Patent
US 9,847,184Supercapacitor Electrode Having Highly Oriented and Closely Packed Graphene Sheets and Production Process
Aruna Zhamu, Bor Z. Jang
US
Copyright © 2026 Matter42. All rights reserved.
Patent drawings and their descriptions. Click a drawing to enlarge it.
FIG. 1 (B) having a thickness > 100 nm. These flakes can be formed into graphite paper or mat 106 using a paper- or mat-making process. 15 This expanded …
FIG.2 Schematic of a conventional activated carbon-based supercapacitor cell.
FIG.3(A) Schematic drawing to illustrate an example of a compressing and consolidating operation (using a mold cavity cell equipped with a piston or ram) for …
FIG. 4. There are several significant observations that can be made from these data: (A) Given comparable electrode thickness, the(presently invented graphene …
FIG.5 Ragone plots (grav in etric and volumetric power density vs. energy density) of symmetric supercapacitor (EDLC) cells containing isolated nitrogen-doped …
FIG.6 shows the Ragone plots of two pristine graphene-based EDLC supercapacitors, one 5 having graphene sheets parallel to the current collector surface plane …
FIG.7 are the Ragone plots of two graphene-conductive polymer redox supercapacitors (pseudo-capacitors) having electrodes based on graphene/sulfonated …
FIG.8 Ragone plots of lithium ion capacitor (LIC) cells containing pristine graphene sheets as the electrode ac t ive material and lithium salt-PC/DEC organic …
FIG.9 for reduced graphene oxide-based EDLC supercapacitors. The cell-level gravimetric and volumetric energy densities plotted over the achievable electrode …
FIG. 10 The cell-level gravimetric energy densities plotted over the achievable active material proportion (active material weight/total cell weight) in a …
Claims define the patent's legal scope. Independent claims stand alone; dependent claims (nested) narrow them. Click a claim to expand its dependents.
A process for producing an electrolyte-impregnated laminar graphene structure for use as a supercapacitor electrode, said process comprising: (a) preparing a graphene dispersion having multiple isolated graphene sheets dispersed in a liquid or gel electrolyte; and (b) subjecting said graphene dispersion to a forced assembly procedure, forcing said multiple graphene sheets to assemble into said electrolyte-impregnated laminar graphene structure, wherein said multiple graphene sheets are alternately spaced by thin electrolyte layers, SVG 14998672.10-10-2017.J₈LT₆EDBRXEAPX1.CLM.1.17.1857.1554.1950.1611.svg 0.19 0.31 Chemistry Black and white having a thickness from 0.4 nm to 10 nm, and said multiple graphene sheets are substantially aligned along a desired direction, and wherein said laminar graphene structure has a physical density from 0.5 to 1.7 g/cm 3 and a specific surface area from 50 to 3,300, when measured in a dried state of said laminar structure with said electrolyte removed. Original
The process of claim 1, wherein said isolated graphene sheets are selected from a pristine graphene or a non-pristine graphene material, having a content of non-carbon elements greater than 2% by weight, selected from graphene oxide, reduced graphene oxide, graphene fluoride, graphene chloride, graphene bromide, graphene iodide, hydrogenated graphene, nitrogenated graphene, chemically functionalized graphene, doped graphene, or a combination thereof. Original
The process of claim 1, wherein said isolated graphene sheets are pre-deposited with a nanoscaled coating or particles of a redox pair partner selected from an intrinsically conductive polymer, a transition metal oxide, and/or an organic molecule, wherein said redox pair partner and said graphene sheets form a redox pair for pseudo-capacitance. Original
The process of claim 1, wherein said liquid electrolyte contains an aqueous electrolyte, an organic electrolyte, an ionic liquid electrolyte, or a mixture of an organic and an ionic electrolyte. The process of claim 1, wherein said forced assembly procedure is conducted in the presence of a current collector, which current collector is embedded in said electrolyte- impregnated laminar graphene structure or bonded to said electrolyte-impregnated laminar graphene structure to form said supercapacitor electrode. Original
The process of claim 1, wherein said forced assembly procedure includes introducing said graphene dispersion, having an initial volume V 1, in a mold cavity cell and driving a piston into said mold cavity cell to reduce the graphene dispersion volume to a smaller value V 2, allowing excess electrolyte to flow out of said cavity cell and aligning said multiple graphene sheets along a desired direction.. The process of claim 1, wherein said forced assembly procedure includes introducing said graphene dispersion in a mold cavity cell having an initial volume V 1, and applying a suction pressure through a porous wall of said mold cavity to reduce the graphene dispersion volume to a smaller value V 2, allowing excess electrolyte to flow out of said cavity cell through said porous wall and aligning said multiple graphene sheets along a desired direction.. The process of claim 1, wherein said forced assembly procedure includes introducing a first layer of said graphene dispersion onto a surface of a supporting conveyor and driving said layer of graphene suspension supported on said conveyor through at least a pair of pressing rollers to reduce a thickness of said graphene dispersion layer and align said multiple graphene sheets along a direction parallel to said conveyor surface for forming a layer of electrolyte-impregnated laminar graphene structure. Original
The process of claim 1, further including a step of compressing or roll-pressing said electrolyte-impregnated laminar structure to reduce a thin electrolyte layer thickness in said impregnated laminar structure, improve orientation of graphene sheets, and squeeze excess electrolyte out of said impregnated laminar graphene structure for forming said supercapacitor electrode. Original
The process of claim 1, further comprising a step of cutting said electrolyte- impregnated laminar graphene structure into multiple sheets and stacking said multiple sheets to form a supercapacitor electrode. Original
The process of claim 1, further comprising a step of attaching said electrolyte- impregnated laminar graphene structure to a current collector, wherein said graphene sheets are aligned parallel to a primary surface of said current collector. Original
The process of claim 1, further comprising a step of attaching said electrolyte- impregnated laminar graphene structure to a current collector, wherein said graphene sheets are aligned perpendicular to a primary surface of said current collector. Original
