From zeozymes to bio-inspired heterogeneous solids: evolution of design strategies for sustainable catalysis
From zeozymes to bio-inspired heterogeneous solids: evolution of design strategies for sustainable catalysis
Bio-derived transition-metal complexes containing well-defined and well-characterized active sites can be anchored, in a site-isolated fashion, on to the inner walls of porous inorganic supports, for generating highly active and selective single-site heterogeneous catalysts, which can serve as effective functional mimics of metalloenzymes. The nature of an active site in an enzyme and its ability to harness a particular catalytic function with remarkable selectivity, via its protein tertiary structure, could be judiciously transposed to zeolitic architectures with specifically engineered active sites. Throughout this article we follow the progress and evolution of engineering enzymatic activity and selectivity in synthetically designed catalysts, emphasizing the importance and the advantages of the different synthesis methodologies in immobilizing bio-inspired catalytically active single-sites on varying solid supports. The benefits of such systems are highlighted in terms of their environmental impact by reduction of waste, mitigating the generation of greenhouse gases, boosting the enantioselectivity in heterogeneously catalyzed reactions and in the utilization of ‘greener’ oxidants; with conclusions drawn on how specific supports affect catalytic properties via modification of the local environment of the active site. The seminal contributions of Dr. Ratnasamy in this field have paved the way for a more fundamental understanding of how the support environment, and its interactions with the active site at a molecular level, can lead to development of structure–activity relationships, which in the future can provide avenues for specifically tailoring catalytic outcomes from a mechanistic standpoint.
enzyme mimics, bio-inspired catalysts, single-site heterogeneous catalysts, amino acids, zeozymes, organocatalysis
Xuereb, David J.
788dea38-5c2c-4590-93f0-67892c36472e
Dzierzak, Joanna
3b71e434-edcf-4a8d-afdb-f0cbd4ab89e0
Raja, Robert
74faf442-38a6-4ac1-84f9-b3c039cb392b
30 December 2012
Xuereb, David J.
788dea38-5c2c-4590-93f0-67892c36472e
Dzierzak, Joanna
3b71e434-edcf-4a8d-afdb-f0cbd4ab89e0
Raja, Robert
74faf442-38a6-4ac1-84f9-b3c039cb392b
Xuereb, David J., Dzierzak, Joanna and Raja, Robert
(2012)
From zeozymes to bio-inspired heterogeneous solids: evolution of design strategies for sustainable catalysis.
Catalysis Today.
(doi:10.1016/j.cattod.2012.04.050).
Abstract
Bio-derived transition-metal complexes containing well-defined and well-characterized active sites can be anchored, in a site-isolated fashion, on to the inner walls of porous inorganic supports, for generating highly active and selective single-site heterogeneous catalysts, which can serve as effective functional mimics of metalloenzymes. The nature of an active site in an enzyme and its ability to harness a particular catalytic function with remarkable selectivity, via its protein tertiary structure, could be judiciously transposed to zeolitic architectures with specifically engineered active sites. Throughout this article we follow the progress and evolution of engineering enzymatic activity and selectivity in synthetically designed catalysts, emphasizing the importance and the advantages of the different synthesis methodologies in immobilizing bio-inspired catalytically active single-sites on varying solid supports. The benefits of such systems are highlighted in terms of their environmental impact by reduction of waste, mitigating the generation of greenhouse gases, boosting the enantioselectivity in heterogeneously catalyzed reactions and in the utilization of ‘greener’ oxidants; with conclusions drawn on how specific supports affect catalytic properties via modification of the local environment of the active site. The seminal contributions of Dr. Ratnasamy in this field have paved the way for a more fundamental understanding of how the support environment, and its interactions with the active site at a molecular level, can lead to development of structure–activity relationships, which in the future can provide avenues for specifically tailoring catalytic outcomes from a mechanistic standpoint.
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More information
Accepted/In Press date: 6 April 2012
e-pub ahead of print date: 8 June 2012
Published date: 30 December 2012
Keywords:
enzyme mimics, bio-inspired catalysts, single-site heterogeneous catalysts, amino acids, zeozymes, organocatalysis
Organisations:
Chemistry
Identifiers
Local EPrints ID: 344394
URI: http://eprints.soton.ac.uk/id/eprint/344394
ISSN: 0920-5861
PURE UUID: 6ec9cac6-e77d-477c-a0fd-d6ea33fbb7d1
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Date deposited: 22 Oct 2012 15:21
Last modified: 15 Mar 2024 03:26
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Author:
David J. Xuereb
Author:
Joanna Dzierzak
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