Department of Chemistry, University of California Riverside, 900 University Ave., Riverside, CA, 92521 (USA).
ChemSusChem. 2013 Oct;6(10):2001-8. doi: 10.1002/cssc.201300416. Epub 2013 Sep 10.
Mesoporous hollow colloidal particles with well-defined characteristics have potential use in many applications. In liquid-phase catalysis, in particular, they can provide a large active surface area, reduced diffusion resistance, improved accessibility to reactants, and excellent dispersity in reaction media. Herein, we report the tailored synthesis of sulfated ZrO2 hollow nanostructures and their catalytic applications in the dehydration of fructose. ZrO2 hollow nanoshells with controllable thickness were first synthesized through a robust sol-gel process. Acidic functional groups were further introduced to the surface of hollow ZrO2 shells by sulfuric acid treatment followed by calcination. The resulting sulfated ZrO2 hollow particles showed advantageous properties for liquid-phase catalysis, such as well-maintained structural integrity, good dispersity, favorable mesoporosity, and a strongly acidic surface. By controlling the synthesis and calcination conditions and optimizing the properties of sulfated ZrO2 hollow shells, we have been able to design superacid catalysts with superior performance in the dehydration of fructose to 5-hydroxymethyfurfural than the solid sulfated ZrO2 nanocatalyst.
具有明确定义特征的介孔中空胶体颗粒在许多应用中具有潜在用途。特别是在液相催化中，它们可以提供大的活性表面积、降低扩散阻力、改善反应物的可及性以及在反应介质中的优异分散性。在此，我们报告了定制合成硫酸化氧化锆中空纳米结构及其在果糖脱水反应中的催化应用。通过稳健的溶胶-凝胶工艺首先合成了具有可控厚度的氧化锆中空纳米壳。通过硫酸处理和随后的煅烧，进一步在中空氧化锆壳的表面引入酸性官能团。所得的硫酸化氧化锆中空颗粒在液相催化中表现出有利的性质，例如保持结构完整性、良好的分散性、有利的中孔性和强酸性表面。通过控制合成和煅烧条件以及优化硫酸化氧化锆中空壳的性能，我们已经能够设计出在果糖脱水为 5-羟甲基糠醛方面具有优异性能的超酸催化剂，优于固体硫酸化氧化锆纳米催化剂。
