Abstract: A method for electrodeposition of pure phase crystalline SnSb from deep eutectic ethaline is described. Thin films of SnSb were synthesized using a solution containing equimolar Sn(II) and Sb(III) chlorides as precursors, and ethaline (1:2 by weight of choline chloride and ethylene chloride) was used as the solvent for the electrodeposition solution. The purity of the product is important, as the impure phase is found to be detrimental to the material's lifetime as both a sodium-ion and a lithium-ion anode. For sodium-ions, the directly deposited electrode was able to retain 95% capacity after 300 cycles, and only fall below 80% capacity retention after 800 cycles when cycled versus sodium. The electrodeposited SnSb used as a Li-ion battery anode showed stability, only failing below 80% capacity retention after 400 cycles.

Abstract: A lithium-ion battery including an electrodeposited anode material having a micron-scale, three-dimensional porous foam structure separated from interpenetrating cathode material that fills the void space of the porous foam structure by a thin solid-state electrolyte which has been reductively polymerized onto the anode material in a uniform and pinhole free manner, which will significantly reduce the distance which the Li-ions are required to traverse upon the charge/discharge of the battery cell over other types of Li-ion cell designs, and a procedure for fabricating the battery are described. The interpenetrating three-dimensional structure of the cell will also provide larger energy densities than conventional solid-state Li-ion cells based on thin-film technologies. The electrodeposited anode may include an intermetallic composition effective for reversibly intercalating Li-ions.

Abstract: An apparatus and method for measuring the isoelectric pH for materials deposited on or otherwise affixed onto and in contact with an electrode surface, and a method for utilizing the isoelectric pH to form nanometer thickness, self-assembled layers on the material, are described. Forming such layers utilizing information obtained about the isoelectric pH values of the substrate and the coating is advantageous since the growth of the coating is self-limiting because once the surface charge has been neutralized there is no longer a driving force for the solid electrolyte coating thickness to increase, and uniform coatings without pinhole defects will be produced because a local driving force for assembly will exist if any bare electrode material is exposed to the solution. The present self-assembly procedure, when combined with electrodeposition, may be used to increase the coating thickness.

Abstract: Electrochemical methods for probing solid polymer electrolyte surface coatings on electrically conducting, active, three-dimensional electrode materials for use in lithium-ion batteries, to quantitatively determine the conformity, uniformity, and the presence of pinholes, and/or other defects in coatings, without requiring the detachment of the coating from the electrode or otherwise inducing damage to the coating, are described. Coated electrodes are submersed in an electrolyte solution containing a redox-active probe species which does not induce electrochemical damage to either the working electrode or the solid polymer electrolyte surface coating. For coated Cu2Sb working electrodes, molecules including a water-soluble redox active viologen moiety have been found to be effective.

Abstract: A lithium-ion battery having an anode including an array of nanowires electrochemically coated with a polymer electrolyte, and surrounded by a cathode matrix, forming thereby interpenetrating electrodes, wherein the diffusion length of the Li+ ions is significantly decreased, leading to faster charging/discharging, greater reversibility, and longer battery lifetime, is described. The battery design is applicable to a variety of battery materials. Methods for directly electrodepositing Cu2Sb from aqueous solutions at room temperature using citric acid as a complexing agent to form an array of nanowires for the anode, are also described. Conformal coating of poly-[Zn(4-vinyl-4?methyl-2,2?-bipyridine)3](PF6)2 by electroreductive polymerization onto films and high-aspect ratio nanowire arrays for a solid-state electrolyte is also described, as is reductive electropolymerization of a variety of vinyl monomers, such as those containing the acrylate functional group.

Abstract: Methods are described for forming insulating hybrid organic-inorganic solid electrolytes on conducting electrodes that are active materials in Li-ion batteries by electrochemical deposition, and for forming second conducting electrodes on the solid electrolytes using aqueous slurries, whereby Li-ion battery cells having solid electrolytes are generated. X-ray photoelectron spectroscopy is utilized for determining that the solid electrolytes are defect and pinhole free.

Abstract: Methods for reductively polymerizing vinylic based monomers from a solution thereof onto the surface of an electrode material, resulting in thin, electrically insulating solid-polymer electrolyte coatings strongly bound to the surface of the electrode material, are described. The strong bond permits a second electrode to be coated directly onto the solid-polymer electrolyte, thereby incorporating the required components for a Li-ion battery cell. At least one initiator species, which is readily reduced by accepting an electron from the electrode material, is included in electropolymerization deposition solution for permitting the polymerization of vinylic species that would otherwise not electrochemically polymerize without damage to either the electrode material or to the solvents employed.

Abstract: An apparatus and method for measuring the isoelectric pH for materials deposited on or otherwise affixed onto and in contact with an electrode surface, and a method for utilizing the isoelectric pH to form nanometer thickness, self-assembled layers on the material, are described. Forming such layers utilizing information obtained about the isoelectric pH values of the substrate and the coating is advantageous since the growth of the coating is self-limiting because once the surface charge has been neutralized there is no longer a driving force for the solid electrolyte coating thickness to increase, and uniform coatings without pinhole defects will be produced because a local driving force for assembly will exist if any bare electrode material is exposed to the solution. The present self-assembly procedure, when combined with electrodeposition, may be used to increase the coating thickness.

Abstract: An apparatus and method for measuring the isoelectric pH for materials deposited on or otherwise affixed onto and in contact with an electrode surface, and a method for utilizing the isoelectric pH to form nanometer thickness, self-assembled layers on the material, are described. Forming such layers utilizing information obtained about the isoelectric pH values of the substrate and the coating is advantageous since the growth of the coating is self-limiting because once the surface charge has been neutralized there is no longer a driving force for the solid electrolyte coating thickness to increase, and uniform coatings without pinhole defects will be produced because a local driving force for assembly will exist if any bare electrode material is exposed to the solution. The present self-assembly procedure, when combined with electrodeposition, may be used to increase the coating thickness.

