4.6 Article

Reaction-diffusion hydrogels from urease enzyme particles for patterned coatings

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COMMUNICATIONS CHEMISTRY
卷 4, 期 1, 页码 -

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NATURE RESEARCH
DOI: 10.1038/s42004-021-00538-7

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资金

  1. Engineering and Physical Sciences Research Council (EPSRC) [EP/K030574/2]
  2. Louisiana Board of Regents
  3. EPSRC [EP/K030574/2] Funding Source: UKRI

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Enzyme reaction networks can control the formation of hydrogels in spatial and temporal dimensions. By mimicking biofilm formation, urease-containing particles are used to induce the polymerization of thiol-acrylate, with properties adjusted by solution viscosity, particle dimensions, and spatial configuration. This method allows for the growth of enzyme-hydrogels with tunable properties for potential applications in biocatalytic flow reactors.
Enzyme reaction networks can control the spatial and temporal formation of hydrogels. Here, inspired by biofilm formation, urease-containing particles create a propagating pH gradient which induces thiol-acrylate polymerization, with properties tuned by solution viscosity, particle dimensions, and spatial configuration. The reaction and diffusion of small molecules is used to initiate the formation of protective polymeric layers, or biofilms, that attach cells to surfaces. Here, inspired by biofilm formation, we present a general method for the growth of hydrogels from urease enzyme-particles by combining production of ammonia with a pH-regulated polymerization reaction in solution. We show through experiments and simulations how the propagating basic front and thiol-acrylate polymerization were continuously maintained by the localized urease reaction in the presence of urea, resulting in hydrogel layers around the enzyme particles at surfaces, interfaces or in motion. The hydrogels adhere the enzyme-particles to surfaces and have a tunable growth rate of the order of 10 mu m min(-1) that depends on the size and spatial distribution of particles. This approach can be exploited to create enzyme-hydrogels or chemically patterned coatings for applications in biocatalytic flow reactors.

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