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US5965299A Expired / Lapsed US ⏱️ 0.0 years remaining

Composite electrolyte containing surface modified fumed silica

Assignee: UNIVERSITY MICHIGAN STATE
•
Filing: 1997-06-23
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Granted: 1999-10-12
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Expires: 2017-06-23
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Abstract

Abstract A composite electrolyte comprises (a) surface modified fumed silica filler, wherein the surface modified fumed silica comprises polymerizable groups on the surface thereof, the polymerizable groups being bonded to each other such that the surface modified fumed silica filler is crosslinked in a three-dimensional structure; (b) a dissociable lithium salt; and (c) a bulk medium which contains the surface modified fumed silica filler and the dissociable lithium salt. An electrochemical cell comprises an anode, a cathode, and a composite electrolyte dispersed between the anode and cathode.

Inventors

  • 👤 Saad A. Khan
  • 👤 Peter S. Fedkiw
  • 👤 Gregory L. Baker
  • 👤 Jiang Fan
  • 👤 Srinivasa R. Raghavan
  • 👤 Jun Hou

Bibliographic Details

Application Number —
Jurisdiction US
Data Source google_patents
Last Synchronized 2026-10-26 18:56
CPC Classifications
H; H01; H01M; H01M10/00; H01M10/05; H01M10/052; C; C08; C08F; C08F292/00; C09; C09C; C09C1/00; C09C1/28; C09C1/30; C09C1/3072; H01M10/056; H01M10/0564; H01M10/0565; H01M4/00; H01M4/02; H01M4/62; H01M4/621; H01M6/00; H01M6/22; C01; C01P; C01P2004/00; C01P2004/50; C01P2006/00; C01P2006/40; C01P2006/90; H01M6/14; H01M6/16; H01M6/162; H01M6/168; Y; Y02; Y02E; Y02E60/00; Y02E60/10

Claims Analysis

Total Claims: 60
Claim 1
Independent Claim 95 words
A composite electrolyte comprising: (a) a filler comprising surface modified fumed silica particles, wherein said surface modified fumed silica comprises polymerizable groups on the surface thereof, said polymerizable groups being covalently bonded to each other in a chemical reaction such that said surface modified fumed silica filler is bridged by polymer chains formed from the polymerizable groups, the surface modified fumed silica filler being crosslinked and present as a three-dimensional structure and; (b) a dissociable lithium salt; and (b) a bulk medium which contains said surface modified fumed silica filler and said dissociable lithium salt.
Claim 2
Dependent Claim 95 words
A composite electrolyte comprising: (a) a filler comprising surface modified fumed silica particles, wherein said surface modified fumed silica comprises polymerizable groups on the surface thereof, said polymerizable groups being covalently bonded to each other in a chemical reaction such that said surface modified fumed silica filler is bridged by polymer chains formed from the polymerizable groups, the surface modified fumed silica filler being crosslinked and present as a three-dimensional structure and; (b) a dissociable lithium salt; and (b) a bulk medium which contains said surface modified fumed silica filler and said dissociable lithium salt.
Claim 3
Dependent Claim 42 words
The composite electrolyte according to claim 1, wherein said bulk medium comprises a liquid component selected from the group consisting of a poly(ethylene glycol) polymer having a weight average molecular weight of less than about 1000, an organic carbonate, and mixtures thereof.
Claim 4
Dependent Claim 33 words
The composite electrolyte according to claim 2, wherein said poly(ethylene glycol) polymer is selected from the group consisting of poly(ethylene glycol), poly(ethylene glycol) mono methyl ether, poly(ethylene glycol) dimethyl ether, and mixtures thereof.
Claim 5
Dependent Claim 27 words
The composite electrolyte according to claim 2, wherein said organic carbonate is selected from the group consisting of dimethyl carbonate, propylene carbonate, ethylene carbonate, and mixtures thereof.
