METHOD FOR PREPARATION OF GRAPHENE USING SPONTANEOUS PROCESS | Matter42 Literature
Patent
Atlas literature
Patent
US 9,644,275
METHOD FOR PREPARATION OF GRAPHENE USING SPONTANEOUS PROCESS
Chong Min KOO
US
Drawings
Patent drawings and their descriptions. Click a drawing to enlarge it.
FIG. 1
process chamber schematic
FIG. 1 0 a is an atomic force microscope (AFM) of the graphene prepared through Example 1 of the present invention.
FIG. 2
process chamber schematic
FIG. 2 is a schematic view illustrating a process of immersing graphite surrounded with a lithium foil prepared by the method of
FIG. 3
process chamber schematic
FIG. 3 is a schematic view representing a method of obtaining graphene by separating the graphite intercalation compound formed by the method of
FIG. 4
process chamber schematic
FIG. 4 is a schematic view illustrating a process in which the graphite intercalation compound is formed from graphite.
FIG. 5
process chamber schematic
FIG. 5 is a schematic view representing a phenomenon in which lithium and the electrolyte are co-intercalated into the interlayer region of graphite by 20 s …
FIG. 6
FIG. 6 is a small-angle X-ray scattering (SAXS) peak illustrating that l ithium is intercalated into the interlayer region of graphite in Example 1 of the …
FIG. 7
FIG. 7 is an electron diffraction pattern of the graphene prepared through 25 Example 1 of the present invention. 19
FIG. 8
FIG. 8 is a Raman spectroscopy result of the graphene prepared through Example 1 of the present invention and graphite which is the material thereof.
FIG. 9
FIG. 9 is a high-magnification transmission electron microscope (TEM) of the graphene prepared through Example 1 of the present invention. 5
FIG. 10
performance graph
FIG. 10 b is a graph showing a height of a graphene sheet prepared through Example 1 of the present invention.
Claims
Claims define the patent's legal scope. Independent claims stand alone; dependent claims (nested) narrow them. Click a claim to expand its dependents.
The method of claim 1 8, wherein the di s per sive solv ent i s selected from the group c onsis ting of N- methyl -2- pyrr o lidone (NMP), dimethylform a mide (DM F), imethyl a cet a mide (DMA c), dimethyl s ulf ox ide (DM₈₀), a nd the c om bin ations thereof.
2
IndependentLiCsecond metal (Cu, Ag, Au, Pt)CuAgAu
Thmethodof-taimrwherein step-(4) further omprises A ethod for preparing grahene sin spontaneous process, the method comprising: (1) disposing lithium metal in surface contact with graphite and disposing a second metal in surface contact with the graphite, the second metal is selected from the group consisting of copper (Cu), silver (Ag), gold (Au), platinum (Pt), and the combinations thereof, and the lithium metal and the second metal are in surface contact with each other while the graphite is interposed therebetween; (2)immersin the surface contacted lithiu r rnetal and qraphite in an electrolyte for a lithium ion batter to form a ra hite intercalation com ound; and (3) introducing the graphite intercalation compound into water or alcohol to form graphene while generating hydrogen gas.
4
Dependent← claim 2LiCsecond metal (Cu, Ag, Au, Pt)
(o riginal) The meth o d of claim 2, w herein step (2) is accelerated b y virtue of an increased p o tential difference caused due to a fi x ed surface c o ntact between the lithium metal and the sec o nd metal, wherein the graphite is interp o sed therebet w een.
6
Dependent← claim 2second metal (Cu, Ag, Au, Pt)
(o riginal) The meth o d of claim 2, w herein the sec o nd metal is in a form of a foil.
13
Dependent← claim 2LiCsecond metal (Cu, Ag, Au, Pt)
(o rigi n al) The m eth o d of claim 2, w herei n step (1) co mpri ses co mpre ss ing a s tru c ture f o rmed by pla cin g a seco nd metal f o il o n the lithium f o il on whic h graphite is applied, o r r o lli n g the s tru c ture i nto a r oun d shape o r be ndin g the s tru c ture so as to f orm an angle. Page 4 of 8 Application Serial No. 14/470,083 PATENT Reply to office action of Docket: CU-71513
3
IndependentLiC
The method of claim [[1]] 2, wherein step (2) is spontaneously performed by virtue of a potential difference due to a fixed surface contact between the lithium metal and the graphite. Page 2 of 8 Application Serial No. 14/470,083 PATENT Reply to office action of Docket: CU-71513
5
IndependentLi
(curren tly am ende d) The meth o d of claim [[1]] 2, wherein the lithium metal is in a form of a foil.
7
IndependentLixCy (0 < x ≤ 1, y = 6)
(curren tly a mended) The meth o d of claim [[1]] 2, wherein the graphite intercalation compound is LixC y, where 0 < x 1 and y = 6.
8
IndependentC
(c urre nt ly a men ded) The meth o d of claim [[1]] 2, wherein the graphite is selected from the group consisting of artificial graphite, natural graphite, and the combinations thereof.
9
IndependentC
(c urre nt ly a men ded) The meth o d of claim [[1]] 2, wherein the graphite is selected fr o m the gr o up consisting of a pow der f o rm, a granule f o rm, a rod f o rm, a fiber fo rm graphite, and the co m binations thereof.
