Electrochemical devices or systems comprising redox-functionalized electrodes and uses thereof
US-2020399146-A1 · Dec 24, 2020 · US
US11779861B2 · US · B2
| Field | Value |
|---|---|
| Publication number | US-11779861-B2 |
| Application number | US-201716345676-A |
| Country | US |
| Kind code | B2 |
| Filing date | Oct 27, 2017 |
| Priority date | Oct 27, 2016 |
| Publication date | Oct 10, 2023 |
| Grant date | Oct 10, 2023 |
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Various aspects described herein relate to electrochemical devices, e.g., for separation of one or more biomolecules from a solution, and methods of using the same. Methods for using the electrochemical devices for biocatalysis are also described herein.
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What is claimed is: 1. A method of separating a target biomolecule from an aqueous solution comprising: contacting the aqueous solution with: (i) a first electrode comprising a first substrate and a first redox species immobilized to the first substrate, wherein the first redox species is selective toward a target functional group of the target biomolecule based on a specific chemical interaction between the first redox species and the target functional group, wherein the specific chemical interaction is activated by a Faradaic/redox reaction; and (ii) a second electrode; and applying an electrical potential across the first electrode and the second electrode such that the first redox species transforms from a first redox state to a second redox state and binds to the target functional group of the target biomolecule present in the aqueous solution, thereby separating the target biomolecule from the aqueous solution. 2. The method of claim 1 , wherein the target biomolecule is selected from the group consisting of proteins, nucleic acids, viruses, bacteria, peptides, amino acid fragments, antibodies, enzymes, sugars, fatty acids, lipids, vitamins, co-enzymes, and combinations thereof. 3. The method of claim 1 , wherein the first redox species is an organometallic compound or metallocene, an organic species or organic polymer, a crystalline solid, a cyclodextrin-based system, a metal-polypyrridyl system, a metal dicarbamate, a cryptand, a redox-active arene, a dendrimer comprising a redox-active center, or a redox-active organic macrocycle. 4. The method of claim 1 , wherein the first redox species is an organometallic compound or metallocene. 5. The method of claim 1 , wherein the target functional group comprises a carboxylate moiety, an amino group, a hydrophobic domain, a hydrophilic domain, and/or a specific charge distribution. 6. The method of claim 1 , wherein: (i) the aqueous solution has a pH that is above an isoelectric point of the target biomolecule for anion-selective separation; or (ii) the aqueous solution has a pH that is below the isoelectric point of the target biomolecule for cation-selective separation. 7. The method of claim 1 , wherein the aqueous solution has an ionic strength of 0 mM to 10 M. 8. The method of claim 1 , wherein the target biomolecule is present in the aqueous solution at a concentration of about 50 μg/mL to about 5000 mg/mL. 9. The method of claim 1 , wherein: (i) the first electrode is an anodic electrode having an electrical potential of about 0.1 V to about 0.8 V; or (ii) the first electrode is a cathodic electrode having an electrical potential of about 0 V to about −1 V. 10. The method of claim 1 , wherein the target biomolecule has a weight average molecular weight of about 10 kDa to about 100 kDa. 11. The method of claim 1 , wherein the second electrode comprises a second substrate and a second redox species immobilized to the second substrate. 12. The method of claim 11 , wherein the second redox species is selective toward an ionic species present in the aqueous solution such that the second electrode captures the ionic species. 13. The method of claim 12 , wherein the ionic species is a cationic species, optionally which is a positively-charged biomolecule selected from the group consisting of proteins, DNA, RNA, viruses, peptides, amino acid fragments, antibodies, enzymes, sugars, fatty acids, lipids, vitamins, co-enzymes, and combinations thereof. 14. The method of claim 13 , wherein the cationic species is selected from the group consisting of heavy metals, transition metals, lanthanides, organic cations, metal-organic cations, alkali metal ions, alkaline earth metal ions, and rare earth metal ions. 15. The method of claim 11 , wherein the second redox species is chemically different from the first redox species. 16. The method of claim 11 , wherein the second redox species is a charged species. 17. The method of claim 11 , wherein the second redox species is a molecule comprising an electron-accepting functional moiety. 18. The method of claim 11 , wherein the second redox species is a charged species of the first redox species, optionally wherein the first redox species is selected from the group consisting of quinone-containing polymers, cobaltocenium-containing polymers, polypyrrole, cyclodextrin-based systems, metal-polypyridyl systems, metal-dicarbamates, cryptands, dendrimers comprising redox-active centers, and redox-active organic macrocycles. 19. The method of claim 1 , wherein the first substrate comprises multiwalled carbon nanotubes and the first redox species comprises poly(vinyl)ferrocene (PVF). 20. The method of claim 12 , further comprising reversing the applied electrical potential to release the bound target biomolecule from the first electrode and/or the captured ionic species from the second electrode. 21. The method of claim 20 , wherein the release of the bound biomolecule and/or the captured ionic species is performed: (i) at the same pH as the aqueous solution; or (ii) at a different pH from the aqueous solution. 22. The method of claim 1 , wherein the aqueous solution further comprises at least one non-target biomolecule. 23. The method of claim 22 , wherein the at least one non-target biomolecule does not comprise the same target functional group as the target biomolecule. 24. The method of claim 22 , wherein the at least one non-target biomolecule has a molecular weight that is different from that of the target biomolecule. 25. The method of claim 22 , wherein the at least one non-target biomolecule has an isoelectric point that is different from that of the target biomolecule. 26. The method of claim 22 , wherein the at least one non-target biomolecule has a charge distribution that is different from that of the target biomolecule. 27. The method of claim 22 , wherein the at least one non-target biomolecule has a dipole moment that is different from that of the target biomolecule. 28. The method of claim 24 , wherein the at least one non-target biomolecule comprises a functional group that is the same as the target functional group of the target biomolecule.
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