A process of producing a supercapacitor electrode, comprising stacking a current collector with at least a layer of said electrolyte-impregnated laminar graphene structure of claim 1 to form a multiple-layer structure and further comprising a step of compressing and consolidating said multi-layer structure to increase a physical density and decrease a thickness of said multi-layer structure to form said supercapacitor electrode. 17. The process of claim 16, wherein at least one layer of said electrolyte- impregnated laminar graphene structure is attached to one surface of said current collector and at least one layer of said electrolyte-impregnated laminar graphene structure is attached to the opposing surface of said current collector prior to said step of compressing and: onsolidating. Original
The process of claim 1, wherein said graphene dispersion contains a graphene oxide dispersion prepared by immersing a graphitic material in a powder or fibrous form in an oxidizing liquid in a reaction vessel at a reaction temperature for a length of time ufficient to obtain said graphene dispersion wherein said graphitic material is selected from iatural graphite, artificial graphite, mesophase carbon, mesophase pitch, mesocarbon micro-bead, soft carbon, hard carbon, coke, carbon fiber,: arbon nanofiber, carbon nanotube, or a combination thereof and wherein said graphene oxide has an oxygen content no less than 5% by weight. Currently amended
A supercapacitor comprising an anode, a cathode, an ion-permeable separator that lectronically separates said anode and said cathode, and an electrolyte in ionic contact with aid anode and said cathode, wherein the anode and/or the cathode contains the electrolyte-mpregnated laminar graphene structure of claim 1. Original
The process of claim 9, further including a step of introducing a second layer of said graphene dispersion onto a surface of said layer of electrolyte-impregnated laminar graphene structure to form a two layer laminar structure, and driving said two-layer laminar structure through at least a pair of pressing rollers to reduce a thickness of said second layer Original
The process of claim 9, which is a roll-to-roll process wherein said forced assembly procedure includes feeding said supporting conveyor, in a continuous film form, from a feeder roller to a deposition zone, continuously or intermittently depositing said graphene dispersion onto a surface of said supporting conveyor film to form said layer of graphene dispersion thereon, and collecting said layer of electrolyte-impregnated laminar graphene structure supported on conveyor film on a collector roller. Original
A supercapacitor comprising an anode current collector, an anode, a cathode, a cathode current collector, an ion-permeable separator that electronically separates said anode and said cathode, and an electrolyte in ionic contact with said anode and said cathode, wherein the anode and/or the cathode contains an electrolyte-impregnated laminar graphene structure, which is composed of multiple graphene sheets being alternately spaced by thin SVG 14998672.10-10-2017.J₈LT₆EDBRXEAPX1.CLM.5.6.375.558.469.615.svg 0.19 0.313 Chemistry Black and white SVG 14998672.10-10-2017.J₈LT₆EDBRXEAPX1.CLM.5.5.1137.472.1250.529.svg 0.19 0.377 Chemistry Black and white Original
The supercapacitor of claim 22, which is a lithium-ion capacitor or sodium-ion capacitor, wherein said cathode contains said electrolyte-impregnated laminar graphene structure and said anode contains a pre-lithiated anode active material or a pre-sodiated anode active material. Original
A supercapacitor electrode containing an electrolyte-impregnated laminar graphene structure, which is composed of multiple graphene sheets being alternately spaced by thin electrolyte layers, less than 10 nm in thickness, and said multiple graphene sheets are substantially aligned along a desired direction, and wherein said laminar graphene structure has a physical density from 0.5 to 1.7 g/cm 3 and a specific surface area from 50 to 3,300, when measured in a dried state of said laminar graphene structure with said electrolyte removed. SVG 14998672.10-10-2017.J₈LT₆EDBRXEAPX1.CLM.5.13.375.1187.469.1244.svg 0.19 0.313 Chemistry Black and white Original
Layer stacks claimed or described, ordered top of device to substrate.
supercapacitor electrode (electrolyte-impregnated laminar graphene structure)
supercapacitor
Materials described outside the worked examples.
graphene sheets
electrolyte
graphene oxide
reduced graphene oxide
graphene fluoride
graphene chloride
graphene bromide
graphene iodide
hydrogenated graphene
nitrogenated graphene
doped graphene
intrinsically conductive polymer
transition metal oxide
organic molecule
polyaniline
polypyrrole
polythiophene
polyfuran
sulfonated polyaniline
sulfonated polypyrrole
sulfonated polythiophene
sulfonated polyfuran
sulfonated polyacetylene
graphitic material
Measurements and analyses referenced in the patent, with their drawing references.
FIG. 1 (B) having a thickness > 100 nm. These flakes can be formed into graphite paper or mat 106 using a paper- or mat-making process. 15 This expanded …
FIG. 4. There are several significant observations that can be made from these data: (A) Given comparable electrode thickness, the(presently invented graphene …
FIG.5 Ragone plots (grav in etric and volumetric power density vs. energy density) of symmetric supercapacitor (EDLC) cells containing isolated nitrogen-doped …
FIG.9 for reduced graphene oxide-based EDLC supercapacitors. The cell-level gravimetric and volumetric energy densities plotted over the achievable electrode …
Performance values and ranges asserted in the specification or claims.
| Property | Value | Material |
|---|---|---|
Physical Density | 0.5–1.7 | graphene sheets |
Specific Surface Area | 50–3300 | graphene sheets |
Electrolyte Layer Thickness | 0.4–10 | electrolyte |
Gravimetric Specific Capacitance | 150–350 | graphene sheets |
Volumetric Specific Capacitance | 150–450 | graphene sheets |
Duration | 15–120 s | — |
Duration | 900–7200 s | — |
Thickness | 0.5–10 nm | — |
Thickness | 10–10000000 nm | — |
Duration | 0.5–96 hours | — |
Duration | 48–72 hours | — |
Duration | 5–16 hours | — |
Duration | 48–96 hours | — |
Duration | 10–100 minutes | — |
Thickness | ≤ 10 nm | — |
Thickness | ≤ 5 nm | — |
Thickness | ≤ 2 nm | — |
Thickness | ≥ 2 nm | — |
Thickness | ≥ 1 nm | — |
Thickness | 0.4–10 nm | — |
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Patent drawings and their descriptions. Click a drawing to enlarge it.