Claim 6
Dependent Claim 28 words
The composite electrolyte according to claim 1, wherein said bulk medium comprises material having a weight average molecular weight ranging from about 1000 to about 10 7 .
Claim 7
Dependent Claim 40 words
The composite electrolyte according to claim 1, wherein said dissociable lithium salt is selected from the group consisting of lithium imide, lithium triflate, lithium tetrafluoroborate, lithium perchlorate, lithium iodide, lithium trifluorocarbonate, lithium nitrate, lithium thiocyanate, lithium hexafluoroarsenate, and mixtures thereof.
Claim 8
Dependent Claim 30 words
The composite electrolyte according to claim 1, wherein said electrolyte has an ionic conductivity measured at room temperature ranging from about 10 -3 to about 10 -2 Scm -1 .
Claim 9
Dependent Claim 24 words
The composite electrolyte according to claim 1, wherein said electrolyte has an elastic modulus ranging from about 10 4 to about 10 7 Pa.
Claim 10
Dependent Claim 38 words
The composite electrolyte according to claim 1, wherein said composite electrolyte has an electrochemical stability characterized by a current density ranging from about 10 to about 20 μA/cm 2 at a voltage of at least about 4.5 V.
Claim 11
Dependent Claim 103 words
The composite electrolyte according to claim 1, wherein said electrolyte comprises: (a) from about 1 to about 50 percent by weight of surface modified fumed silica filler, wherein said surface modified fumed silica comprises polymerizable groups on the surface thereof, said polymerizable groups being bonded to each other such that said surface modified fumed silica filler is crosslinked in a three-dimensional structure; (b) from about 5 to about 40 percent by weight of a dissociable lithium salt; and (c) up to about 90 percent by weight of a bulk medium which contains said surface modified fumed silica filler and said dissociable lithium salt.
Claim 12
Dependent Claim 117 words
An electrochemical cell comprising: (a) an anode; (b) a cathode; and (c) interposed between said anode and said cathode, a composite electrolyte, wherein said composite electrolyte comprises: (i) a filler comprising surface modified fumed silica particles, wherein said surface modified fumed silica comprises polymerizable groups on the surface thereof, said polymerizable groups being covalently bonded to each other in a chemical reaction such that said surface modified fumed silica filler is bridged by polvmer chains formed from the polymerizable groups, the surface modified fumed silica filler being crosslinked and present as a three-dimensional structure; (ii) a dissociable lithium salt; and (iii) a bulk medium which contains said surface modified fumed silica filler and said dissociable lithium salt.
Claim 13
Dependent Claim 117 words
An electrochemical cell comprising: (a) an anode; (b) a cathode; and (c) interposed between said anode and said cathode, a composite electrolyte, wherein said composite electrolyte comprises: (i) a filler comprising surface modified fumed silica particles, wherein said surface modified fumed silica comprises polymerizable groups on the surface thereof, said polymerizable groups being covalently bonded to each other in a chemical reaction such that said surface modified fumed silica filler is bridged by polvmer chains formed from the polymerizable groups, the surface modified fumed silica filler being crosslinked and present as a three-dimensional structure; (ii) a dissociable lithium salt; and (iii) a bulk medium which contains said surface modified fumed silica filler and said dissociable lithium salt.
Claim 14
Dependent Claim 14 words
The electrochemical cell according to claim 11, wherein said anode is a lithium anode.
Claim 15
Dependent Claim 43 words
The electrochemical cell according to claim 11, wherein said cathode is selected from the group consisting of TiS 2 , V 6 O 13 , FeS 2 , LiNiO 2 , LiCO 2 , LiMn 2 O 4 , and organic sulfur cathodes.
Claim 16
Dependent Claim 42 words
The electrochemical cell according to claim 11, wherein said bulk medium comprises a liquid component selected from the group consisting of a poly(ethylene glycol) polymer having a weight average molecular weight of less than about 1000, an organic carbonate, and mixtures thereof.
