Redox enzyme-embedded pyrene-poly(ethylenimine) hydrogel electrode for electrosynthesis
Devices, systems, and compositions of matter involving enzyme-mediated bioelectrocatalysis are disclosed and described. An enzyme electrode can include an electrode, a bioelectric material coupled to the electrode, the bioelectric material further including a water-permeable polymer matrix, a planar linker covalently coupled to the water-permeable polymer matrix and noncovalently coupled to the electrode, and electrochemically active oxidoreductase enzyme molecules functionally embedded in the water-permeable polymer matrix.
1. An enzyme electrode, comprising:
an electrode;
a bioelectric material coupled to the electrode, the bioelectric material further comprising:
a water-permeable polymer matrix;
a planar linker covalently coupled to the water-permeable polymer matrix and noncovalently coupled to the electrode; and
electrochemically active oxidoreductase enzyme molecules functionally embedded in the water-permeable polymer matrix, wherein the water-permeable polymer matrix comprises a covalently crosslinked hydrogel.
2. The enzyme electrode of claim 1 , wherein the covalently crosslinked hydrogel comprises a polymer selected from the group consisting of polyethylenimine, polyvinyl alcohol, polyvinylamine, polyallylamine, polyvinylpyridine, polyvinylimidazole, and mixtures and copolymers thereof.
3. The enzyme electrode of claim 1 , wherein the water-permeable polymer matrix comprises a linear polyethylenimine (LPEI) polymer.
4. The enzyme electrode of claim 1 , wherein the oxidoreductase enzyme molecules comprise an enzyme selected from the group consisting of nitrogenase, laccase, flavodoxin, ferredoxin, cytochrome c, hydrogenase, nitrate reductase, nitrite reductase, quinohemoproteins, multi-copper oxidases, heme containing enzymes, and combinations thereof.
5. The enzyme electrode of claim 1 , wherein the oxidoreductase enzyme molecules comprise an enzyme selected from the group consisting of nitrogenase, laccase, formate dehydrogenase, hydrogenase, and combinations thereof.
6. The enzyme electrode of claim 1 , wherein the electrode comprises a material selected from the group consisting of carbon nanotubes (CNTs), graphene, carbon black, carbon felt, indium-tin oxide (no), metals and metal alloys, and combinations thereof.
7. The enzyme electrode of claim 1 , wherein the planar linker is a polycyclic aromatic hydrocarbon or a polycyclic highly conjugated hydrocarbon.
8. The enzyme electrode of claim 1 , wherein the planar linker is pyrene.
9. A system, comprising:
a reaction chamber, comprising;
an enzyme electrode positioned within the reaction chamber, the enzyme electrode further comprising:
an electrode; and
a bioelectric material coupled to the electrode, the bioelectric material further comprising:
a water-permeable polymer matrix;
a planar linker covalently coupled to the water-permeable polymer matrix and noncovalently coupled to the electrode; and
electrochemically active oxidoreductase enzyme molecules functionally embedded in the water-permeable polymer matrix, wherein the water-permeable polymer matrix comprises a covalently crosslinked hydrogel;
a reactant input positioned to deliver a reactant to the enzyme electrode;
a product output positioned to receive a reaction product from the enzyme electrode; and
power supply contacts configured to electrically couple to a power supply and provide electrical current to the electrode when in use.
10. The system of claim 9 , wherein the oxidoreductase enzyme molecules comprise an enzyme selected from the group consisting of nitrogenase, laccase, flavodoxin, ferredoxin, cytochrome c, hydrogenase, nitrate reductase, nitrite reductase, quinohemoproteins, multi-copper oxidases, heme containing enzymes, and combinations thereof.
11. The system of claim 9 , wherein the oxidoreductase enzyme molecules comprise an enzyme selected from the group consisting of nitrogenase, laccase, formate dehydrogenase, hydrogenase, and combinations thereof.
12. The system of claim 9 , wherein the oxidoreductase enzyme molecules comprise laccase and the reaction product is water.
13. The system of claim 9 , wherein the oxidoreductase enzyme molecules comprise nitrogenase and the reaction product is a molecule selected from the group consisting of ammonia, methane, ethylene, propylene, and combinations thereof.
14. A polymer substrate, comprising:
a water-permeable polymer matrix; and
a planar linker covalently coupled to the water-permeable polymer matrix, wherein the planar linker is pyrene and the water-permeable polymer matrix comprises a covalently crosslinked hydrogel.
15. The polymer substrate of claim 14 , wherein the covalently crosslinked hydrogel comprises a polymer selected from the group consisting of polyamines, polyethers, polyamides, N-substituted polyamides, polyheterocycles, and mixtures and copolymers thereof.
16. The polymer substrate of claim 14 , wherein the covalently crosslinked hydrogel comprises a polymer selected from the group consisting of polyethylenimine, polyvinyl alcohol, polyvinylamine, polyallylamine, polyvinylpyridine, polyvinylimidazole, and mixtures and copolymers thereof.
17. The polymer substrate of claim 14 , wherein the water-permeable polymer matrix comprises a linear polyethylenimine (LPEI) polymer.
18. The polymer substrate of claim 14 , further comprising electrochemically active oxidoreductase enzyme molecules embedded in the water-permeable polymer matrix.