FIG. 1 (B) having a thickness > 100 nm. These flakes can be formed into graphite paper or mat 106 using a paper- or mat-making process. 15 This expanded …
FIG.2 Schematic of a conventional activated carbon-based supercapacitor cell.
FIG.3(A) Schematic drawing to illustrate an example of a compressing and consolidating operation (using a mold cavity cell equipped with a piston or ram) for …
FIG. 4. There are several significant observations that can be made from these data: (A) Given comparable electrode thickness, the(presently invented graphene …
FIG.5 Ragone plots (grav in etric and volumetric power density vs. energy density) of symmetric supercapacitor (EDLC) cells containing isolated nitrogen-doped …
FIG.6 shows the Ragone plots of two pristine graphene-based EDLC supercapacitors, one 5 having graphene sheets parallel to the current collector surface plane …
FIG.7 are the Ragone plots of two graphene-conductive polymer redox supercapacitors (pseudo-capacitors) having electrodes based on graphene/sulfonated …
FIG.8 Ragone plots of lithium ion capacitor (LIC) cells containing pristine graphene sheets as the electrode ac t ive material and lithium salt-PC/DEC organic …
FIG.9 for reduced graphene oxide-based EDLC supercapacitors. The cell-level gravimetric and volumetric energy densities plotted over the achievable electrode …
FIG. 10 The cell-level gravimetric energy densities plotted over the achievable active material proportion (active material weight/total cell weight) in a …
Claims define the patent's legal scope. Independent claims stand alone; dependent claims (nested) narrow them. Click a claim to expand its dependents.
A process for producing an electrolyte-impregnated laminar graphene structure for use as a supercapacitor electrode, said process comprising: (a) preparing a graphene dispersion having multiple isolated graphene sheets dispersed in a liquid or gel electrolyte; and (b) subjecting said graphene dispersion to a forced assembly procedure, forcing said multiple graphene sheets to assemble into said electrolyte-impregnated laminar graphene structure, wherein said multiple graphene sheets are alternately spaced by thin electrolyte layers, SVG 14998672.10-10-2017.J₈LT₆EDBRXEAPX1.CLM.1.17.1857.1554.1950.1611.svg 0.19 0.31 Chemistry Black and white having a thickness from 0.4 nm to 10 nm, and said multiple graphene sheets are substantially aligned along a desired direction, and wherein said laminar graphene structure has a physical density from 0.5 to 1.7 g/cm 3 and a specific surface area from 50 to 3,300, when measured in a dried state of said laminar structure with said electrolyte removed. Original
The process of claim 1, wherein said isolated graphene sheets are selected from a pristine graphene or a non-pristine graphene material, having a content of non-carbon elements greater than 2% by weight, selected from graphene oxide, reduced graphene oxide, graphene fluoride, graphene chloride, graphene bromide, graphene iodide, hydrogenated graphene, nitrogenated graphene, chemically functionalized graphene, doped graphene, or a combination thereof. Original
The process of claim 1, wherein said isolated graphene sheets are pre-deposited with a nanoscaled coating or particles of a redox pair partner selected from an intrinsically conductive polymer, a transition metal oxide, and/or an organic molecule, wherein said redox pair partner and said graphene sheets form a redox pair for pseudo-capacitance. Original
The process of claim 1, wherein said liquid electrolyte contains an aqueous electrolyte, an organic electrolyte, an ionic liquid electrolyte, or a mixture of an organic and an ionic electrolyte. The process of claim 1, wherein said forced assembly procedure is conducted in the presence of a current collector, which current collector is embedded in said electrolyte- impregnated laminar graphene structure or bonded to said electrolyte-impregnated laminar graphene structure to form said supercapacitor electrode. Original
The process of claim 1, wherein said forced assembly procedure includes introducing said graphene dispersion, having an initial volume V 1, in a mold cavity cell and driving a piston into said mold cavity cell to reduce the graphene dispersion volume to a smaller value V 2, allowing excess electrolyte to flow out of said cavity cell and aligning said multiple graphene sheets along a desired direction.. The process of claim 1, wherein said forced assembly procedure includes introducing said graphene dispersion in a mold cavity cell having an initial volume V 1, and applying a suction pressure through a porous wall of said mold cavity to reduce the graphene dispersion volume to a smaller value V 2, allowing excess electrolyte to flow out of said cavity cell through said porous wall and aligning said multiple graphene sheets along a desired direction.. The process of claim 1, wherein said forced assembly procedure includes introducing a first layer of said graphene dispersion onto a surface of a supporting conveyor and driving said layer of graphene suspension supported on said conveyor through at least a pair of pressing rollers to reduce a thickness of said graphene dispersion layer and align said multiple graphene sheets along a direction parallel to said conveyor surface for forming a layer of electrolyte-impregnated laminar graphene structure. Original
The process of claim 1, further including a step of compressing or roll-pressing said electrolyte-impregnated laminar structure to reduce a thin electrolyte layer thickness in said impregnated laminar structure, improve orientation of graphene sheets, and squeeze excess electrolyte out of said impregnated laminar graphene structure for forming said supercapacitor electrode. Original
The process of claim 1, further comprising a step of cutting said electrolyte- impregnated laminar graphene structure into multiple sheets and stacking said multiple sheets to form a supercapacitor electrode. Original
The process of claim 1, further comprising a step of attaching said electrolyte- impregnated laminar graphene structure to a current collector, wherein said graphene sheets are aligned parallel to a primary surface of said current collector. Original
The process of claim 1, further comprising a step of attaching said electrolyte- impregnated laminar graphene structure to a current collector, wherein said graphene sheets are aligned perpendicular to a primary surface of said current collector. Original