Claim 17
Dependent Claim 33 words
The electrochemical cell according to claim 14, wherein said poly(ethylene glycol) polymer is selected from the group consisting of poly(ethylene glycol), poly(ethylene glycol) mono methyl ether, poly(ethylene glycol) dimethyl ether, and mixtures thereof.
Claim 18
Dependent Claim 27 words
The electrochemical cell according to claim 14, wherein said organic carbonate is selected from the group consisting of dimethyl carbonate, propylene carbonate, ethylene carbonate, and mixtures thereof.
Claim 19
Dependent Claim 28 words
The electrochemical cell according to claim 11, wherein said bulk medium comprises material having a weight average molecular weight ranging from about 1000 to about 10 7 .
Claim 20
Dependent Claim 40 words
The electrochemical cell according to claim 11, wherein said dissociable lithium salt is selected from the group consisting of lithium imide, lithium triflate, lithium tetrafluoroborate, lithium perchlorate, lithium iodide, lithium trifluorocarbonate, lithium nitrate, lithium thiocyanate, lithium hexafluoroarsenate, and mixtures thereof.
Claim 21
Dependent Claim 30 words
The electrochemical cell according to claim 11, wherein said electrolyte has an ionic conductivity measured at room temperature ranging from about 10 -3 to about 10 -2 Scm -1 .
Claim 22
Dependent Claim 24 words
The electrochemical cell according to claim 12, wherein said electrolyte has an elastic modulus ranging from about 10 4 to about 10 7 Pa.
Claim 23
Dependent Claim 38 words
The electrochemical cell according to claim 12, wherein said composite electrolyte has an electrochemical stability characterized by a current density ranging from about 10 to about 20 μA/cm 2 at a voltage of at least about 4.5 V.
Claim 24
Dependent Claim 116 words
A battery comprising: (a) an anode; (b) a cathode; and (c) interposed between said anode and said cathode, a composite electrolyte, wherein said composite electrolyte comprises: (i) a filler comprising surface modified fumed silica particles, wherein said surface modified fumed silica comprises polymerizable groups on the surface thereof, said polymerizable groups being covalently bonded to each other in a chemical reaction such that said surface modified fumed silica filler is bridged by polymer chains formed from the polymerizable groups, the surface modified fumed silica filler being crosslinked and present as a three-dimensional structure; (ii) a dissociable lithium salt; and (iii) a bulk medium which contains said surface modified fumed silica filler and said dissociable lithium salt.
Claim 25
Dependent Claim 116 words
A battery comprising: (a) an anode; (b) a cathode; and (c) interposed between said anode and said cathode, a composite electrolyte, wherein said composite electrolyte comprises: (i) a filler comprising surface modified fumed silica particles, wherein said surface modified fumed silica comprises polymerizable groups on the surface thereof, said polymerizable groups being covalently bonded to each other in a chemical reaction such that said surface modified fumed silica filler is bridged by polymer chains formed from the polymerizable groups, the surface modified fumed silica filler being crosslinked and present as a three-dimensional structure; (ii) a dissociable lithium salt; and (iii) a bulk medium which contains said surface modified fumed silica filler and said dissociable lithium salt.
Claim 26
Dependent Claim 41 words
The battery according to claim 22, wherein said bulk medium comprises a liquid component selected from the group consisting of a poly(ethylene glycol) polymer having a weight average molecular weight of less than about 1000, an organic carbonate, and mixtures thereof.
Claim 27
Dependent Claim 32 words
The battery according to claim 23, wherein said poly(ethylene glycol) polymer is selected from the group consisting of poly(ethylene glycol), poly(ethylene glycol) mono methyl ether, poly(ethylene glycol) dimethyl ether, and mixtures thereof.
Claim 28
Dependent Claim 26 words
The battery according to claim 23, wherein said organic carbonate is selected from the group consisting of dimethyl carbonate, propylene carbonate, ethylene carbonate, and mixtures thereof.
Claim 29
Dependent Claim 27 words
The battery according to claim 22, wherein said bulk medium comprises material having a weight average molecular weight ranging from about 1000 to about 10 7 .