10
Independentelectrolyte for lithium ion battery
(currently amended) The meth o d of claim [[1]] 2, wherein Page 3 of 8 Application Serial No. 14/470,083 PATENT Reply to office action of Docket: CU-71513 the ele ctro lyte f or a lithium i on battery i s s ele c ted fr o m the g ro up consistin g of an ethyle ne c arb on ate so luti on in which a lithiu m salt i s di ssolv ed, a dimethyl c arb o nate so luti o n i n which a lithi um salt i s dis solv ed, a diethyl c arb on ate so luti on in which a lithium salt i s di ssolv ed, an ethyl methyl c arb on ate so luti o n in which a lithium salt i s dissolv ed, a pr o pyle ne c arb on ate so luti on in which a lithium salt i s di sso lved, and the co mbi n ati ons there o f, and the lithium s alt i s s ele c ted from the g ro up c onsistin g of Li PF6, Li ClO4, Li CF₃SO3, LiBF4, Li AsF6, Li C₂F₆NO₄S2, Li B(C₂₀₄)2, Li H₂PO4, LiA lCl4, Li GaCl4, an d the co mbi n ati ons there of.
11
Independentelectrolyte for lithium ion battery
(o riginal) The m eth o d of c laim 10, w herei n the ele ctro lyte f o r a lithium i on battery further com pri ses one s ele c ted from the gr o up consistin g of methyl acetate (MA), methyl pr opion ate (MP), ethyl acetate (EA), ethyl pr opion ate (EP), a n d the co mbi n ati ons there of.
12
IndependentLiC
(c u rre n tly amen ded) The m eth o d of claim [[1]] 2, w herei n step (1) com pri s es applying graphite on a lithium f o il to com pre ss the lithium f o il o r to r ol l the lithium fo il i nto a roun d shape o r to be n d the lithi um fo il s o as to f orm an angle.
14
Independent
(c urren tly amen ded) The method of claim [[1]] 2, wherein step (2) is performed for 1 minute to 48 hours.
15
Independent
(currently amende d) The method of claim [[1]] 2, wherein step (3) is performed for 1 second to 12 hours.
16
Independentgraphene
(c urr en tly a mended) The method of clai m [[1]] 2, wherein step (3) further comprises filtering and washing the graphene formed, and the filtering is performed by using a centrifuge or a vacuum filter.
17
Dependent← claim 16
17. (o rigin al) The method of claim 16, wherein the va cuum filter ha s a po re size f 0. 0 1 t o 0.1 um.
18. (cu rre n tly amended) The method of claim [[1]] 2, further comprising: (4) di s per s ing the gr a phene f o rmed in step (3) into a di s per sive so lvent; and (5) drying the di s per s ed gr a phene to f o rm graphene powder.
20
IndependentLiCsecond metal (Cu, Ag, Au, Pt)grapheneelectrolyte for lithium ion battery
A m eth od for p rep arin g gr a phe ne using a sp ontaneous Page 5 of 8 Application Serial No. 14/470,083 PATENT Reply to office action of Docket: CU-71513 process, the m eth od com pri sing: (1) di sposin g lithi um metal i n surface contact w ith graphite an d disp os ing a seco nd m etal i n su rfa ce contact w ith the graphite, the secon d metal i s selected fr om the gr o up consisting of co pper (Cu), silv er (Ag), g o ld (Au), platin um (P t), a n d the com binati ons thereof, a nd the lithi um m etal a n d the second m etal are i n su rfa c e c ontact w ith each o ther while the graphite i s in terp os ed therebet ween; (2) i mmersing the su rfa ce contac ted lithi um metal a n d graphite i n an ele ctro lyte f or a lithi um ion battery t o form a graphite i n ter c alati on compound; and (3) introducin g the graphite i n ter c ala tion compoun d i nto w ater o r al coho l t o form graphene while ge n erati n g hydr ogen ga s, w herein step (2) is a cc elera t ed by v irt ue o f a n inc rea s ed p oten tia l differe nce caus ed d u e t o a fi x ed su rfa ce contact between the lithi um m etal a nd the secon d metal, w herei n the graphi t e is i n terp os ed therebet w een. Page 6 of 8
Materials
Materials described outside the worked examples.
lithium metal
Li
Intercalant/Reductant For Graphite Intercalation
graphite
C
Starting Material/Graphene Precursor
Process steps
Additional fabrication and treatment steps described in the patent.
1
Spontaneous Electrochemical Intercalation And Exfoliation
Step 1
Process details
step 1:Dispose lithium metal foil in surface contact with graphite; optionally dispose a second metal (Cu, Ag, Au, or Pt) in surface contact with graphite so that lithium and second metal contact each other with graphite interposed
step 2:Immerse surface-contacted lithium metal and graphite in lithium-ion battery electrolyte to form graphite intercalation compound (LixCy, 0<x≤1, y=6); spontaneously driven by potential difference; accelerated by galvanic couple with second metal; duration 1 min to 48 h
step 3:Introduce graphite intercalation compound into water or alcohol to form graphene while generating hydrogen gas; duration 1 s to 12 h; optionally filter (centrifuge or vacuum filter, pore size 0.01–0.1 μm) and wash
Characterization
Measurements and analyses referenced in the patent, with their drawing references.
afm
AFM
FIG. 1 0 a is an atomic force microscope (AFM) of the graphene prepared through Example 1 of the present invention.
