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Facile Synthesis of Spatially‐Functionalized Core‐Shell Nanocatalysts with 3‐D Mesopore Structure
ChemCatChem ( IF 3.8 ) Pub Date : 2020-11-23 , DOI: 10.1002/cctc.202001737 Cornelia Baeckmann 1 , Constantin Eisen 1 , Hanspeter Kählig 2 , Patrick Guggenberger 1 , Freddy Kleitz 1
ChemCatChem ( IF 3.8 ) Pub Date : 2020-11-23 , DOI: 10.1002/cctc.202001737 Cornelia Baeckmann 1 , Constantin Eisen 1 , Hanspeter Kählig 2 , Patrick Guggenberger 1 , Freddy Kleitz 1
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Hollow mesoporous silica particles (HMSPs) have recently drawn much attention as nanocatalysts, owing to their benefits and potential for greener chemical processes. Here, improved synthesis of HMSPs exhibiting a shell with a 3‐D pore structure is proposed to overcome previous synthetic issues, such as reproducibility, particle size distribution, precise tailoring of size/shell thickness, low yield, etc. Additionally, precisely controlled and selective functionalization with amine groups is achieved owing to careful protection and sequential extraction protocols. To overcome time‐consuming and complex multistep extraction procedures, different methods were optimized towards the most efficient protocol. The obtained materials are characterized in terms of structure, porosity and functions, and the confined catalytic activity was tested in a Knoevenagel reaction. The nanocatalysts were compared before and after the core template was removed to confirm that the only catalytic species are free amines located on the inner external surface of the shell (i. e., the surface exposed towards the hollow core).
中文翻译：
具有3-D中孔结构的空间功能化核壳纳米催化剂的简便合成
空心中孔二氧化硅颗粒（HMSPs）作为纳米催化剂最近受到了广泛的关注，这是因为它们的好处以及在绿色化学过程中的潜力。在此，提出了一种改进的具有3D孔结构壳的HMSP合成方法，以克服以前的合成问题，例如重现性，粒度分布，尺寸/壳厚度的精确调整，产率低等。此外，精确控制和由于精心的保护和顺序提取方案，实现了具有胺基团的选择性官能化。为了克服耗时且复杂的多步骤提取程序，针对最有效的协议对不同的方法进行了优化。获得的材料根据结构，孔隙率和功能进行表征，并在Knoevenagel反应中测试了受限的催化活性。在去除核心模板之前和之后比较了纳米催化剂，以确认唯一的催化物种是位于内部的游离胺。壳体的外表面（即，暴露于空心的表面）。
更新日期：2020-11-23
中文翻译：
具有3-D中孔结构的空间功能化核壳纳米催化剂的简便合成
空心中孔二氧化硅颗粒（HMSPs）作为纳米催化剂最近受到了广泛的关注，这是因为它们的好处以及在绿色化学过程中的潜力。在此，提出了一种改进的具有3D孔结构壳的HMSP合成方法，以克服以前的合成问题，例如重现性，粒度分布，尺寸/壳厚度的精确调整，产率低等。此外，精确控制和由于精心的保护和顺序提取方案，实现了具有胺基团的选择性官能化。为了克服耗时且复杂的多步骤提取程序，针对最有效的协议对不同的方法进行了优化。获得的材料根据结构，孔隙率和功能进行表征，并在Knoevenagel反应中测试了受限的催化活性。在去除核心模板之前和之后比较了纳米催化剂，以确认唯一的催化物种是位于内部的游离胺。壳体的外表面（即，暴露于空心的表面）。
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