A process of producing a supercapacitor electrode, comprising stacking a current collector with at least a layer of said electrolyte-impregnated laminar graphene structure of claim 1 to form a multiple-layer structure and further comprising a step of compressing and consolidating said multi-layer structure to increase a physical density and decrease a thickness of said multi-layer structure to form said supercapacitor electrode. 17. The process of claim 16, wherein at least one layer of said electrolyte- impregnated laminar graphene structure is attached to one surface of said current collector and at least one layer of said electrolyte-impregnated laminar graphene structure is attached to the opposing surface of said current collector prior to said step of compressing and: onsolidating. Original
The process of claim 1, wherein said graphene dispersion contains a graphene oxide dispersion prepared by immersing a graphitic material in a powder or fibrous form in an oxidizing liquid in a reaction vessel at a reaction temperature for a length of time ufficient to obtain said graphene dispersion wherein said graphitic material is selected from iatural graphite, artificial graphite, mesophase carbon, mesophase pitch, mesocarbon micro-bead, soft carbon, hard carbon, coke, carbon fiber,: arbon nanofiber, carbon nanotube, or a combination thereof and wherein said graphene oxide has an oxygen content no less than 5% by weight. Currently amended
A supercapacitor comprising an anode, a cathode, an ion-permeable separator that lectronically separates said anode and said cathode, and an electrolyte in ionic contact with aid anode and said cathode, wherein the anode and/or the cathode contains the electrolyte-mpregnated laminar graphene structure of claim 1. Original
The process of claim 9, further including a step of introducing a second layer of said graphene dispersion onto a surface of said layer of electrolyte-impregnated laminar graphene structure to form a two layer laminar structure, and driving said two-layer laminar structure through at least a pair of pressing rollers to reduce a thickness of said second layer Original
The process of claim 9, which is a roll-to-roll process wherein said forced assembly procedure includes feeding said supporting conveyor, in a continuous film form, from a feeder roller to a deposition zone, continuously or intermittently depositing said graphene dispersion onto a surface of said supporting conveyor film to form said layer of graphene dispersion thereon, and collecting said layer of electrolyte-impregnated laminar graphene structure supported on conveyor film on a collector roller. Original
A supercapacitor comprising an anode current collector, an anode, a cathode, a cathode current collector, an ion-permeable separator that electronically separates said anode and said cathode, and an electrolyte in ionic contact with said anode and said cathode, wherein the anode and/or the cathode contains an electrolyte-impregnated laminar graphene structure, which is composed of multiple graphene sheets being alternately spaced by thin SVG 14998672.10-10-2017.J₈LT₆EDBRXEAPX1.CLM.5.6.375.558.469.615.svg 0.19 0.313 Chemistry Black and white SVG 14998672.10-10-2017.J₈LT₆EDBRXEAPX1.CLM.5.5.1137.472.1250.529.svg 0.19 0.377 Chemistry Black and white Original
The supercapacitor of claim 22, which is a lithium-ion capacitor or sodium-ion capacitor, wherein said cathode contains said electrolyte-impregnated laminar graphene structure and said anode contains a pre-lithiated anode active material or a pre-sodiated anode active material. Original
A supercapacitor electrode containing an electrolyte-impregnated laminar graphene structure, which is composed of multiple graphene sheets being alternately spaced by thin electrolyte layers, less than 10 nm in thickness, and said multiple graphene sheets are substantially aligned along a desired direction, and wherein said laminar graphene structure has a physical density from 0.5 to 1.7 g/cm 3 and a specific surface area from 50 to 3,300, when measured in a dried state of said laminar graphene structure with said electrolyte removed. SVG 14998672.10-10-2017.J₈LT₆EDBRXEAPX1.CLM.5.13.375.1187.469.1244.svg 0.19 0.313 Chemistry Black and white Original
Layer stacks claimed or described, ordered top of device to substrate.
supercapacitor electrode (electrolyte-impregnated laminar graphene structure)
supercapacitor
Materials described outside the worked examples.
graphene sheets
electrolyte
graphene oxide
reduced graphene oxide
graphene fluoride
graphene chloride
graphene bromide
graphene iodide
hydrogenated graphene
nitrogenated graphene
doped graphene
intrinsically conductive polymer
transition metal oxide
organic molecule
polyaniline
polypyrrole
polythiophene
polyfuran
sulfonated polyaniline
sulfonated polypyrrole
sulfonated polythiophene
sulfonated polyfuran
sulfonated polyacetylene
graphitic material
Measurements and analyses referenced in the patent, with their drawing references.
FIG. 1 (B) having a thickness > 100 nm. These flakes can be formed into graphite paper or mat 106 using a paper- or mat-making process. 15 This expanded …
FIG. 4. There are several significant observations that can be made from these data: (A) Given comparable electrode thickness, the(presently invented graphene …
FIG.5 Ragone plots (grav in etric and volumetric power density vs. energy density) of symmetric supercapacitor (EDLC) cells containing isolated nitrogen-doped …
FIG.9 for reduced graphene oxide-based EDLC supercapacitors. The cell-level gravimetric and volumetric energy densities plotted over the achievable electrode …
Performance values and ranges asserted in the specification or claims.
| Property | Value | Material |
|---|---|---|
Physical Density | 0.5–1.7 | graphene sheets |
Specific Surface Area | 50–3300 | graphene sheets |
Electrolyte Layer Thickness | 0.4–10 | electrolyte |
Gravimetric Specific Capacitance | 150–350 | graphene sheets |
Volumetric Specific Capacitance | 150–450 | graphene sheets |
Duration | 15–120 s | — |
Duration | 900–7200 s | — |
Thickness | 0.5–10 nm | — |
Thickness | 10–10000000 nm | — |
Duration | 0.5–96 hours | — |
Duration | 48–72 hours | — |
Duration | 5–16 hours | — |
Duration | 48–96 hours | — |
Duration | 10–100 minutes | — |
Thickness | ≤ 10 nm | — |
Thickness | ≤ 5 nm | — |
Thickness | ≤ 2 nm | — |
Thickness | ≥ 2 nm | — |
Thickness | ≥ 1 nm | — |
Thickness | 0.4–10 nm | — |
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Patent drawings and their descriptions. Click a drawing to enlarge it.