METHOD FOR PREPARATION OF GRAPHENE USING SPONTANEOUS PROCESS
Chong Min KOO
US
Drawings
Patent drawings and their descriptions. Click a drawing to enlarge it.
FIG. 1
process chamber schematic
FIG. 1 0 a is an atomic force microscope (AFM) of the graphene prepared through Example 1 of the present invention.
FIG. 2
process chamber schematic
FIG. 2 is a schematic view illustrating a process of immersing graphite surrounded with a lithium foil prepared by the method of
FIG. 3
process chamber schematic
FIG. 3 is a schematic view representing a method of obtaining graphene by separating the graphite intercalation compound formed by the method of
FIG. 4
process chamber schematic
FIG. 4 is a schematic view illustrating a process in which the graphite intercalation compound is formed from graphite.
FIG. 5
process chamber schematic
FIG. 5 is a schematic view representing a phenomenon in which lithium and the electrolyte are co-intercalated into the interlayer region of graphite by 20 s …
FIG. 6
FIG. 6 is a small-angle X-ray scattering (SAXS) peak illustrating that l ithium is intercalated into the interlayer region of graphite in Example 1 of the …
FIG. 7
FIG. 7 is an electron diffraction pattern of the graphene prepared through 25 Example 1 of the present invention. 19
FIG. 8
FIG. 8 is a Raman spectroscopy result of the graphene prepared through Example 1 of the present invention and graphite which is the material thereof.
FIG. 9
FIG. 9 is a high-magnification transmission electron microscope (TEM) of the graphene prepared through Example 1 of the present invention. 5
FIG. 10
performance graph
FIG. 10 b is a graph showing a height of a graphene sheet prepared through Example 1 of the present invention.
Claims
Claims define the patent's legal scope. Independent claims stand alone; dependent claims (nested) narrow them. Click a claim to expand its dependents.
The method of claim 1 8, wherein the di s per sive solv ent i s selected from the group c onsis ting of N- methyl -2- pyrr o lidone (NMP), dimethylform a mide (DM F), imethyl a cet a mide (DMA c), dimethyl s ulf ox ide (DM₈₀), a nd the c om bin ations thereof.
2
IndependentLiCsecond metal (Cu, Ag, Au, Pt)CuAgAu
Thmethodof-taimrwherein step-(4) further omprises A ethod for preparing grahene sin spontaneous process, the method comprising: (1) disposing lithium metal in surface contact with graphite and disposing a second metal in surface contact with the graphite, the second metal is selected from the group consisting of copper (Cu), silver (Ag), gold (Au), platinum (Pt), and the combinations thereof, and the lithium metal and the second metal are in surface contact with each other while the graphite is interposed therebetween; (2)immersin the surface contacted lithiu r rnetal and qraphite in an electrolyte for a lithium ion batter to form a ra hite intercalation com ound; and (3) introducing the graphite intercalation compound into water or alcohol to form graphene while generating hydrogen gas.
4
Dependent← claim 2LiCsecond metal (Cu, Ag, Au, Pt)
(o riginal) The meth o d of claim 2, w herein step (2) is accelerated b y virtue of an increased p o tential difference caused due to a fi x ed surface c o ntact between the lithium metal and the sec o nd metal, wherein the graphite is interp o sed therebet w een.
6
Dependent← claim 2second metal (Cu, Ag, Au, Pt)
(o riginal) The meth o d of claim 2, w herein the sec o nd metal is in a form of a foil.
13
Dependent← claim 2LiCsecond metal (Cu, Ag, Au, Pt)
(o rigi n al) The m eth o d of claim 2, w herei n step (1) co mpri ses co mpre ss ing a s tru c ture f o rmed by pla cin g a seco nd metal f o il o n the lithium f o il on whic h graphite is applied, o r r o lli n g the s tru c ture i nto a r oun d shape o r be ndin g the s tru c ture so as to f orm an angle. Page 4 of 8 Application Serial No. 14/470,083 PATENT Reply to office action of Docket: CU-71513
3
IndependentLiC
The method of claim [[1]] 2, wherein step (2) is spontaneously performed by virtue of a potential difference due to a fixed surface contact between the lithium metal and the graphite. Page 2 of 8 Application Serial No. 14/470,083 PATENT Reply to office action of Docket: CU-71513
5
IndependentLi
(curren tly am ende d) The meth o d of claim [[1]] 2, wherein the lithium metal is in a form of a foil.
7
IndependentLixCy (0 < x ≤ 1, y = 6)
(curren tly a mended) The meth o d of claim [[1]] 2, wherein the graphite intercalation compound is LixC y, where 0 < x 1 and y = 6.
8
IndependentC
(c urre nt ly a men ded) The meth o d of claim [[1]] 2, wherein the graphite is selected from the group consisting of artificial graphite, natural graphite, and the combinations thereof.
9
IndependentC
(c urre nt ly a men ded) The meth o d of claim [[1]] 2, wherein the graphite is selected fr o m the gr o up consisting of a pow der f o rm, a granule f o rm, a rod f o rm, a fiber fo rm graphite, and the co m binations thereof.
