Abstract
An industrial process for the selective activation of methane under mild conditions would be highly valuable for controlling emissions to the environment and for utilizing vast new sources of natural gas. The only selective catalysts for methane activation and conversion to methanol under mild conditions are methane monooxygenases (MMOs) found in methanotrophic bacteria; however, these enzymes are not amenable to standard enzyme immobilization approaches. Using particulate methane monooxygenase (pMMO), we create a biocatalytic polymer material that converts methane to methanol. We demonstrate embedding the material within a silicone lattice to create mechanically robust, gas-permeable membranes, and direct printing of micron-scale structures with controlled geometry. Remarkably, the enzymes retain up to 100% activity in the polymer construct. The printed enzyme-embedded polymer motif is highly flexible for future development and should be useful in a wide range of applications, especially those involving gas–liquid reactions.
Highlights
An industrial process for the selective activation of methane under mild conditions would be highly valuable for controlling emissions to the environment and for utilizing vast new sources of natural gas
We developed and optimized a biocatalytic material consisting of active particulate methane monooxygenase (pMMO) embedded in polyethylene glycol diacrylate (PEGDA) hydrogel
In an effort to develop a biocatalytic material that can be molded into controlled, predetermined structures with tunable permeability and surface area, we explored several methods for embedding Methylococcus capsulatus (Bath) pMMO in a PEGDA-based polymer hydrogel
Summary
An industrial process for the selective activation of methane under mild conditions would be highly valuable for controlling emissions to the environment and for utilizing vast new sources of natural gas. Isolated enzymes offer the promise of highly controlled reactions at ambient conditions with higher conversion efficiency and greater flexibility of reactor and process design[8]. There are both soluble (sMMO) and particulate (pMMO) forms of MMO5,9. In order to use pMMO most effectively, the traditional methods of enzyme immobilization and exposure to reactants are not sufficient These typical methods include crosslinking enzymes or immobilizing them on a solid support so that they can be separated from the products[13] and carrying out batch reactions in the aqueous phase in a stirred tank reactor. The majority of the surface area in mesoporous materials is accessible only to proteins significantly smaller than 50 nm (ref. 21), and would be inaccessible to the large (44100 nm), optically opaque vesicles and liposomes that comprise membrane-bound pMMO
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