FIG. 1 (B) having a thickness > 100 nm. These flakes can be formed into graphite paper or mat 106 using a paper- or mat-making process. 15 This expanded …
FIG.2 Schematic of a conventional activated carbon-based supercapacitor cell.
FIG.3(A) Schematic drawing to illustrate an example of a compressing and consolidating operation (using a mold cavity cell equipped with a piston or ram) for …
FIG. 4. There are several significant observations that can be made from these data: (A) Given comparable electrode thickness, the(presently invented graphene …
FIG.5 Ragone plots (grav in etric and volumetric power density vs. energy density) of symmetric supercapacitor (EDLC) cells containing isolated nitrogen-doped …
FIG.6 shows the Ragone plots of two pristine graphene-based EDLC supercapacitors, one 5 having graphene sheets parallel to the current collector surface plane …
FIG.7 are the Ragone plots of two graphene-conductive polymer redox supercapacitors (pseudo-capacitors) having electrodes based on graphene/sulfonated …
FIG.8 Ragone plots of lithium ion capacitor (LIC) cells containing pristine graphene sheets as the electrode ac t ive material and lithium salt-PC/DEC organic …
FIG.9 for reduced graphene oxide-based EDLC supercapacitors. The cell-level gravimetric and volumetric energy densities plotted over the achievable electrode …
FIG. 10 The cell-level gravimetric energy densities plotted over the achievable active material proportion (active material weight/total cell weight) in a …
Claims define the patent's legal scope. Independent claims stand alone; dependent claims (nested) narrow them. Click a claim to expand its dependents.
A process for producing an electrolyte-impregnated laminar graphene structure for use as a supercapacitor electrode, said process comprising: (a) preparing a graphene dispersion having multiple isolated graphene sheets dispersed in a liquid or gel electrolyte; and (b) subjecting said graphene dispersion to a forced assembly procedure, forcing said multiple graphene sheets to assemble into said electrolyte-impregnated laminar graphene structure, wherein said multiple graphene sheets are alternately spaced by thin electrolyte layers, SVG 14998672.10-10-2017.J₈LT₆EDBRXEAPX1.CLM.1.17.1857.1554.1950.1611.svg 0.19 0.31 Chemistry Black and white having a thickness from 0.4 nm to 10 nm, and said multiple graphene sheets are substantially aligned along a desired direction, and wherein said laminar graphene structure has a physical density from 0.5 to 1.7 g/cm 3 and a specific surface area from 50 to 3,300, when measured in a dried state of said laminar structure with said electrolyte removed. Original
The process of claim 1, wherein said isolated graphene sheets are selected from a pristine graphene or a non-pristine graphene material, having a content of non-carbon elements greater than 2% by weight, selected from graphene oxide, reduced graphene oxide, graphene fluoride, graphene chloride, graphene bromide, graphene iodide, hydrogenated graphene, nitrogenated graphene, chemically functionalized graphene, doped graphene, or a combination thereof. Original
The process of claim 1, wherein said isolated graphene sheets are pre-deposited with a nanoscaled coating or particles of a redox pair partner selected from an intrinsically conductive polymer, a transition metal oxide, and/or an organic molecule, wherein said redox pair partner and said graphene sheets form a redox pair for pseudo-capacitance. Original
The process of claim 1, wherein said liquid electrolyte contains an aqueous electrolyte, an organic electrolyte, an ionic liquid electrolyte, or a mixture of an organic and an ionic electrolyte. The process of claim 1, wherein said forced assembly procedure is conducted in the presence of a current collector, which current collector is embedded in said electrolyte- impregnated laminar graphene structure or bonded to said electrolyte-impregnated laminar graphene structure to form said supercapacitor electrode. Original
The process of claim 1, wherein said forced assembly procedure includes introducing said graphene dispersion, having an initial volume V 1, in a mold cavity cell and driving a piston into said mold cavity cell to reduce the graphene dispersion volume to a smaller value V 2, allowing excess electrolyte to flow out of said cavity cell and aligning said multiple graphene sheets along a desired direction.. The process of claim 1, wherein said forced assembly procedure includes introducing said graphene dispersion in a mold cavity cell having an initial volume V 1, and applying a suction pressure through a porous wall of said mold cavity to reduce the graphene dispersion volume to a smaller value V 2, allowing excess electrolyte to flow out of said cavity cell through said porous wall and aligning said multiple graphene sheets along a desired direction.. The process of claim 1, wherein said forced assembly procedure includes introducing a first layer of said graphene dispersion onto a surface of a supporting conveyor and driving said layer of graphene suspension supported on said conveyor through at least a pair of pressing rollers to reduce a thickness of said graphene dispersion layer and align said multiple graphene sheets along a direction parallel to said conveyor surface for forming a layer of electrolyte-impregnated laminar graphene structure. Original
The process of claim 1, further including a step of compressing or roll-pressing said electrolyte-impregnated laminar structure to reduce a thin electrolyte layer thickness in said impregnated laminar structure, improve orientation of graphene sheets, and squeeze excess electrolyte out of said impregnated laminar graphene structure for forming said supercapacitor electrode. Original
The process of claim 1, further comprising a step of cutting said electrolyte- impregnated laminar graphene structure into multiple sheets and stacking said multiple sheets to form a supercapacitor electrode. Original
The process of claim 1, further comprising a step of attaching said electrolyte- impregnated laminar graphene structure to a current collector, wherein said graphene sheets are aligned parallel to a primary surface of said current collector. Original
The process of claim 1, further comprising a step of attaching said electrolyte- impregnated laminar graphene structure to a current collector, wherein said graphene sheets are aligned perpendicular to a primary surface of said current collector. Original
