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Fabrication of propylsulfonic acid functionalized SiO2 core/PMO shell structured PrSO3H-SiO2@Si(R)Si nanospheres for the effective conversion of d-fructose into ethyl levulinate
Applied Catalysis A: General ( IF 5.5 ) Pub Date : 2017-08-04 , DOI: 10.1016/j.apcata.2017.08.004
Daiyu Song , Yingnan Sun , Qingqing Zhang , Panpan Zhang , Yihang Guo , Jiyan Leng

Propylsulfonic acid functionalized SiO2 core/alkyl- or phenyl-bridged organosilica shell structured PrSO3H-SiO2@Si(R)Si (R = C2H4, C6H4 or C6H4C6H4) nanospheres are facilely prepared by a CTAB-directed one-pot two-step condensation strategy. The morphological characteristics, textural properties, Brønsted acid nature and structure of the PrSO3H-SiO2@Si(R)Si nanospheres are well characterized. The materials are successfully applied in the catalytic transformation of D-fructose into the important organic chemical, ethyl levulinate, in the presence of ethanol as both reactant and solvent. The catalytic activity of the PrSO3H-SiO2@Si(R)Si nanospheres outperform commercially available Amberlyst-15, HY zeolite and HCl, mainly attributing to their strong Brønsted acid nature; additionally, unique core-shell structure with excellent porosity properties and well-adjusted hydrophilicity/hydrophobicity also give the positive influence on the ethanolysis activity, which can improve the accessibility of the reactants to the PrSO3H sites and facilitate the multi-step ethanolysis reaction proceeding to the formation of the final product. The PrSO3H-SiO2@Si(R)Si nanospheres can be reused three times without obvious activity loss, contributed from covalent bonding of the PrSO3H groups with the silica and organosilica framework as well as hydrophobic PrSO3H-functionalized organosilica shell.



中文翻译:

丙磺酸官能化的SiO 2核/ PMO壳结构的PrSO 3 H-SiO 2 @Si(R)Si纳米球的制备,用于将D-果糖有效转化为乙酰丙酸乙酯

丙磺酸官能化的SiO 2核/烷基或苯基桥连的有机硅壳结构的PrSO 3 H-SiO 2 @Si(R)Si(R =  C 2 H 4C 6 H 4C 6 H 4 C 6 H 4)通过CTAB定向的一锅两步缩合策略可轻松制备纳米球。PrSO 3 H-SiO 2的形貌特征,织构特性,布朗斯台德酸性质和结构Si(R)Si纳米球具有良好的特性。该材料在乙醇作为反应物和溶剂的情况下,成功地用于将D-果糖催化转化为重要的有机化学物质乙酰丙酸乙酯。PrSO 3 H-SiO 2 @Si(R)Si纳米球的催化活性优于市售的Amberlyst-15,HY沸石和HCl,主要归因于其强的布朗斯台德酸性质。此外,独特的核-壳结构具有优异的孔隙率特性和良好的亲水性/疏水性,也对乙醇分解活性产生了积极影响,可以改善反应物对PrSO 3的可及性。H位点并促进多步乙醇解反应进行到最终产物的形成。PrSO 3 H-SiO 2 @Si(R)Si纳米球可重复使用3次而不会造成明显的活性损失,这归因于PrSO 3 H基团与二氧化硅和有机硅骨架以及疏水的PrSO 3 H-官能化有机硅的共价键合壳。

更新日期:2017-08-04
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