Spatially orthogonal chemical functionalization of a hierarchical pore network for catalytic cascade reactions

Christopher M.A. Parlett, Mark A. Isaacs, Simon K. Beaumont, Laura M. Bingham, Nicole S. Hondow, Karen Wilson, Adam F. Lee*

*Corresponding author for this work

Research output: Contribution to journalLetter

Abstract

The chemical functionality within porous architectures dictates their performance as heterogeneous catalysts; however, synthetic routes to control the spatial distribution of individual functions within porous solids are limited. Here we report the fabrication of spatially orthogonal bifunctional porous catalysts, through the stepwise template removal and chemical functionalization of an interconnected silica framework. Selective removal of polystyrene nanosphere templates from a lyotropic liquid crystal-templated silica sol–gel matrix, followed by extraction of the liquid crystal template, affords a hierarchical macroporous–mesoporous architecture. Decoupling of the individual template extractions allows independent functionalization of macropore and mesopore networks on the basis of chemical and/or size specificity. Spatial compartmentalization of, and directed molecular transport between, chemical functionalities affords control over the reaction sequence in catalytic cascades; herein illustrated by the Pd/Pt-catalysed oxidation of cinnamyl alcohol to cinnamic acid. We anticipate that our methodology will prompt further design of multifunctional materials comprising spatially compartmentalized functions.

Original languageEnglish
Pages (from-to)178-182
Number of pages5
JournalNature Materials
Volume15
Issue number2
Early online date16 Nov 2015
DOIs
Publication statusPublished - Feb 2016

Bibliographical note

Supplementary information: http://www.nature.com/nmat/journal/vaop/ncurrent/extref/nmat4478-s1.pdf

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    Parlett, C. M. A., Isaacs, M. A., Beaumont, S. K., Bingham, L. M., Hondow, N. S., Wilson, K., & Lee, A. F. (2016). Spatially orthogonal chemical functionalization of a hierarchical pore network for catalytic cascade reactions. Nature Materials, 15(2), 178-182. https://doi.org/10.1038/nmat4478