10
Independentelectrolyte for lithium ion battery
(currently amended) The meth o d of claim [[1]] 2, wherein Page 3 of 8 Application Serial No. 14/470,083 PATENT Reply to office action of Docket: CU-71513 the ele ctro lyte f or a lithium i on battery i s s ele c ted fr o m the g ro up consistin g of an ethyle ne c arb on ate so luti on in which a lithiu m salt i s di ssolv ed, a dimethyl c arb o nate so luti o n i n which a lithi um salt i s dis solv ed, a diethyl c arb on ate so luti on in which a lithium salt i s di ssolv ed, an ethyl methyl c arb on ate so luti o n in which a lithium salt i s dissolv ed, a pr o pyle ne c arb on ate so luti on in which a lithium salt i s di sso lved, and the co mbi n ati ons there o f, and the lithium s alt i s s ele c ted from the g ro up c onsistin g of Li PF6, Li ClO4, Li CF₃SO3, LiBF4, Li AsF6, Li C₂F₆NO₄S2, Li B(C₂₀₄)2, Li H₂PO4, LiA lCl4, Li GaCl4, an d the co mbi n ati ons there of.
11
Independentelectrolyte for lithium ion battery
(o riginal) The m eth o d of c laim 10, w herei n the ele ctro lyte f o r a lithium i on battery further com pri ses one s ele c ted from the gr o up consistin g of methyl acetate (MA), methyl pr opion ate (MP), ethyl acetate (EA), ethyl pr opion ate (EP), a n d the co mbi n ati ons there of.
12
IndependentLiC
(c u rre n tly amen ded) The m eth o d of claim [[1]] 2, w herei n step (1) com pri s es applying graphite on a lithium f o il to com pre ss the lithium f o il o r to r ol l the lithium fo il i nto a roun d shape o r to be n d the lithi um fo il s o as to f orm an angle.
14
Independent
(c urren tly amen ded) The method of claim [[1]] 2, wherein step (2) is performed for 1 minute to 48 hours.
15
Independent
(currently amende d) The method of claim [[1]] 2, wherein step (3) is performed for 1 second to 12 hours.
16
Independentgraphene
(c urr en tly a mended) The method of clai m [[1]] 2, wherein step (3) further comprises filtering and washing the graphene formed, and the filtering is performed by using a centrifuge or a vacuum filter.
17
Dependent← claim 16
17. (o rigin al) The method of claim 16, wherein the va cuum filter ha s a po re size f 0. 0 1 t o 0.1 um.
18. (cu rre n tly amended) The method of claim [[1]] 2, further comprising: (4) di s per s ing the gr a phene f o rmed in step (3) into a di s per sive so lvent; and (5) drying the di s per s ed gr a phene to f o rm graphene powder.
20
IndependentLiCsecond metal (Cu, Ag, Au, Pt)grapheneelectrolyte for lithium ion battery
A m eth od for p rep arin g gr a phe ne using a sp ontaneous Page 5 of 8 Application Serial No. 14/470,083 PATENT Reply to office action of Docket: CU-71513 process, the m eth od com pri sing: (1) di sposin g lithi um metal i n surface contact w ith graphite an d disp os ing a seco nd m etal i n su rfa ce contact w ith the graphite, the secon d metal i s selected fr om the gr o up consisting of co pper (Cu), silv er (Ag), g o ld (Au), platin um (P t), a n d the com binati ons thereof, a nd the lithi um m etal a n d the second m etal are i n su rfa c e c ontact w ith each o ther while the graphite i s in terp os ed therebet ween; (2) i mmersing the su rfa ce contac ted lithi um metal a n d graphite i n an ele ctro lyte f or a lithi um ion battery t o form a graphite i n ter c alati on compound; and (3) introducin g the graphite i n ter c ala tion compoun d i nto w ater o r al coho l t o form graphene while ge n erati n g hydr ogen ga s, w herein step (2) is a cc elera t ed by v irt ue o f a n inc rea s ed p oten tia l differe nce caus ed d u e t o a fi x ed su rfa ce contact between the lithi um m etal a nd the secon d metal, w herei n the graphi t e is i n terp os ed therebet w een. Page 6 of 8
Materials
Materials described outside the worked examples.
lithium metal
Li
Intercalant/Reductant For Graphite Intercalation
graphite
C
Starting Material/Graphene Precursor
Process steps
Additional fabrication and treatment steps described in the patent.
1
Spontaneous Electrochemical Intercalation And Exfoliation
Step 1
Process details
step 1:Dispose lithium metal foil in surface contact with graphite; optionally dispose a second metal (Cu, Ag, Au, or Pt) in surface contact with graphite so that lithium and second metal contact each other with graphite interposed
step 2:Immerse surface-contacted lithium metal and graphite in lithium-ion battery electrolyte to form graphite intercalation compound (LixCy, 0<x≤1, y=6); spontaneously driven by potential difference; accelerated by galvanic couple with second metal; duration 1 min to 48 h
step 3:Introduce graphite intercalation compound into water or alcohol to form graphene while generating hydrogen gas; duration 1 s to 12 h; optionally filter (centrifuge or vacuum filter, pore size 0.01–0.1 μm) and wash
Characterization
Measurements and analyses referenced in the patent, with their drawing references.
afm
AFM
FIG. 1 0 a is an atomic force microscope (AFM) of the graphene prepared through Example 1 of the present invention.
