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

Parlett, Christopher M.A., Isaacs, Mark A., Beaumont, Simon K., Bingham, Laura M., Hondow, Nicole S., Wilson, Karen and Lee, Adam F. (2016). Spatially orthogonal chemical functionalization of a hierarchical pore network for catalytic cascade reactions. Nature Materials, 15 (2), pp. 178-182.


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.

Publication DOI:
Divisions: Engineering & Applied Sciences
Engineering & Applied Sciences > Chemical Engineering & Applied Chemistry
Engineering & Applied Sciences > European Bioenergy Research Institute (EBRI)
Additional Information: Supplementary information:
Uncontrolled Keywords: Mechanical Engineering,Mechanics of Materials,Condensed Matter Physics,Materials Science(all),Chemistry(all)
Full Text Link: http://dro.dur. ... 979/1/16979.pdf
Related URLs: http://www.scop ... tnerID=8YFLogxK (Scopus URL)
https://www.nat ... ticles/nmat4478 (Publisher URL)
Published Date: 2016-02
Authors: Parlett, Christopher M.A. ( 0000-0002-3651-7314)
Isaacs, Mark A.
Beaumont, Simon K.
Bingham, Laura M.
Hondow, Nicole S.
Wilson, Karen ( 0000-0003-4873-708X)
Lee, Adam F. ( 0000-0002-2153-1391)

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