than redox modifiers (Fe and Ce) supported on small SiO2 particles.



中文翻译:

纳米结构的二氧化硅负载的金:纳米粒度分布和电子态对其在氧化反应中催化性能的影响

在多种氧化反应中具有活性的金纳米催化剂,其运行时间稳定性不足。解决此问题的最简单方法是修改支撑,因为金属与支撑之间会发生相互作用。这项研究比较了MgO和La 2 O 3对惰性纳米结构SiO 2负载的Au纳米颗粒(NPs)的质构,电子和催化性能的改性作用。在CO氧化和液相1-辛醇氧化中 用La和Mg改性二氧化硅载体表面会增加金属载体之间的相互作用,导致金颗粒的主要尺寸为1 nm但具有不同的稳定性:在不同的预处理条件下对Mg改性的样品稳定,但对La改性的预处理高度敏感样品。两种改性剂均改变了负载型金的电子性质,有利于Auδ +态的形成和稳定,这是催化氧化还原过程中可能的金活性位点。La和Mg氧化物的改性改变了H 2中预处理前后的CO氧化催化性能。在300°C下放置1小时。在La和Mg改性的二氧化硅上负载的金催化剂在1-辛醇氧化中表现出相似的性能,其转化率高于未改性的Au / SiO 2。与负载在较小SiO 2颗粒上的氧化还原改性剂(Fe和Ce)相比,La和Mg在该反应中显示出更好的催化性能促进作用。

更新日期:2020-09-02
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