METHOD FOR PREPARATION OF GRAPHENE USING SPONTANEOUS PROCESS
Chong Min KOO
US
Drawings
Patent drawings and their descriptions. Click a drawing to enlarge it.
FIG. 1
process chamber schematic
FIG. 1 0 a is an atomic force microscope (AFM) of the graphene prepared through Example 1 of the present invention.
FIG. 2
process chamber schematic
FIG. 2 is a schematic view illustrating a process of immersing graphite surrounded with a lithium foil prepared by the method of
FIG. 3
process chamber schematic
FIG. 3 is a schematic view representing a method of obtaining graphene by separating the graphite intercalation compound formed by the method of
FIG. 4
process chamber schematic
FIG. 4 is a schematic view illustrating a process in which the graphite intercalation compound is formed from graphite.
FIG. 5
process chamber schematic
FIG. 5 is a schematic view representing a phenomenon in which lithium and the electrolyte are co-intercalated into the interlayer region of graphite by 20 s …
FIG. 6
FIG. 6 is a small-angle X-ray scattering (SAXS) peak illustrating that l ithium is intercalated into the interlayer region of graphite in Example 1 of the …
FIG. 7
FIG. 7 is an electron diffraction pattern of the graphene prepared through 25 Example 1 of the present invention. 19
FIG. 8
FIG. 8 is a Raman spectroscopy result of the graphene prepared through Example 1 of the present invention and graphite which is the material thereof.
FIG. 9
FIG. 9 is a high-magnification transmission electron microscope (TEM) of the graphene prepared through Example 1 of the present invention. 5
FIG. 10
performance graph
FIG. 10 b is a graph showing a height of a graphene sheet prepared through Example 1 of the present invention.
Claims
Claims define the patent's legal scope. Independent claims stand alone; dependent claims (nested) narrow them. Click a claim to expand its dependents.
The method of claim 1 8, wherein the di s per sive solv ent i s selected from the group c onsis ting of N- methyl -2- pyrr o lidone (NMP), dimethylform a mide (DM F), imethyl a cet a mide (DMA c), dimethyl s ulf ox ide (DM₈₀), a nd the c om bin ations thereof.
2
IndependentLiCsecond metal (Cu, Ag, Au, Pt)CuAgAu
Thmethodof-taimrwherein step-(4) further omprises A ethod for preparing grahene sin spontaneous process, the method comprising: (1) disposing lithium metal in surface contact with graphite and disposing a second metal in surface contact with the graphite, the second metal is selected from the group consisting of copper (Cu), silver (Ag), gold (Au), platinum (Pt), and the combinations thereof, and the lithium metal and the second metal are in surface contact with each other while the graphite is interposed therebetween; (2)immersin the surface contacted lithiu r rnetal and qraphite in an electrolyte for a lithium ion batter to form a ra hite intercalation com ound; and (3) introducing the graphite intercalation compound into water or alcohol to form graphene while generating hydrogen gas.
4
Dependent← claim 2LiCsecond metal (Cu, Ag, Au, Pt)
(o riginal) The meth o d of claim 2, w herein step (2) is accelerated b y virtue of an increased p o tential difference caused due to a fi x ed surface c o ntact between the lithium metal and the sec o nd metal, wherein the graphite is interp o sed therebet w een.
6
Dependent← claim 2second metal (Cu, Ag, Au, Pt)
(o riginal) The meth o d of claim 2, w herein the sec o nd metal is in a form of a foil.
13
Dependent← claim 2LiCsecond metal (Cu, Ag, Au, Pt)
(o rigi n al) The m eth o d of claim 2, w herei n step (1) co mpri ses co mpre ss ing a s tru c ture f o rmed by pla cin g a seco nd metal f o il o n the lithium f o il on whic h graphite is applied, o r r o lli n g the s tru c ture i nto a r oun d shape o r be ndin g the s tru c ture so as to f orm an angle. Page 4 of 8 Application Serial No. 14/470,083 PATENT Reply to office action of Docket: CU-71513
3
IndependentLiC
The method of claim [[1]] 2, wherein step (2) is spontaneously performed by virtue of a potential difference due to a fixed surface contact between the lithium metal and the graphite. Page 2 of 8 Application Serial No. 14/470,083 PATENT Reply to office action of Docket: CU-71513
5
IndependentLi
(curren tly am ende d) The meth o d of claim [[1]] 2, wherein the lithium metal is in a form of a foil.
7
IndependentLixCy (0 < x ≤ 1, y = 6)
(curren tly a mended) The meth o d of claim [[1]] 2, wherein the graphite intercalation compound is LixC y, where 0 < x 1 and y = 6.
8
IndependentC
(c urre nt ly a men ded) The meth o d of claim [[1]] 2, wherein the graphite is selected from the group consisting of artificial graphite, natural graphite, and the combinations thereof.
9
IndependentC
(c urre nt ly a men ded) The meth o d of claim [[1]] 2, wherein the graphite is selected fr o m the gr o up consisting of a pow der f o rm, a granule f o rm, a rod f o rm, a fiber fo rm graphite, and the co m binations thereof.