Claim 30
Dependent Claim 39 words
The battery according to claim 22, wherein said dissociable lithium salt is selected from the group consisting of lithium imide, lithium triflate, lithium tetrafluoroborate, lithium perchlorate, lithium iodide, lithium trifluorocarbonate, lithium nitrate, lithium thiocyanate, lithium hexafluoroarsenate, and mixtures thereof.
Claim 31
Dependent Claim 29 words
The battery according to claim 22, wherein said electrolyte has an ionic conductivity measured at room temperature ranging from about 10 -3 to about 10 -2 Scm -1 .
Claim 32
Dependent Claim 23 words
The battery according to claim 22, wherein said electrolyte has an elastic modulus ranging from about 10 4 to about 10 7 Pa.
Claim 33
Dependent Claim 37 words
The battery according to claim 22, wherein said electrolyte has an electrochemical stability characterized by having a current density ranging from about 10 to about 20 μA/cm 2 at a voltage of at least about 4.5 V.
Claim 34
Dependent Claim 13 words
The battery according to claim 22, wherein said battery is a lithium battery.
Claim 35
Dependent Claim 13 words
The battery according to claim 22, wherein said battery is a lithium-ion battery.
Claim 36
Independent Claim 133 words
A method of producing a composite electrolyte comprising: reacting fumed silica with a surface monomer to modify the surface of the fumed silica, wherein polymerizable groups become present on the surface of the fumed silica; contacting the fumed silica with a bulk medium comprising a dissociable lithium salt, an initiator, and a monomer which does not react with the surface of the fumed silica but is capable of reacting with the polymerizable groups; processing the mixture into a defined geometry; and polymerizing the mixture such that the polymerizable groups on the surface of the fumed silica become covalently bonded to each other in a chemical reaction such that the surface modified fumed silica filler is bridged by polymer chains formed from the polymerizable groups, and wherein a three-dimensional composite electrolyte structure is formed.
Claim 37
Independent Claim 133 words
A method of producing a composite electrolyte comprising: reacting fumed silica with a surface monomer to modify the surface of the fumed silica, wherein polymerizable groups become present on the surface of the fumed silica; contacting the fumed silica with a bulk medium comprising a dissociable lithium salt, an initiator, and a monomer which does not react with the surface of the fumed silica but is capable of reacting with the polymerizable groups; processing the mixture into a defined geometry; and polymerizing the mixture such that the polymerizable groups on the surface of the fumed silica become covalently bonded to each other in a chemical reaction such that the surface modified fumed silica filler is bridged by polymer chains formed from the polymerizable groups, and wherein a three-dimensional composite electrolyte structure is formed.
Claim 38
Dependent Claim 13 words
The method according to claim 33, wherein said polymerization step is thermally initiated.
Claim 39
Dependent Claim 15 words
The method according to claim 33, wherein said polymerization step is initiated by actinic radiation.
Claim 40
Dependent Claim 17 words
The method according to claim 33, wherein said polymerization step is initiated by utilizing an electron beam.
Claim 41
Dependent Claim 110 words
A composite electrolyte comprising: (a) a surface modified fumed silica filler, wherein said surface modified fumed silica comprises polymerizable groups on the surface thereof, said polymerizable groups being covalently bonded to each other in a chemical reaction such that said surface modified fumed silica filler is bridged by polymer chains formed from the polymerizable groups, the surface modified fumed silica being crosslinked and present as a three-dimensional structure, and wherein said surface modified fumed silica filler has at least one methacrylate-terminated oligomeric chain on the surface thereof; (b) a dissociable lithium salt; and (c) a bulk medium which contains said surface modified fumed silica filler and said dissociable lithium salt.