A process of producing a supercapacitor electrode, comprising stacking a current collector with at least a layer of said electrolyte-impregnated laminar graphene structure of claim 1 to form a multiple-layer structure and further comprising a step of compressing and consolidating said multi-layer structure to increase a physical density and decrease a thickness of said multi-layer structure to form said supercapacitor electrode. 17. The process of claim 16, wherein at least one layer of said electrolyte- impregnated laminar graphene structure is attached to one surface of said current collector and at least one layer of said electrolyte-impregnated laminar graphene structure is attached to the opposing surface of said current collector prior to said step of compressing and: onsolidating. Original
The process of claim 1, wherein said graphene dispersion contains a graphene oxide dispersion prepared by immersing a graphitic material in a powder or fibrous form in an oxidizing liquid in a reaction vessel at a reaction temperature for a length of time ufficient to obtain said graphene dispersion wherein said graphitic material is selected from iatural graphite, artificial graphite, mesophase carbon, mesophase pitch, mesocarbon micro-bead, soft carbon, hard carbon, coke, carbon fiber,: arbon nanofiber, carbon nanotube, or a combination thereof and wherein said graphene oxide has an oxygen content no less than 5% by weight. Currently amended
A supercapacitor comprising an anode, a cathode, an ion-permeable separator that lectronically separates said anode and said cathode, and an electrolyte in ionic contact with aid anode and said cathode, wherein the anode and/or the cathode contains the electrolyte-mpregnated laminar graphene structure of claim 1. Original
The process of claim 9, further including a step of introducing a second layer of said graphene dispersion onto a surface of said layer of electrolyte-impregnated laminar graphene structure to form a two layer laminar structure, and driving said two-layer laminar structure through at least a pair of pressing rollers to reduce a thickness of said second layer Original
The process of claim 9, which is a roll-to-roll process wherein said forced assembly procedure includes feeding said supporting conveyor, in a continuous film form, from a feeder roller to a deposition zone, continuously or intermittently depositing said graphene dispersion onto a surface of said supporting conveyor film to form said layer of graphene dispersion thereon, and collecting said layer of electrolyte-impregnated laminar graphene structure supported on conveyor film on a collector roller. Original
A supercapacitor comprising an anode current collector, an anode, a cathode, a cathode current collector, an ion-permeable separator that electronically separates said anode and said cathode, and an electrolyte in ionic contact with said anode and said cathode, wherein the anode and/or the cathode contains an electrolyte-impregnated laminar graphene structure, which is composed of multiple graphene sheets being alternately spaced by thin SVG 14998672.10-10-2017.J₈LT₆EDBRXEAPX1.CLM.5.6.375.558.469.615.svg 0.19 0.313 Chemistry Black and white SVG 14998672.10-10-2017.J₈LT₆EDBRXEAPX1.CLM.5.5.1137.472.1250.529.svg 0.19 0.377 Chemistry Black and white Original
The supercapacitor of claim 22, which is a lithium-ion capacitor or sodium-ion capacitor, wherein said cathode contains said electrolyte-impregnated laminar graphene structure and said anode contains a pre-lithiated anode active material or a pre-sodiated anode active material. Original
A supercapacitor electrode containing an electrolyte-impregnated laminar graphene structure, which is composed of multiple graphene sheets being alternately spaced by thin electrolyte layers, less than 10 nm in thickness, and said multiple graphene sheets are substantially aligned along a desired direction, and wherein said laminar graphene structure has a physical density from 0.5 to 1.7 g/cm 3 and a specific surface area from 50 to 3,300, when measured in a dried state of said laminar graphene structure with said electrolyte removed. SVG 14998672.10-10-2017.J₈LT₆EDBRXEAPX1.CLM.5.13.375.1187.469.1244.svg 0.19 0.313 Chemistry Black and white Original
Layer stacks claimed or described, ordered top of device to substrate.
supercapacitor electrode (electrolyte-impregnated laminar graphene structure)
supercapacitor
Materials described outside the worked examples.
graphene sheets
electrolyte
graphene oxide
reduced graphene oxide
graphene fluoride
graphene chloride
graphene bromide
graphene iodide
hydrogenated graphene
nitrogenated graphene
doped graphene
intrinsically conductive polymer
transition metal oxide
organic molecule
polyaniline
polypyrrole
polythiophene
polyfuran
sulfonated polyaniline
sulfonated polypyrrole
sulfonated polythiophene
sulfonated polyfuran
sulfonated polyacetylene
graphitic material
Measurements and analyses referenced in the patent, with their drawing references.
FIG. 1 (B) having a thickness > 100 nm. These flakes can be formed into graphite paper or mat 106 using a paper- or mat-making process. 15 This expanded …
FIG. 4. There are several significant observations that can be made from these data: (A) Given comparable electrode thickness, the(presently invented graphene …
FIG.5 Ragone plots (grav in etric and volumetric power density vs. energy density) of symmetric supercapacitor (EDLC) cells containing isolated nitrogen-doped …
FIG.9 for reduced graphene oxide-based EDLC supercapacitors. The cell-level gravimetric and volumetric energy densities plotted over the achievable electrode …
Performance values and ranges asserted in the specification or claims.
| Property | Value | Material |
|---|---|---|
Physical Density | 0.5–1.7 | graphene sheets |
Specific Surface Area | 50–3300 | graphene sheets |
Electrolyte Layer Thickness | 0.4–10 | electrolyte |
Gravimetric Specific Capacitance | 150–350 | graphene sheets |
Volumetric Specific Capacitance | 150–450 | graphene sheets |
Duration | 15–120 s | — |
Duration | 900–7200 s | — |
Thickness | 0.5–10 nm | — |
Thickness | 10–10000000 nm | — |
Duration | 0.5–96 hours | — |
Duration | 48–72 hours | — |
Duration | 5–16 hours | — |
Duration | 48–96 hours | — |
Duration | 10–100 minutes | — |
Thickness | ≤ 10 nm | — |
Thickness | ≤ 5 nm | — |
Thickness | ≤ 2 nm | — |
Thickness | ≥ 2 nm | — |
Thickness | ≥ 1 nm | — |
Thickness | 0.4–10 nm | — |
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Patent drawings and their descriptions. Click a drawing to enlarge it.
