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Jorge AR, Chernobryva M, Rigby SE, et al. Incorporation of Cobalt-Cyclen Complexes into Templated Nanogels Results in Enhanced Activity. Chemistry. 2015;22(11):3764-74doi: 10.1002/chem.201503946.
Jorge, A. R., Chernobryva, M., Rigby, S. E., Watkinson, M., & Resmini, M. (2016). Incorporation of Cobalt-Cyclen Complexes into Templated Nanogels Results in Enhanced Activity. Chemistry (Weinheim an der Bergstrasse, Germany), 22(11), 3764-74. https://doi.org/10.1002/chem.201503946
Jorge, Ana Rita, et al. "Incorporation of Cobalt-Cyclen Complexes into Templated Nanogels Results in Enhanced Activity." Chemistry (Weinheim an der Bergstrasse, Germany) vol. 22,11 (2016): 3764-74. doi: https://doi.org/10.1002/chem.201503946
Jorge AR, Chernobryva M, Rigby SE, Watkinson M, Resmini M. Incorporation of Cobalt-Cyclen Complexes into Templated Nanogels Results in Enhanced Activity. Chemistry. 2016 Mar 07;22(11):3764-74. doi: 10.1002/chem.201503946. Epub 2015 Dec 10. PMID: 26661923; PMCID: PMC4797703.
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Chemistry. 2016 Mar 07;22(11):3764-74. doi: 10.1002/chem.201503946. Epub 2015 Dec 10.

Incorporation of Cobalt-Cyclen Complexes into Templated Nanogels Results in Enhanced Activity.

Chemistry (Weinheim an der Bergstrasse, Germany)

Ana Rita Jorge, Mariya Chernobryva, Stephen E J Rigby, Michael Watkinson, Marina Resmini

Affiliations

  1. Department of Chemistry and Biochemistry, School of Biological and Chemical Sciences, Queen Mary University of London, Mile End Road, London, E1 4NS, UK.
  2. Faculty of Life Sciences, Manchester Institute of Biotechnology, 131 Princess Street, Manchester, M1 7DN, UK.
  3. Department of Chemistry and Biochemistry, School of Biological and Chemical Sciences, Queen Mary University of London, Mile End Road, London, E1 4NS, UK. [email protected].
  4. Department of Chemistry and Biochemistry, School of Biological and Chemical Sciences, Queen Mary University of London, Mile End Road, London, E1 4NS, UK. [email protected].

PMID: 26661923 PMCID: PMC4797703 DOI: 10.1002/chem.201503946

Abstract

Recent advances in nanomaterials have identified nanogels as an excellent matrix for novel biomimetic catalysts using the molecular imprinting approach. Polymerisable Co-cyclen complexes with phosphonate and carbonate templates have been prepared, fully characterised and used to obtain nanogels that show high activity and turnover with low catalytic load, compared to the free complex, in the hydrolysis of 4-nitrophenyl phosphate, a nerve agent simulant. This work demonstrates that the chemical structure of the template has an impact on the coordination geometry and oxidation state of the metal centre in the polymerisable complex resulting in very significant changes in the catalytic properties of the polymeric matrix. Both pseudo-octahedral cobalt(III) and trigonal-bipyramidal cobalt(II) structures have been used for the synthesis of imprinted nanogels, and the catalytic data demonstrate that: i) the imprinted nanogels can be used in 15 % load and show turnover; ii) the structural differences in the polymeric matrices resulting from the imprinting approach with different templates are responsible for the molecular recognition capabilities and the catalytic activity. Nanogel P1, imprinted with the carbonate template, shows >50 % higher catalytic activity than P2 imprinted with the phosphonate.

© 2016 The Authors. Published by Wiley-VCH Verlag GmbH & Co. KGaA.

Keywords: cyclen; enzyme mimics; molecular imprinting; nanogels; phosphatase

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