10
Independentelectrolyte for lithium ion battery
(currently amended) The meth o d of claim [[1]] 2, wherein Page 3 of 8 Application Serial No. 14/470,083 PATENT Reply to office action of Docket: CU-71513 the ele ctro lyte f or a lithium i on battery i s s ele c ted fr o m the g ro up consistin g of an ethyle ne c arb on ate so luti on in which a lithiu m salt i s di ssolv ed, a dimethyl c arb o nate so luti o n i n which a lithi um salt i s dis solv ed, a diethyl c arb on ate so luti on in which a lithium salt i s di ssolv ed, an ethyl methyl c arb on ate so luti o n in which a lithium salt i s dissolv ed, a pr o pyle ne c arb on ate so luti on in which a lithium salt i s di sso lved, and the co mbi n ati ons there o f, and the lithium s alt i s s ele c ted from the g ro up c onsistin g of Li PF6, Li ClO4, Li CF₃SO3, LiBF4, Li AsF6, Li C₂F₆NO₄S2, Li B(C₂₀₄)2, Li H₂PO4, LiA lCl4, Li GaCl4, an d the co mbi n ati ons there of.
11
Independentelectrolyte for lithium ion battery
(o riginal) The m eth o d of c laim 10, w herei n the ele ctro lyte f o r a lithium i on battery further com pri ses one s ele c ted from the gr o up consistin g of methyl acetate (MA), methyl pr opion ate (MP), ethyl acetate (EA), ethyl pr opion ate (EP), a n d the co mbi n ati ons there of.
12
IndependentLiC
(c u rre n tly amen ded) The m eth o d of claim [[1]] 2, w herei n step (1) com pri s es applying graphite on a lithium f o il to com pre ss the lithium f o il o r to r ol l the lithium fo il i nto a roun d shape o r to be n d the lithi um fo il s o as to f orm an angle.
14
Independent
(c urren tly amen ded) The method of claim [[1]] 2, wherein step (2) is performed for 1 minute to 48 hours.
15
Independent
(currently amende d) The method of claim [[1]] 2, wherein step (3) is performed for 1 second to 12 hours.
16
Independentgraphene
(c urr en tly a mended) The method of clai m [[1]] 2, wherein step (3) further comprises filtering and washing the graphene formed, and the filtering is performed by using a centrifuge or a vacuum filter.
17
Dependent← claim 16
17. (o rigin al) The method of claim 16, wherein the va cuum filter ha s a po re size f 0. 0 1 t o 0.1 um.
18. (cu rre n tly amended) The method of claim [[1]] 2, further comprising: (4) di s per s ing the gr a phene f o rmed in step (3) into a di s per sive so lvent; and (5) drying the di s per s ed gr a phene to f o rm graphene powder.
20
IndependentLiCsecond metal (Cu, Ag, Au, Pt)grapheneelectrolyte for lithium ion battery
A m eth od for p rep arin g gr a phe ne using a sp ontaneous Page 5 of 8 Application Serial No. 14/470,083 PATENT Reply to office action of Docket: CU-71513 process, the m eth od com pri sing: (1) di sposin g lithi um metal i n surface contact w ith graphite an d disp os ing a seco nd m etal i n su rfa ce contact w ith the graphite, the secon d metal i s selected fr om the gr o up consisting of co pper (Cu), silv er (Ag), g o ld (Au), platin um (P t), a n d the com binati ons thereof, a nd the lithi um m etal a n d the second m etal are i n su rfa c e c ontact w ith each o ther while the graphite i s in terp os ed therebet ween; (2) i mmersing the su rfa ce contac ted lithi um metal a n d graphite i n an ele ctro lyte f or a lithi um ion battery t o form a graphite i n ter c alati on compound; and (3) introducin g the graphite i n ter c ala tion compoun d i nto w ater o r al coho l t o form graphene while ge n erati n g hydr ogen ga s, w herein step (2) is a cc elera t ed by v irt ue o f a n inc rea s ed p oten tia l differe nce caus ed d u e t o a fi x ed su rfa ce contact between the lithi um m etal a nd the secon d metal, w herei n the graphi t e is i n terp os ed therebet w een. Page 6 of 8
Materials
Materials described outside the worked examples.
lithium metal
Li
Intercalant/Reductant For Graphite Intercalation
graphite
C
Starting Material/Graphene Precursor
Process steps
Additional fabrication and treatment steps described in the patent.
1
Spontaneous Electrochemical Intercalation And Exfoliation
Step 1
Process details
step 1:Dispose lithium metal foil in surface contact with graphite; optionally dispose a second metal (Cu, Ag, Au, or Pt) in surface contact with graphite so that lithium and second metal contact each other with graphite interposed
step 2:Immerse surface-contacted lithium metal and graphite in lithium-ion battery electrolyte to form graphite intercalation compound (LixCy, 0<x≤1, y=6); spontaneously driven by potential difference; accelerated by galvanic couple with second metal; duration 1 min to 48 h
step 3:Introduce graphite intercalation compound into water or alcohol to form graphene while generating hydrogen gas; duration 1 s to 12 h; optionally filter (centrifuge or vacuum filter, pore size 0.01–0.1 μm) and wash
Characterization
Measurements and analyses referenced in the patent, with their drawing references.
afm
AFM
FIG. 1 0 a is an atomic force microscope (AFM) of the graphene prepared through Example 1 of the present invention.