Abstract: A lithium-ion battery having an anode including an array of nanowires electrochemically coated with a polymer electrolyte, and surrounded by a cathode matrix, forming thereby interpenetrating electrodes, wherein the diffusion length of the Li+ ions is significantly decreased, leading to faster charging/discharging, greater reversibility, and longer battery lifetime, is described. The battery design is applicable to a variety of battery materials. Methods for directly electrodepositing Cu2Sb from aqueous solutions at room temperature using citric acid as a complexing agent to form an array of nanowires for the anode, are also described. Conformal coating of poly-[Zn(4-vinyl-4? methyl-2,2?-bipyridine)3](PF6)2 by electroreductive polymerization onto films and high-aspect ratio nanowire arrays for a solid-state electrolyte is also described, as is reductive electropolymerization of a variety of vinyl monomers, such as those containing the acrylate functional group.

Abstract: A lithium-ion battery having an anode including an array of nanowires electrochemically coated with a polymer electrolyte, and surrounded by a cathode matrix, forming thereby interpenetrating electrodes, wherein the diffusion length of the Li+ ions is significantly decreased, leading to faster charging/discharging, greater reversibility, and longer battery lifetime, is described. The battery design is applicable to a variety of battery materials. Methods for directly electrodepositing Cu2Sb from aqueous solutions at room temperature using citric acid as a complexing agent to form an array of nanowires for the anode, are also described. Conformal coating of poly-[Zn(4-vinyl-4?methyl-2,2?-bipyridine)3](PF6)2 by electroreductive polymerization onto films and high-aspect ratio nanowire arrays for a solid-state electrolyte is also described, as is reductive electropolymerization of a variety of vinyl monomers, such as those containing the acrylate functional group.

Abstract: Electrochemical methods for probing solid polymer electrolyte surface coatings on electrically conducting, active, three-dimensional electrode materials for use in lithium-ion batteries, to quantitatively determine the conformity, uniformity, and the presence of pinholes, and/or other defects in coatings, without requiring the detachment of the coating from the electrode or otherwise inducing damage to the coating, are described. Coated electrodes are submersed in an electrolyte solution containing a redox-active probe species which does not induce electrochemical damage to either the working electrode or the solid polymer electrolyte surface coating. For coated Cu2Sb working electrodes, molecules including a water-soluble redox active viologen moiety have been found to be effective.

Abstract: Methods for reductively polymerizing vinylic based monomers from a solution thereof onto the surface of an electrode material, resulting in thin, electrically insulating solid-polymer electrolyte coatings strongly bound to the surface of the electrode material, are described. The strong bond permits a second electrode to be coated directly onto the solid-polymer electrolyte, thereby incorporating the required components for a Li-ion battery cell. At least one initiator species, which is readily reduced by accepting an electron from the electrode material, is included in electropolymerization deposition solution for permitting the polymerization of vinylic species that would otherwise not electrochemically polymerize without damage to either the electrode material or to the solvents employed.

Abstract: Methods are described for forming insulating hybrid organic-inorganic solid electrolytes on conducting electrodes that are active materials in Li-ion batteries by electrochemical deposition, and for forming second conducting electrodes on the solid electrolytes using aqueous slurries, whereby Li-ion battery cells having solid electrolytes are generated. X-ray photoelectron spectroscopy is utilized for determining that the solid electrolytes are defect and pinhole free.

Abstract: A lithium-ion battery including an electrodeposited anode material having a micron-scale, three-dimensional porous foam structure separated from interpenetrating cathode material that fills the void space of the porous foam structure by a thin solid-state electrolyte which has been reductively polymerized onto the anode material in a uniform and pinhole free manner, which will significantly reduce the distance which the Li-ions are required to traverse upon the charge/discharge of the battery cell over other types of Li-ion cell designs, and a procedure for fabricating the battery are described. The interpenetrating three-dimensional structure of the cell will also provide larger energy densities than conventional solid-state Li-ion cells based on thin-film technologies. The electrodeposited anode may include an intermetallic composition effective for reversibly intercalating Li-ions.

Abstract: An apparatus and method for measuring the isoelectric pH for materials deposited on or otherwise affixed onto and in contact with an electrode surface, and a method for utilizing the isoelectric pH to form nanometer thickness, self-assembled layers on the material, are described. Forming such layers utilizing information obtained about the isoelectric pH values of the substrate and the coating is advantageous since the growth of the coating is self-limiting because once the surface charge has been neutralized there is no longer a driving force for the solid electrolyte coating thickness to increase, and uniform coatings without pinhole defects will be produced because a local driving force for assembly will exist if any bare electrode material is exposed to the solution. The present self-assembly procedure, when combined with electrodeposition, may be used to increase the coating thickness.

Abstract: A lithium-ion battery having an anode including an array of nanowires electrochemically coated with a polymer electrolyte, and surrounded by a cathode matrix, forming thereby interpenetrating electrodes, wherein the diffusion length of the Li+ ions is significantly decreased, leading to faster charging/discharging, greater reversibility, and longer battery lifetime, is described. The battery design is applicable to a variety of battery materials. Methods for directly electrodepositing Cu2Sb from aqueous solutions at room temperature using citric acid as a complexing agent to form an array of nanowires for the anode, are also described. Conformal coating of poly-[Zn(4-vinyl-4?methyl-2,2?-bipyridine)3](PF6)2 by electroreductive polymerization onto films and high-aspect ratio nanowire arrays for a solid-state electrolyte is also described, as is reductive electropolymerization of a variety of vinyl monomers, such as those containing the acrylate functional group.