Claim 42
Dependent Claim 110 words
A composite electrolyte comprising: (a) a surface modified fumed silica filler, wherein said surface modified fumed silica comprises polymerizable groups on the surface thereof, said polymerizable groups being covalently bonded to each other in a chemical reaction such that said surface modified fumed silica filler is bridged by polymer chains formed from the polymerizable groups, the surface modified fumed silica being crosslinked and present as a three-dimensional structure, and wherein said surface modified fumed silica filler has at least one methacrylate-terminated oligomeric chain on the surface thereof; (b) a dissociable lithium salt; and (c) a bulk medium which contains said surface modified fumed silica filler and said dissociable lithium salt.
Claim 43
Dependent Claim 23 words
The composite electrolyte according to claim 37, wherein said methacrylate-terminated oligomeric chain is connected to a C 1 to C 16 hydrocarbon group.
Claim 44
Dependent Claim 41 words
The composite electrolyte according to claim 37, wherein said bulk medium comprises a liquid component selected from the group consisting of poly(ethylene glycol) polymer having a weight average molecular weight of less than about 1000, an organic carbonate, and mixtures thereof.
Claim 45
Dependent Claim 30 words
The composite electrolyte according to claim 37, wherein said electrolyte has an ionic conductivity measured at room temperature ranging from about 10 -3 to about 10 -2 Scm -1 .
Claim 46
Dependent Claim 132 words
An electrochemical cell comprising: (a) an anode; (b) a cathode; and (c) interposed between said anode and said cathode, a composite electrolyte, wherein said composite electrolyte comprises: (i) surface modified fumed silica filler, wherein said surface modified fumed silica comprises polymerizable groups on the surface thereof, said polymerizable groups being covalently bonded to each other in a chemical reaction such that said surface modified fumed silica filler is bridged by polymer chains formed from the polymerizable groups, the surface modified fumed silica being crosslinked and present as a three-dimensional structure, and wherein said surface modified fumed silica filler has at least one methacrylate-terminated oligomeric chain on the surface thereof; (ii) a dissociable lithium salt; and (iv) a bulk medium which contains said surface modified fumed silica filler and said dissociable lithium salt.
Claim 47
Dependent Claim 132 words
An electrochemical cell comprising: (a) an anode; (b) a cathode; and (c) interposed between said anode and said cathode, a composite electrolyte, wherein said composite electrolyte comprises: (i) surface modified fumed silica filler, wherein said surface modified fumed silica comprises polymerizable groups on the surface thereof, said polymerizable groups being covalently bonded to each other in a chemical reaction such that said surface modified fumed silica filler is bridged by polymer chains formed from the polymerizable groups, the surface modified fumed silica being crosslinked and present as a three-dimensional structure, and wherein said surface modified fumed silica filler has at least one methacrylate-terminated oligomeric chain on the surface thereof; (ii) a dissociable lithium salt; and (iv) a bulk medium which contains said surface modified fumed silica filler and said dissociable lithium salt.
Claim 48
Dependent Claim 23 words
The electrochemical cell according to claim 41, wherein said methacrylate-terminated oligomeric chain is connected to a C 1 to C 16 hydrocarbon group.
Claim 49
Dependent Claim 41 words
The electrochemical cell according to claim 41, wherein said bulk medium comprises a liquid component selected from the group consisting of poly(ethylene glycol) polymer having a weight average molecular weight of less than about 1000, an organic carbonate, and mixtures thereof.
Claim 50
Dependent Claim 30 words
The electrochemical cell according to claim 37, wherein said electrolyte has an ionic conductivity measured at room temperature ranging from about 10 -3 to about 10 -2 Scm -1 .
Claim 51
Dependent Claim 131 words
A battery comprising: (a) an anode; (b) a cathode; and (c) interposed between said anode and said cathode, a composite electrolyte, wherein said composite electrolyte comprises: (i) surface modified fumed silica filler, wherein said surface modified fumed silica comprises polymerizable groups on the surface thereof, said polymerizable groups being bonded covalently to each other in a chemical reaction such that said surface modified fumed silica filler is bridged by polymer chains formed from the polymerizable groups, the surface modified fumed silica being crosslinked and present as a three-dimensional structure, and wherein said surface modified fumed silica filler has at least one methacrylate-terminated oligomeric chain on the surface thereof; (ii) a dissociable lithium salt; and (iii) a bulk medium which contains said surface modified fumed silica filler and said dissociable lithium salt.