METHOD FOR PREPARATION OF GRAPHENE USING SPONTANEOUS PROCESS
Chong Min KOO
US
Drawings
Patent drawings and their descriptions. Click a drawing to enlarge it.
FIG. 1
process chamber schematic
FIG. 1 0 a is an atomic force microscope (AFM) of the graphene prepared through Example 1 of the present invention.
FIG. 2
process chamber schematic
FIG. 2 is a schematic view illustrating a process of immersing graphite surrounded with a lithium foil prepared by the method of
FIG. 3
process chamber schematic
FIG. 3 is a schematic view representing a method of obtaining graphene by separating the graphite intercalation compound formed by the method of
FIG. 4
process chamber schematic
FIG. 4 is a schematic view illustrating a process in which the graphite intercalation compound is formed from graphite.
FIG. 5
process chamber schematic
FIG. 5 is a schematic view representing a phenomenon in which lithium and the electrolyte are co-intercalated into the interlayer region of graphite by 20 s …
FIG. 6
FIG. 6 is a small-angle X-ray scattering (SAXS) peak illustrating that l ithium is intercalated into the interlayer region of graphite in Example 1 of the …
FIG. 7
FIG. 7 is an electron diffraction pattern of the graphene prepared through 25 Example 1 of the present invention. 19
FIG. 8
FIG. 8 is a Raman spectroscopy result of the graphene prepared through Example 1 of the present invention and graphite which is the material thereof.
FIG. 9
FIG. 9 is a high-magnification transmission electron microscope (TEM) of the graphene prepared through Example 1 of the present invention. 5
FIG. 10
performance graph
FIG. 10 b is a graph showing a height of a graphene sheet prepared through Example 1 of the present invention.
Claims
Claims define the patent's legal scope. Independent claims stand alone; dependent claims (nested) narrow them. Click a claim to expand its dependents.
The method of claim 1 8, wherein the di s per sive solv ent i s selected from the group c onsis ting of N- methyl -2- pyrr o lidone (NMP), dimethylform a mide (DM F), imethyl a cet a mide (DMA c), dimethyl s ulf ox ide (DM₈₀), a nd the c om bin ations thereof.
2
IndependentLiCsecond metal (Cu, Ag, Au, Pt)CuAgAu
Thmethodof-taimrwherein step-(4) further omprises A ethod for preparing grahene sin spontaneous process, the method comprising: (1) disposing lithium metal in surface contact with graphite and disposing a second metal in surface contact with the graphite, the second metal is selected from the group consisting of copper (Cu), silver (Ag), gold (Au), platinum (Pt), and the combinations thereof, and the lithium metal and the second metal are in surface contact with each other while the graphite is interposed therebetween; (2)immersin the surface contacted lithiu r rnetal and qraphite in an electrolyte for a lithium ion batter to form a ra hite intercalation com ound; and (3) introducing the graphite intercalation compound into water or alcohol to form graphene while generating hydrogen gas.
4
Dependent← claim 2LiCsecond metal (Cu, Ag, Au, Pt)
(o riginal) The meth o d of claim 2, w herein step (2) is accelerated b y virtue of an increased p o tential difference caused due to a fi x ed surface c o ntact between the lithium metal and the sec o nd metal, wherein the graphite is interp o sed therebet w een.
6
Dependent← claim 2second metal (Cu, Ag, Au, Pt)
(o riginal) The meth o d of claim 2, w herein the sec o nd metal is in a form of a foil.
13
Dependent← claim 2LiCsecond metal (Cu, Ag, Au, Pt)
(o rigi n al) The m eth o d of claim 2, w herei n step (1) co mpri ses co mpre ss ing a s tru c ture f o rmed by pla cin g a seco nd metal f o il o n the lithium f o il on whic h graphite is applied, o r r o lli n g the s tru c ture i nto a r oun d shape o r be ndin g the s tru c ture so as to f orm an angle. Page 4 of 8 Application Serial No. 14/470,083 PATENT Reply to office action of Docket: CU-71513
3
IndependentLiC
The method of claim [[1]] 2, wherein step (2) is spontaneously performed by virtue of a potential difference due to a fixed surface contact between the lithium metal and the graphite. Page 2 of 8 Application Serial No. 14/470,083 PATENT Reply to office action of Docket: CU-71513
5
IndependentLi
(curren tly am ende d) The meth o d of claim [[1]] 2, wherein the lithium metal is in a form of a foil.
7
IndependentLixCy (0 < x ≤ 1, y = 6)
(curren tly a mended) The meth o d of claim [[1]] 2, wherein the graphite intercalation compound is LixC y, where 0 < x 1 and y = 6.
8
IndependentC
(c urre nt ly a men ded) The meth o d of claim [[1]] 2, wherein the graphite is selected from the group consisting of artificial graphite, natural graphite, and the combinations thereof.
9
IndependentC
(c urre nt ly a men ded) The meth o d of claim [[1]] 2, wherein the graphite is selected fr o m the gr o up consisting of a pow der f o rm, a granule f o rm, a rod f o rm, a fiber fo rm graphite, and the co m binations thereof.
