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Effect of the type of siliceous template and carbon precursor on physicochemical and catalytic properties of mesoporous nanostructured carbon-palladium systems
Journal of Porous Materials ( IF 2.5 ) Pub Date : 2020-05-24 , DOI: 10.1007/s10934-020-00896-y
Ireneusz Szewczyk , Robert Kosydar , Piotr Natkański , Dorota Duraczyńska , Jacek Gurgul , Piotr Kuśtrowski , Alicja Drelinkiewicz

Two series of nanostructured carbon replicas were synthesized through a hard-templating method using ordered SBA-15 or disordered mesoporous spherical silica gel as the templates and furfuryl alcohol or sucrose as the carbon source. They were explored to synthesize the Pd catalysts (ca. 1.5 wt% Pd loading) by the colloid-based microemulsion procedure which allowed preparing the catalysts of monodispersed Pd particles of similar size (4–5 nm). The palladium phase in the catalysts (e.g. the Pd particles distribution and extent of agglomeration) varied depending on the textural and surface characteristics of the carbon replicas. In the furfural hydrogenation studied as a probe reaction (2-propanol, 35 °C, 6 bar H2), furfuryl alcohol and tetrahydrofurfuryl alcohol were the major products formed. The catalytic reactivity has been related to the properties of the Pd phase including the surface Pd concentration and the extent of the Pd particles aggregation accompanied by the nearest palladium environment expressed by the surface O/Pd atomic ratio. At high O/Pd ratio the reaction slowed down because of a facilitated furfuryl alcohol adsorption resulting most probably in a blockage of the active sites. The SiOsucrose system provided the catalyst which was characterized by relatively low O/Pd ratio with well-dispersed Pd particles and the highest and stable activity for the furfural hydrogenation. The SBA-series catalysts, with lower O/Pd and more aggregated Pd particles, exhibited lower activity but somewhat higher tendency to the tetrahydrofurfuryl alcohol formation.



中文翻译:

硅质模板和碳前驱体类型对介孔纳米结构碳钯体系理化和催化性能的影响

通过有序SBA-15或无序介孔球形硅胶为模板,糠醇或蔗糖为碳源,通过硬模板法合成了两个系列的纳米结构碳复制体。他们探索了通过基于胶体的微乳液程序来合成Pd催化剂(约1.5 wt%Pd负载),该程序允许制备尺寸相似(4-5 nm)的单分散Pd颗粒的催化剂。催化剂中的钯相(例如,Pd颗粒分布和团聚程度)根据碳复制品的质地和表面特性而变化。在糠醛氢化中作为探针反应进行研究(2-丙醇,35°C,6 bar H 2),糠醇和四氢糠醇是形成的主要产物。催化反应性与Pd相的性质有关,包括表面Pd浓度和Pd颗粒聚集的程度,伴随着以表面O / Pd原子比表示的最近的钯环境。在高O / Pd比下,反应加快,这是因为糠醇易于吸附,最有可能导致活性位点的阻塞。SiO 蔗糖体系提供的催化剂具有较低的O / Pd比,良好分散的Pd颗粒和最高且稳定的糠醛加氢活性。具有较低O / Pd和更多聚集Pd颗粒的SBA系列催化剂显示出较低的活性,但四氢糠醇形成的趋势较高。

更新日期:2020-05-24
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