# US 10,766,795 B2 · Electrochemical devices or systems comprising redox-functionalized electrodes and uses thereof

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- Number: US 10,766,795 B2
- Document ID: US10766795B2
- Status: Granted
- Kind: B2
- Application number: 15/336,637
- Filed: 2016-10-27
- Published: 2017-04-27
- Granted: 2020-09-08
- Earliest claimed: 2015-10-27
- Assignees: Massachusetts Institute of Technology
- Applicants: Massachusetts Institute of Technology
- Inventors: Xiao Su; Demetra S. Achilleos; Trevor Alan Hatton
- Web page: https://patentgrep.com/patent/US10766795B2

## CPC

- C02F 1/469: by electrochemical separation, e.g. by electro-osmosis, electrodialysis, electrophoresis
- C02F 1/4672: {by electrooxydation}
- C02F 2001/46138: {Electrodes comprising a substrate and a coating}
- C02F 2101/20: Heavy metals or heavy metal compounds
- C02F 2101/301: {Detergents, surfactants}
- C02F 2101/306: {Pesticides}
- C02F 2103/343: {from the pharmaceutical industry, e.g. containing antibiotics}
- C02F 2201/46105: Details relating to the electrolytic devices
- Y02W 10/37: using solar energy
- C02F: TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE (separation in general B01D; special arrangements on waterborne vessels of installations for treating water, waste water or sewage, e.g. for producing fresh water, B63J; adding materials to water to prevent corrosion C23F; treating radioactively-contaminated liquids G21F9/04; regeneration of reactants for recirculation into processes, see the relevant places for the processes)
- Y02W: CLIMATE CHANGE MITIGATION TECHNOLOGIES RELATED TO WASTEWATER TREATMENT OR WASTE MANAGEMENT

## Abstract

Various aspects described herein relate to electrochemical devices, e.g., for separation of one or more target organic or inorganic molecules (e.g., charged or neutral molecules) from solution, and methods of using the same. In particular embodiments, the electrochemical devices and methods described herein involve at least one redox-functionalized electrode, wherein the electrode comprises an immobilized redox-species that is selective toward a target molecule (e.g., charged molecule such as ion or neutral molecule). The selectivity is based on a Faradaic/redox-activated chemical interaction (e.g., directional hydrogen binding) between the oxidized state of the redox species and a moiety of the target molecule (e.g., charged molecule such as ion or neutral molecule).

## Claims

### Claim 1

A method of separating at least one target molecule from a fluid source comprising:
a. placing in a fluid source (i) a first electrode comprising a first solid substrate and a first redox species immobilized to the first solid substrate; and (ii) a second electrode comprising a second solid substrate and a second redox species immobilized to the second solid substrate, wherein the first redox species and the second redox species comprise chemically different metallocenes; and
b. applying an electrical potential across the first electrode and the second electrode such that the first redox species transforms to an oxidized state and selectively binds to a target electron-donating functional group of a target molecule present in the fluid source,
thereby separating at least one target molecule comprising the target electron-donating functional group from the fluid source.

### Claim 2 (depends on 1)

The method of claim 1, wherein the second redox species selectively captures a cationic species present in the fluid source.

### Claim 3 (depends on 2)

The method of claim 2, wherein the cationic species is selected from the group consisting of heavy metals, transition metals, lanthanides, organic cations, inorganic cations, metal-organic cations, metal-inorganic cations, alkali metal ions, alkaline earth metal ions, and rare earth metal ions.

### Claim 4 (depends on 2)

The method of claim 2, wherein the target molecule and/or the cationic species is a micropollutant or a nanopollutant.

### Claim 5 (depends on 2)

The method of claim 2, further comprising reversing the applied electrical potential to release the bound target molecule and/or the captured cationic species from the electrodes.

### Claim 6 (depends on 1)

The method of claim 1, wherein the target molecule is an organic anion, an inorganic anion, a neutral molecule, or an oxygen-containing complex.

### Claim 7 (depends on 1)

The method of claim 1, wherein the target molecule comprises a carboxylate, sulfonate, phosphonate, carbonate, carbamate, phosphate, sulfate, chromate, vanadate, manganate, and/or selenate.

### Claim 8 (depends on 1)

The method of claim 1, wherein that target molecular is or comprises paraquat, quinclorac, sodium dodecyl benzoate, ibuprofen, or 2,45-trichlorophenoxyacetic acid.

### Claim 9

A method of increasing separation efficiency of a target molecule from a fluid source or increasing energy storage performance of an electrochemical device or system comprising:
a. placing in a fluid source (i) a first electrode comprising a first solid substrate and a first redox species immobilized to the first solid substrate; and (ii) a second electrode comprising a second solid substrate and a second redox species immobilized to the solid second solid substrate, wherein the first redox species and the second redox species comprise chemically different metallocenes; and
b. applying an electrical potential across the first electrode and the second electrode such that the first redox species transforms to an oxidized state and selectively binds to a target electron-donating functional group of a target molecule present in the fluid source and the second redox species undergoes a self-exchange reaction within the second electrode,
thereby increasing the separation efficiency or energy storage performance of the electrochemical device or system by diverting at least a portion of electron transfer toward the self-exchange reaction of the second redox species and reducing electron transfer toward the fluid source.

### Claim 10 (depends on 9)

The method of claim 9, wherein the fluid source is an aqueous fluid or an organic fluid.