FIG. 1 (B) having a thickness > 100 nm. These flakes can be formed into graphite paper or mat 106 using a paper- or mat-making process. 15 This expanded …
FIG.2 Schematic of a conventional activated carbon-based supercapacitor cell.
FIG.3(A) Schematic drawing to illustrate an example of a compressing and consolidating operation (using a mold cavity cell equipped with a piston or ram) for …
FIG. 4. There are several significant observations that can be made from these data: (A) Given comparable electrode thickness, the(presently invented graphene …
FIG.5 Ragone plots (grav in etric and volumetric power density vs. energy density) of symmetric supercapacitor (EDLC) cells containing isolated nitrogen-doped …
FIG.6 shows the Ragone plots of two pristine graphene-based EDLC supercapacitors, one 5 having graphene sheets parallel to the current collector surface plane …
FIG.7 are the Ragone plots of two graphene-conductive polymer redox supercapacitors (pseudo-capacitors) having electrodes based on graphene/sulfonated …
FIG.8 Ragone plots of lithium ion capacitor (LIC) cells containing pristine graphene sheets as the electrode ac t ive material and lithium salt-PC/DEC organic …
FIG.9 for reduced graphene oxide-based EDLC supercapacitors. The cell-level gravimetric and volumetric energy densities plotted over the achievable electrode …
FIG. 10 The cell-level gravimetric energy densities plotted over the achievable active material proportion (active material weight/total cell weight) in a …
Claims define the patent's legal scope. Independent claims stand alone; dependent claims (nested) narrow them. Click a claim to expand its dependents.
A process for producing an electrolyte-impregnated laminar graphene structure for use as a supercapacitor electrode, said process comprising: (a) preparing a graphene dispersion having multiple isolated graphene sheets dispersed in a liquid or gel electrolyte; and (b) subjecting said graphene dispersion to a forced assembly procedure, forcing said multiple graphene sheets to assemble into said electrolyte-impregnated laminar graphene structure, wherein said multiple graphene sheets are alternately spaced by thin electrolyte layers, SVG 14998672.10-10-2017.J₈LT₆EDBRXEAPX1.CLM.1.17.1857.1554.1950.1611.svg 0.19 0.31 Chemistry Black and white having a thickness from 0.4 nm to 10 nm, and said multiple graphene sheets are substantially aligned along a desired direction, and wherein said laminar graphene structure has a physical density from 0.5 to 1.7 g/cm 3 and a specific surface area from 50 to 3,300, when measured in a dried state of said laminar structure with said electrolyte removed. Original
The process of claim 1, wherein said isolated graphene sheets are selected from a pristine graphene or a non-pristine graphene material, having a content of non-carbon elements greater than 2% by weight, selected from graphene oxide, reduced graphene oxide, graphene fluoride, graphene chloride, graphene bromide, graphene iodide, hydrogenated graphene, nitrogenated graphene, chemically functionalized graphene, doped graphene, or a combination thereof. Original
The process of claim 1, wherein said isolated graphene sheets are pre-deposited with a nanoscaled coating or particles of a redox pair partner selected from an intrinsically conductive polymer, a transition metal oxide, and/or an organic molecule, wherein said redox pair partner and said graphene sheets form a redox pair for pseudo-capacitance. Original
The process of claim 1, wherein said liquid electrolyte contains an aqueous electrolyte, an organic electrolyte, an ionic liquid electrolyte, or a mixture of an organic and an ionic electrolyte. The process of claim 1, wherein said forced assembly procedure is conducted in the presence of a current collector, which current collector is embedded in said electrolyte- impregnated laminar graphene structure or bonded to said electrolyte-impregnated laminar graphene structure to form said supercapacitor electrode. Original
The process of claim 1, wherein said forced assembly procedure includes introducing said graphene dispersion, having an initial volume V 1, in a mold cavity cell and driving a piston into said mold cavity cell to reduce the graphene dispersion volume to a smaller value V 2, allowing excess electrolyte to flow out of said cavity cell and aligning said multiple graphene sheets along a desired direction.. The process of claim 1, wherein said forced assembly procedure includes introducing said graphene dispersion in a mold cavity cell having an initial volume V 1, and applying a suction pressure through a porous wall of said mold cavity to reduce the graphene dispersion volume to a smaller value V 2, allowing excess electrolyte to flow out of said cavity cell through said porous wall and aligning said multiple graphene sheets along a desired direction.. The process of claim 1, wherein said forced assembly procedure includes introducing a first layer of said graphene dispersion onto a surface of a supporting conveyor and driving said layer of graphene suspension supported on said conveyor through at least a pair of pressing rollers to reduce a thickness of said graphene dispersion layer and align said multiple graphene sheets along a direction parallel to said conveyor surface for forming a layer of electrolyte-impregnated laminar graphene structure. Original
The process of claim 1, further including a step of compressing or roll-pressing said electrolyte-impregnated laminar structure to reduce a thin electrolyte layer thickness in said impregnated laminar structure, improve orientation of graphene sheets, and squeeze excess electrolyte out of said impregnated laminar graphene structure for forming said supercapacitor electrode. Original
The process of claim 1, further comprising a step of cutting said electrolyte- impregnated laminar graphene structure into multiple sheets and stacking said multiple sheets to form a supercapacitor electrode. Original
The process of claim 1, further comprising a step of attaching said electrolyte- impregnated laminar graphene structure to a current collector, wherein said graphene sheets are aligned parallel to a primary surface of said current collector. Original
The process of claim 1, further comprising a step of attaching said electrolyte- impregnated laminar graphene structure to a current collector, wherein said graphene sheets are aligned perpendicular to a primary surface of said current collector. Original
