Paul Neff, Jee-Yee Chen, Ryan Burrows, Nicholas A. Brunelli
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Investigating cooperative interactions for the nitroaldol reaction and condensation: Clarifying the impact of microporosity and pore size on catalytic activity of mesoporous aminosilica materials
Mesoporous aminosilica materials are active and selective heterogeneous catalysts for the nitroaldol reaction and have many physical and structural characteristics that can be tuned to desired effects. Previous work investigated the impact of tuning pore diameter on catalytic activity in the nitroaldol reaction and observed the highest activity with an MCM-41 support containing pores with an average diameter of 4.5 nm. Our understanding now suggests that these results may have been influenced by differences in microporosity between materials, undermining a comparison between non-microporous MCM-41 and SBA-15 that is known to have micropores. In this work, we introduce a line of SBA-15 supports with negligible microporosity and varied pore diameter. Compared to typical syntheses of SBA-15, these materials show increased catalytic activity as a result of decreased microporosity. Interestingly, a material with a pore diameter of 7.1 nm yields the highest activity among SBA-15-type materials with reduced micropore volume. This is similar to the catalytic activity recorded with an MCM-41 material, suggesting that perceived effects of pore diameter are less important than effects of microporosity. Since SBA-15 is more hydrothermally stable than MCM-41, the ability to use it as a suitable alternative for the nitroaldol reaction when microporosity is reduced is encouraging for future development.
期刊介绍:
Microporous and Mesoporous Materials covers novel and significant aspects of porous solids classified as either microporous (pore size up to 2 nm) or mesoporous (pore size 2 to 50 nm). The porosity should have a specific impact on the material properties or application. Typical examples are zeolites and zeolite-like materials, pillared materials, clathrasils and clathrates, carbon molecular sieves, ordered mesoporous materials, organic/inorganic porous hybrid materials, or porous metal oxides. Both natural and synthetic porous materials are within the scope of the journal.
Topics which are particularly of interest include:
All aspects of natural microporous and mesoporous solids
The synthesis of crystalline or amorphous porous materials
The physico-chemical characterization of microporous and mesoporous solids, especially spectroscopic and microscopic
The modification of microporous and mesoporous solids, for example by ion exchange or solid-state reactions
All topics related to diffusion of mobile species in the pores of microporous and mesoporous materials
Adsorption (and other separation techniques) using microporous or mesoporous adsorbents
Catalysis by microporous and mesoporous materials
Host/guest interactions
Theoretical chemistry and modelling of host/guest interactions
All topics related to the application of microporous and mesoporous materials in industrial catalysis, separation technology, environmental protection, electrochemistry, membranes, sensors, optical devices, etc.