Systematic Enumeration of Microporous Solids: Towards Designer Catalysts

Thomas, John Meurig; Klinowski, Jacek

doi:10.1002/anie.200700666

Cited by 37 publications

(16 citation statements)

References 49 publications

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“…547 A database of hypothetical zeolite structures has been regarded as an important step toward "designer catalysts". 548 It can in principle be screened for zeolites that are suitable for particular applications using the same methodology that is described in this review to screen existing zeolites. To cope with a large number of structures and to identify efficiently those with useful and superior catalytic properties will clearly involve new computational approaches.…”

Section: Discussionmentioning

confidence: 99%

Molecular Simulations of Zeolites: Adsorption, Diffusion, and Shape Selectivity

2008

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Section: Discussionmentioning

confidence: 99%

Molecular Simulations of Zeolites: Adsorption, Diffusion, and Shape Selectivity

2008

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“…Over 190 distinct structural types of these microporous solids have so far been identified. However, in theory, judging by recent computational exercises, many millions more could, in principle, exist (Klinowski & Thomas 2007 (Raja & Thomas 1998), cyclohexane (Raja et al 2000) and toluene (Raja & Thomas 2006), in air or O 2 are formed. The article by Corá et al (2012) gives a quantum-mechanical interpretation of the way in which these SSHCs catalysts activate C-H bonds aerobically and at relatively low temperatures.…”

Section: Definition Of a Single-site Heterogeneous Catalystmentioning

confidence: 99%

The societal significance of catalysis and the growing practical importance of single-site heterogeneous catalysts

Thomas

2012

Proc. R. Soc. A.

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The concept of single-site heterogeneous catalysis, herein defined and extensively illustrated, offers a strategy for the design of new solid catalysts. By capitalizing on the opportunities presented by nanoporous materials to assemble a wide range of new, well-defined, catalytically active centres, it is possible to bring about numerous environmentally benign processes that can replace traditional methods of chemical production. The latter often employs aggressive, corrosive or hazardous reagents. By using both microporous (less than 20 Å diameter) and mesoporous solids (20-500 Å diameter), abundant scope exists for the construction and application of shape-selective, regio-selective and enantioselective catalysts.Keywords: nanoporous solids; selectivity; benign reagents; renewable resources; clean technology; sustainability BackgroundIt would be difficult to overestimate or exaggerate the practical importance of heterogeneous catalysis. Think of the products of petroleum and natural gas upon which civilized life now relies. All the following are manufactured through the agency of solid catalysts: fuels (for transport and heating), fabrics, flavours, fragrances, fertilizers, certain foodstuffs and most pharmaceuticals. Moreover, many of the molecular building blocks for the production of a wide range of the commodities used in everyday life are also generated catalytically: propylene, benzene, toluene, xylene, benzaldehyde, terephthalic acid, adipic acid, caprolactam (precursor of nylon 6) and a variety of monomers for polymeric composites.In fundamental, academic terms, the phenomenon of catalysis is endlessly fascinating and perennially new. Its study presents a multiplicity of intellectual and technological challenges. If we are to understand how and why certain molecules transform readily and others do not when they impinge upon an active site, it is necessary, continually, to devise, develop and deploy new techniques of investigation. This is equally true if our aim-and it is one of prime importanceis to know more about the nature of the active site itself. Without a detailed understanding of the atomic architecture of the catalytically active centre, we are unlikely to be in a position to improve existing catalysts or design superior new ones (Thomas 1997).Because they readily facilitate the separation of products from unreacted reagents, and also because they are amenable to the various processes of thermal reactivation, heterogeneous catalysts (which almost invariably involve solid, active phases) are much more convenient to use than homogeneous ones. Consequently, they now figure eminently in the drive towards green chemistry, clean technology and sustainability. Those scientists concerned with such topics are currently exploring new ways of generating both energy and novel materials and in this regard, solid catalysts are of pivotal importance.There is now an exigent need to design and develop catalysts that can cope with and transform readily available reactants in an environmentally benign manner. N...

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“…This challenge of reconstructing zeolite framework structures from nearest-neighbor connectivity information has been inspired and informed by the methods that have been developed to enumerate all possible hypothetical zeolite structures [23][24][25][26][27][28][29][30][31][32][33][34]. Our earlier graph theory approach was informed by the work of Treacy et al [31,32], while the simulated annealing approach presented in this paper is informed by the work of Deem and Newsam [23][24][25].…”

Section: Introductionmentioning

confidence: 99%