A process of producing a supercapacitor electrode, comprising stacking a current collector with at least a layer of said electrolyte-impregnated laminar graphene structure of claim 1 to form a multiple-layer structure and further comprising a step of compressing and consolidating said multi-layer structure to increase a physical density and decrease a thickness of said multi-layer structure to form said supercapacitor electrode. 17. The process of claim 16, wherein at least one layer of said electrolyte- impregnated laminar graphene structure is attached to one surface of said current collector and at least one layer of said electrolyte-impregnated laminar graphene structure is attached to the opposing surface of said current collector prior to said step of compressing and: onsolidating. Original
The process of claim 1, wherein said graphene dispersion contains a graphene oxide dispersion prepared by immersing a graphitic material in a powder or fibrous form in an oxidizing liquid in a reaction vessel at a reaction temperature for a length of time ufficient to obtain said graphene dispersion wherein said graphitic material is selected from iatural graphite, artificial graphite, mesophase carbon, mesophase pitch, mesocarbon micro-bead, soft carbon, hard carbon, coke, carbon fiber,: arbon nanofiber, carbon nanotube, or a combination thereof and wherein said graphene oxide has an oxygen content no less than 5% by weight. Currently amended
A supercapacitor comprising an anode, a cathode, an ion-permeable separator that lectronically separates said anode and said cathode, and an electrolyte in ionic contact with aid anode and said cathode, wherein the anode and/or the cathode contains the electrolyte-mpregnated laminar graphene structure of claim 1. Original
The process of claim 9, further including a step of introducing a second layer of said graphene dispersion onto a surface of said layer of electrolyte-impregnated laminar graphene structure to form a two layer laminar structure, and driving said two-layer laminar structure through at least a pair of pressing rollers to reduce a thickness of said second layer Original
The process of claim 9, which is a roll-to-roll process wherein said forced assembly procedure includes feeding said supporting conveyor, in a continuous film form, from a feeder roller to a deposition zone, continuously or intermittently depositing said graphene dispersion onto a surface of said supporting conveyor film to form said layer of graphene dispersion thereon, and collecting said layer of electrolyte-impregnated laminar graphene structure supported on conveyor film on a collector roller. Original
A supercapacitor comprising an anode current collector, an anode, a cathode, a cathode current collector, an ion-permeable separator that electronically separates said anode and said cathode, and an electrolyte in ionic contact with said anode and said cathode, wherein the anode and/or the cathode contains an electrolyte-impregnated laminar graphene structure, which is composed of multiple graphene sheets being alternately spaced by thin SVG 14998672.10-10-2017.J₈LT₆EDBRXEAPX1.CLM.5.6.375.558.469.615.svg 0.19 0.313 Chemistry Black and white SVG 14998672.10-10-2017.J₈LT₆EDBRXEAPX1.CLM.5.5.1137.472.1250.529.svg 0.19 0.377 Chemistry Black and white Original
The supercapacitor of claim 22, which is a lithium-ion capacitor or sodium-ion capacitor, wherein said cathode contains said electrolyte-impregnated laminar graphene structure and said anode contains a pre-lithiated anode active material or a pre-sodiated anode active material. Original
A supercapacitor electrode containing an electrolyte-impregnated laminar graphene structure, which is composed of multiple graphene sheets being alternately spaced by thin electrolyte layers, less than 10 nm in thickness, and said multiple graphene sheets are substantially aligned along a desired direction, and wherein said laminar graphene structure has a physical density from 0.5 to 1.7 g/cm 3 and a specific surface area from 50 to 3,300, when measured in a dried state of said laminar graphene structure with said electrolyte removed. SVG 14998672.10-10-2017.J₈LT₆EDBRXEAPX1.CLM.5.13.375.1187.469.1244.svg 0.19 0.313 Chemistry Black and white Original
Layer stacks claimed or described, ordered top of device to substrate.
supercapacitor electrode (electrolyte-impregnated laminar graphene structure)
supercapacitor
Materials described outside the worked examples.
graphene sheets
electrolyte
graphene oxide
reduced graphene oxide
graphene fluoride
graphene chloride
graphene bromide
graphene iodide
hydrogenated graphene
nitrogenated graphene
doped graphene
intrinsically conductive polymer
transition metal oxide
organic molecule
polyaniline
polypyrrole
polythiophene
polyfuran
sulfonated polyaniline
sulfonated polypyrrole
sulfonated polythiophene
sulfonated polyfuran
sulfonated polyacetylene
graphitic material
Measurements and analyses referenced in the patent, with their drawing references.
FIG. 1 (B) having a thickness > 100 nm. These flakes can be formed into graphite paper or mat 106 using a paper- or mat-making process. 15 This expanded …
FIG. 4. There are several significant observations that can be made from these data: (A) Given comparable electrode thickness, the(presently invented graphene …
FIG.5 Ragone plots (grav in etric and volumetric power density vs. energy density) of symmetric supercapacitor (EDLC) cells containing isolated nitrogen-doped …
FIG.9 for reduced graphene oxide-based EDLC supercapacitors. The cell-level gravimetric and volumetric energy densities plotted over the achievable electrode …
Performance values and ranges asserted in the specification or claims.
| Property | Value | Material |
|---|---|---|
Physical Density | 0.5–1.7 | graphene sheets |
Specific Surface Area | 50–3300 | graphene sheets |
Electrolyte Layer Thickness | 0.4–10 | electrolyte |
Gravimetric Specific Capacitance | 150–350 | graphene sheets |
Volumetric Specific Capacitance | 150–450 | graphene sheets |
Duration | 15–120 s | — |
Duration | 900–7200 s | — |
Thickness | 0.5–10 nm | — |
Thickness | 10–10000000 nm | — |
Duration | 0.5–96 hours | — |
Duration | 48–72 hours | — |
Duration | 5–16 hours | — |
Duration | 48–96 hours | — |
Duration | 10–100 minutes | — |
Thickness | ≤ 10 nm | — |
Thickness | ≤ 5 nm | — |
Thickness | ≤ 2 nm | — |
Thickness | ≥ 2 nm | — |
Thickness | ≥ 1 nm | — |
Thickness | 0.4–10 nm | — |
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