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Nanoporous oxidic solids: the confluence of heterogeneous and homogeneous catalysis

Nanoporous oxidic solids: the confluence of heterogeneous and homogeneous catalysis
Nanoporous oxidic solids: the confluence of heterogeneous and homogeneous catalysis
The several factors that render certain kinds of nanoporous oxidic solids valuable for the design of a wide range of new heterogeneous catalysts are outlined and exemplified. These factors include: (i), their relative ease of preparation, when both mesoporous siliceous frameworks (ca. 20 to 250 diameter pores) and microporous framework-substituted aluminophosphates (ca. 4 to 14 diameter pores) can be tailored to suit particular catalytic needs according to whether regiospecific or enantio- or shape-selective conversions are the goal; (ii), the enormous internal (three-dimensional) areas that these nanoporous solids possess (typically 103 m2 g-1) and the consequential ease of access of reactants through the internal pores of the solids; (iii), the ability, by judicious solid-state preparative methods to assemble spatially isolated, single-site active centres at the internal surfaces of these open-structure solids, thereby making the heterogeneous catalyst simulate the characteristic features of homogenous and enzymatic catalysts; (iv), the wide variety of in situ, time-resolved and ex situ experimental techniques, coupled with computational methods, that can pin-point the precise structure of the active site under operating conditions and facilitate the formulation of reaction intermediates and mechanisms. Varieties of catalysts are described for the synthesis (often under environmentally benign and solvent-free conditions) of a wide range of organic materials including commodity chemicals (such as adipic and terephthalic acid), fine and pharmaceutical chemicals (e.g. vitamin B3), alkenes, epoxides, and for the photocatalytic preferential destruction of carbon monoxide in the presence of hydrogen. Nanoporous oxidic solids are ideal materials to investigate the phenomenology of catalysis because, in many of them, little distinction exists between a model and a real catalyst.
1463-9076
2799-2825
Thomas, John Meurig
f1d9bb61-4e2c-4c4b-8115-953d0f3d36bd
Hernandez-Garrido, Juan Carlos
6bc614e3-32ed-4281-92e6-e1d0f48f813b
Raja, Robert
74faf442-38a6-4ac1-84f9-b3c039cb392b
Bell, Robert G.
47951797-cf55-4b61-bc7a-25a1da365711
Thomas, John Meurig
f1d9bb61-4e2c-4c4b-8115-953d0f3d36bd
Hernandez-Garrido, Juan Carlos
6bc614e3-32ed-4281-92e6-e1d0f48f813b
Raja, Robert
74faf442-38a6-4ac1-84f9-b3c039cb392b
Bell, Robert G.
47951797-cf55-4b61-bc7a-25a1da365711

Thomas, John Meurig, Hernandez-Garrido, Juan Carlos, Raja, Robert and Bell, Robert G. (2009) Nanoporous oxidic solids: the confluence of heterogeneous and homogeneous catalysis. Physical Chemistry Chemical Physics, 11 (16), 2799-2825. (doi:10.1039/b819249a).

Record type: Article

Abstract

The several factors that render certain kinds of nanoporous oxidic solids valuable for the design of a wide range of new heterogeneous catalysts are outlined and exemplified. These factors include: (i), their relative ease of preparation, when both mesoporous siliceous frameworks (ca. 20 to 250 diameter pores) and microporous framework-substituted aluminophosphates (ca. 4 to 14 diameter pores) can be tailored to suit particular catalytic needs according to whether regiospecific or enantio- or shape-selective conversions are the goal; (ii), the enormous internal (three-dimensional) areas that these nanoporous solids possess (typically 103 m2 g-1) and the consequential ease of access of reactants through the internal pores of the solids; (iii), the ability, by judicious solid-state preparative methods to assemble spatially isolated, single-site active centres at the internal surfaces of these open-structure solids, thereby making the heterogeneous catalyst simulate the characteristic features of homogenous and enzymatic catalysts; (iv), the wide variety of in situ, time-resolved and ex situ experimental techniques, coupled with computational methods, that can pin-point the precise structure of the active site under operating conditions and facilitate the formulation of reaction intermediates and mechanisms. Varieties of catalysts are described for the synthesis (often under environmentally benign and solvent-free conditions) of a wide range of organic materials including commodity chemicals (such as adipic and terephthalic acid), fine and pharmaceutical chemicals (e.g. vitamin B3), alkenes, epoxides, and for the photocatalytic preferential destruction of carbon monoxide in the presence of hydrogen. Nanoporous oxidic solids are ideal materials to investigate the phenomenology of catalysis because, in many of them, little distinction exists between a model and a real catalyst.

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Published date: 2009

Identifiers

Local EPrints ID: 148281
URI: http://eprints.soton.ac.uk/id/eprint/148281
ISSN: 1463-9076
PURE UUID: f7501be3-144c-411d-b84f-84a262b78843
ORCID for Robert Raja: ORCID iD orcid.org/0000-0002-4161-7053

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Date deposited: 28 Apr 2010 08:52
Last modified: 03 Dec 2019 01:46

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