Control of microenvironment around enzymes by hydrogels

Abstract

The oxidation of substrates by P450 is regulated by introducing an interaction site with decoy molecules into polymer hydrogels.

Harnessing P450 Enzyme for Biotechnology and Synthetic Biology

“…They demonstrated the enzymes activity could be modulated in an artificial microenvironment due to the charge and hydrophobicity of the polymer. Interestingly, the oxidation rate of enzyme‐immobilized hydrogels increased as the cross‐linking density in the hydrogels increased [106] . Nöth et al .…”

“…[96] Kobayashi et al encapsulated P450 SPα into poly-N-isopropylacrylamide (pNIPAAm) based hydrogel and investigated the effects of the cross-linking density, polymer properties and thermal stimulation on the oxidation reaction rate. [106] They demonstrated the enzymes activity could be modulated in an artificial microenvironment due to the charge and hydrophobicity of the polymer. Interestingly, the oxidation rate of enzyme-immobilized hydrogels increased as the cross-linking density in the hydrogels increased.…”

“…Interestingly, the oxidation rate of enzyme-immobilized hydrogels increased as the cross-linking density in the hydrogels increased. [106] Nöth et al immobilized P450BM3 in a new type of positively charged microgel named as PVCL/VimQ (poly(N-vinylcaprolactam) microgel with 1-vinyl-3-methylimidazolium) as a comonomer via electrostatic adsorption. [107] The activity of the P450 microgel showed comparable activity with the free enzyme, high tolerance to organic solvent and excellent recyclability.…”

Three-Dimensional Chiral Supramolecular Microenvironment Strategy for Enhanced Biocatalysis

“…6 Of specific interest has been the incorporation of enzymes into or onto materials to impart materials with biological activity and enhance enzyme properties, such as good catalytic efficiency, high storage stability, and efficient recyclability. Related materials include polymeric supports, 7 nanomaterials, 8,9 microcapsules, 10 hydrogels, 11 and mesoporous silicate materials. 12 Despite extensive efforts made on developing favorable materials of enzyme, some challenges, like a low catalytic activity, toughness of recovery and recycling, remain.…”

“…Of specific interest has been the incorporation of enzymes into or onto materials to impart materials with biological activity and enhance enzyme properties, such as good catalytic efficiency, high storage stability, and efficient recyclability. Related materials include polymeric supports, nanomaterials, , microcapsules, hydrogels, and mesoporous silicate materials . Despite extensive efforts made on developing favorable materials of enzyme, some challenges, like a low catalytic activity, toughness of recovery and recycling, remain. , Overcoming the detrimental effects has proven to be exceptionally difficult because it is a challenge to construct the native three-dimensional (3D) microenvironment of enzyme, and none of the above materials can achieve this goal. , Research on the microenvironment of enzymes found that the precise spatial arrangement of the constituent amino acids building blocks is the key to the efficient catalysis achieved by enzymes and that the microenvironment of the catalytic active site is set by the inherent chirality of these blocks. , Although the chirality is essential for a 3D microenvironment of enzyme catalysis, the effect of the 3D biomimetic chiral microenvironment on enzyme remains poorly understood, and few chiral materials have been used for the recovery and recycling of enzymes.…”