Claim 52
Dependent Claim 131 words
A battery comprising: (a) an anode; (b) a cathode; and (c) interposed between said anode and said cathode, a composite electrolyte, wherein said composite electrolyte comprises: (i) surface modified fumed silica filler, wherein said surface modified fumed silica comprises polymerizable groups on the surface thereof, said polymerizable groups being bonded covalently to each other in a chemical reaction such that said surface modified fumed silica filler is bridged by polymer chains formed from the polymerizable groups, the surface modified fumed silica being crosslinked and present as a three-dimensional structure, and wherein said surface modified fumed silica filler has at least one methacrylate-terminated oligomeric chain on the surface thereof; (ii) a dissociable lithium salt; and (iii) a bulk medium which contains said surface modified fumed silica filler and said dissociable lithium salt.
Claim 53
Dependent Claim 22 words
The batttery according to claim 45, wherein said methacrylate-terminated oligomeric chain is connected to a C 1 to C 16 hydrocarbon group.
Claim 54
Dependent Claim 40 words
The battery according to claim 45, wherein said bulk medium comprises a liquid component selected from the group consisting of poly(ethylene glycol) polymer having a weight average molecular weight of less than about 1000, an organic carbonate, and mixtures thereof.
Claim 55
Dependent Claim 29 words
The battery according to claim 45, wherein said electrolyte has an ionic conductivity measured at room temperature ranging from about 10 -3 to about 10 -2 Scm -1 .
Claim 56
Independent Claim 137 words
A method of producing a composite electrolyte comprising: reacting fumed silica with a surface reactive monomer to modify the surface of the fumed silica, wherein a polymerizable group becomes present on the surface of the fumed silica, said surface modiifed fumed silica filler having a methacrylate-terminated oligomeric chain on the surface thereof; contacting said fumed silica with a bulk medium comprising a dissociable lithium salt, an initiator, and a monomer which does not react with the surface of the fumed silica but is capable of reacting with the polymerizable group; processing the mixture into a defined geometry where the fumed silica filler is bridged by polymer chains formed from the polymerizable group; and polymerizing the mixture such that the polymerizable groups on the surface of the fumed silica become bonded and a three-dimensional composite structure is formed.
Claim 57
Independent Claim 137 words
A method of producing a composite electrolyte comprising: reacting fumed silica with a surface reactive monomer to modify the surface of the fumed silica, wherein a polymerizable group becomes present on the surface of the fumed silica, said surface modiifed fumed silica filler having a methacrylate-terminated oligomeric chain on the surface thereof; contacting said fumed silica with a bulk medium comprising a dissociable lithium salt, an initiator, and a monomer which does not react with the surface of the fumed silica but is capable of reacting with the polymerizable group; processing the mixture into a defined geometry where the fumed silica filler is bridged by polymer chains formed from the polymerizable group; and polymerizing the mixture such that the polymerizable groups on the surface of the fumed silica become bonded and a three-dimensional composite structure is formed.
Claim 58
Dependent Claim 22 words
The method according to claim 49, wherein said methacrylate-terminated oligomeric chain is connected to a C 1 to C 16 hydrocarbon group.
Claim 59
Dependent Claim 40 words
The method according to claim 49, wherein said bulk medium comprises a liquid component selected from the group consisting of poly(ethylene glycol) polymer having a weight average molecular weight of less than about 1000, an organic carbonate, and mixtures thereof.
Claim 60
Dependent Claim 61 words
The method according to claim 49, wherein said electrolyte has an where the fumed silica filler is bridged by polymer chains formed from the polymerizable group, ionic conductivity measured at room temperature ranging from about 10 31 3 to where the fumed silica filler is bridged by polymer chains formed from the polymerizable group, about 10 31 2 Scm -1 .

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