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New strategies for co-immobilization of dehydrogenases, NAD+ cofactor and redox mediators in sol-gel thin films for bioelectrocatalytic applications

Abstract : In this thesis, the research work was focused on designing functional layers based on silica sol-gel thin films to co-immobilize dehydrogenase, cofactor and electron mediator to get the most highly active systems. Immobilization of dehydrogenase in an active form in a sol-gel matrix was obtained by using a positively-charged polyelectrolyte as additive in the starting sol. The optimal sol can be deposited by evaporation or by electrodeposition and was successfully deposited in macroporous electrodes. The immobilization of the cofactor was investigated by simple entrapment, adsorption to carbon nanotube (CNTs), encapsulation of NAD+ chemically attached to dextran(NAD-dextran), and by in-situ coupling with glycidoxypropyltrimethoxysilane (GPS). The last approach allowed stable immobilization of the cofactor. Several mediators (Fc-PEI, Fc-Silane or Osmium polymer) were successfully co-immobilized with dehydrogenase and cofactor in the sol-gel matrix deposited by drop-coating. However, such co-immobilization did not operate in the electrogenerated sol-gel films. The strategies based on CNTs for mediator immobilization were finally developed. They include (1) micro-wave treatment (MWCNTs-µW), (2) electrochemical deposition of poly(methylene green) (MWCNTs-PMG), and (3) wrapping by osmium(III) polymer (MWCNTs-Os). MWCNTs-Os has been the only system that was successfully combined with sol-gel electrodeposition for co-immobilization of dehydrogenase and cofactor.
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  • HAL Id : tel-01746228, version 1

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Zhijie Wang. New strategies for co-immobilization of dehydrogenases, NAD+ cofactor and redox mediators in sol-gel thin films for bioelectrocatalytic applications. Other. Université Henri Poincaré - Nancy 1, 2011. English. ⟨NNT : 2011NAN10061⟩. ⟨tel-01746228⟩

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