4.6 Article

Morphology Tailoring of Sulfonic Acid Functionalized Organosilica Nanohybrids for the Synthesis of Biomass-Derived Alkyl Levulinates

Journal

CHEMISTRY-A EUROPEAN JOURNAL
Volume 21, Issue 30, Pages 10786-10798

Publisher

WILEY-V C H VERLAG GMBH
DOI: 10.1002/chem.201501219

Keywords

biomass; heterogeneous catalysis; nanostructures; organic-inorganic hybrid composites; silicates

Funding

  1. Natural Science Fund Council of China [21173036, 51278092, 51478095]
  2. New Century Excellent Talents in University of Ministry of Education of China [NCET-13-0723]

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Morphology evolution of sulfonic acid functionalized organosilica nanohybrids (Si(Et)Si-Pr/ArSO3H) with a 1D tubular structure (inner diameter of ca. 5nm), a 2D hexagonal mesostructure (pore diameter of ca. 5nm), and a 3D hollow spherical structure (shell thickness of 2-3nm and inner diameter of ca. 15nm) was successfully realized through P123-templated sol-gel cocondensation strategies and fine-tuning of the acidity followed by aging or a hydrothermal treatment. The Si(Et)Si-Pr/ArSO3H nanohybrids were applied in synthesis of alkyl levulinates from the esterification of levulinic acid and ethanolysis of furfural alcohol. Hollow spherical Si(Et)Si-Pr/ArSO3H and hexagonal mesoporous analogues exhibited the highest and lowest catalytic activity, respectively, among three types of nanohybrids; additionally, the activity was influenced by the SO3H loading. The activity differences are explained in terms of different BrOnsted acid and textural properties, reactant/product diffusion, and mass transfer rate, as well as accessibility of SO3H sites to the reactant molecules. The reusability of the nanohybrids was also evaluated.

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