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以高度分散的过渡金属为介质的模板衍生介孔碳用于二苯并噻吩的反应吸附

Template-derived mesoporous carbons with highly dispersed transition metals as media for the reactive adsorption of dibenzothiophene.

作者信息

Seredych Mykola, Bandosz Teresa J

机构信息

Department of Chemistry, The City College of New York, New York, New York 10031, USA.

出版信息

Langmuir. 2007 May 22;23(11):6033-41. doi: 10.1021/la063291j. Epub 2007 Apr 18.

Abstract

Mesoporous carbons with highly dispersed copper, cobalt, and iron were obtained from an organic polymer within amorphous silica powder, alumina, and zeolite 13X. The materials were characterized using the adsorption of nitrogen, potentiometric titration, and elemental analysis. The small metal content (less than 1%) and its chelation in the precursor polymers ensure a high dispersion of metallic centers. The materials obtained are mainly mesoporous but differ significantly in their porosity and surface chemistry, which is linked to the effect of template constraints and chemistry and the kind of metal and is related to the differences in the carbonization mechanism. On the carbon obtained, the adsorption of dibenzothiophene (DBT) from hexane was carried out. The high capacities (up to 130 mg S/g) obtained were linked to the high volume of mesopores and specific interactions of DBT with surface acidic groups and strong interactions of metals with dibenzothiophene via S-M sigma bonds or, in the case of copper, via interaction of metals with disturbed pi electrons of aromatic rings of DBT.

摘要

通过在无定形二氧化硅粉末、氧化铝和13X沸石中的有机聚合物制备出了具有高度分散的铜、钴和铁的介孔碳。使用氮气吸附、电位滴定和元素分析对这些材料进行了表征。前驱体聚合物中低含量的金属(小于1%)及其螯合作用确保了金属中心的高度分散。所获得的材料主要为介孔材料,但它们的孔隙率和表面化学性质存在显著差异,这与模板限制和化学作用的影响、金属种类有关,并且与碳化机理的差异有关。在所得的碳材料上,进行了从己烷中吸附二苯并噻吩(DBT)的实验。所获得的高吸附容量(高达130 mg S/g)与大量的介孔以及DBT与表面酸性基团的特定相互作用和金属与二苯并噻吩通过S-M σ键的强相互作用有关,或者对于铜而言,与金属与DBT芳香环中受干扰的π电子的相互作用有关。

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