10
Independentelectrolyte for lithium ion battery
(currently amended) The meth o d of claim [[1]] 2, wherein Page 3 of 8 Application Serial No. 14/470,083 PATENT Reply to office action of Docket: CU-71513 the ele ctro lyte f or a lithium i on battery i s s ele c ted fr o m the g ro up consistin g of an ethyle ne c arb on ate so luti on in which a lithiu m salt i s di ssolv ed, a dimethyl c arb o nate so luti o n i n which a lithi um salt i s dis solv ed, a diethyl c arb on ate so luti on in which a lithium salt i s di ssolv ed, an ethyl methyl c arb on ate so luti o n in which a lithium salt i s dissolv ed, a pr o pyle ne c arb on ate so luti on in which a lithium salt i s di sso lved, and the co mbi n ati ons there o f, and the lithium s alt i s s ele c ted from the g ro up c onsistin g of Li PF6, Li ClO4, Li CF₃SO3, LiBF4, Li AsF6, Li C₂F₆NO₄S2, Li B(C₂₀₄)2, Li H₂PO4, LiA lCl4, Li GaCl4, an d the co mbi n ati ons there of.
11
Independentelectrolyte for lithium ion battery
(o riginal) The m eth o d of c laim 10, w herei n the ele ctro lyte f o r a lithium i on battery further com pri ses one s ele c ted from the gr o up consistin g of methyl acetate (MA), methyl pr opion ate (MP), ethyl acetate (EA), ethyl pr opion ate (EP), a n d the co mbi n ati ons there of.
12
IndependentLiC
(c u rre n tly amen ded) The m eth o d of claim [[1]] 2, w herei n step (1) com pri s es applying graphite on a lithium f o il to com pre ss the lithium f o il o r to r ol l the lithium fo il i nto a roun d shape o r to be n d the lithi um fo il s o as to f orm an angle.
14
Independent
(c urren tly amen ded) The method of claim [[1]] 2, wherein step (2) is performed for 1 minute to 48 hours.
15
Independent
(currently amende d) The method of claim [[1]] 2, wherein step (3) is performed for 1 second to 12 hours.
16
Independentgraphene
(c urr en tly a mended) The method of clai m [[1]] 2, wherein step (3) further comprises filtering and washing the graphene formed, and the filtering is performed by using a centrifuge or a vacuum filter.
17
Dependent← claim 16
17. (o rigin al) The method of claim 16, wherein the va cuum filter ha s a po re size f 0. 0 1 t o 0.1 um.
18. (cu rre n tly amended) The method of claim [[1]] 2, further comprising: (4) di s per s ing the gr a phene f o rmed in step (3) into a di s per sive so lvent; and (5) drying the di s per s ed gr a phene to f o rm graphene powder.
20
IndependentLiCsecond metal (Cu, Ag, Au, Pt)grapheneelectrolyte for lithium ion battery
A m eth od for p rep arin g gr a phe ne using a sp ontaneous Page 5 of 8 Application Serial No. 14/470,083 PATENT Reply to office action of Docket: CU-71513 process, the m eth od com pri sing: (1) di sposin g lithi um metal i n surface contact w ith graphite an d disp os ing a seco nd m etal i n su rfa ce contact w ith the graphite, the secon d metal i s selected fr om the gr o up consisting of co pper (Cu), silv er (Ag), g o ld (Au), platin um (P t), a n d the com binati ons thereof, a nd the lithi um m etal a n d the second m etal are i n su rfa c e c ontact w ith each o ther while the graphite i s in terp os ed therebet ween; (2) i mmersing the su rfa ce contac ted lithi um metal a n d graphite i n an ele ctro lyte f or a lithi um ion battery t o form a graphite i n ter c alati on compound; and (3) introducin g the graphite i n ter c ala tion compoun d i nto w ater o r al coho l t o form graphene while ge n erati n g hydr ogen ga s, w herein step (2) is a cc elera t ed by v irt ue o f a n inc rea s ed p oten tia l differe nce caus ed d u e t o a fi x ed su rfa ce contact between the lithi um m etal a nd the secon d metal, w herei n the graphi t e is i n terp os ed therebet w een. Page 6 of 8
Materials
Materials described outside the worked examples.
lithium metal
Li
Intercalant/Reductant For Graphite Intercalation
graphite
C
Starting Material/Graphene Precursor
Process steps
Additional fabrication and treatment steps described in the patent.
1
Spontaneous Electrochemical Intercalation And Exfoliation
Step 1
Process details
step 1:Dispose lithium metal foil in surface contact with graphite; optionally dispose a second metal (Cu, Ag, Au, or Pt) in surface contact with graphite so that lithium and second metal contact each other with graphite interposed
step 2:Immerse surface-contacted lithium metal and graphite in lithium-ion battery electrolyte to form graphite intercalation compound (LixCy, 0<x≤1, y=6); spontaneously driven by potential difference; accelerated by galvanic couple with second metal; duration 1 min to 48 h
step 3:Introduce graphite intercalation compound into water or alcohol to form graphene while generating hydrogen gas; duration 1 s to 12 h; optionally filter (centrifuge or vacuum filter, pore size 0.01–0.1 μm) and wash
Characterization
Measurements and analyses referenced in the patent, with their drawing references.
afm
AFM
FIG. 1 0 a is an atomic force microscope (AFM) of the graphene prepared through Example 1 of the present invention.