Notice of Pre-AIA or AIA Status
The present application, filed on or after March 16, 2013, is being examined under the first inventor to file provisions of the AIA .
Information Disclosure Statement
The information disclosure statement (IDS) submitted on 1/31/24 has been considered by the examiner.
Claims Analysis
Claim 1 recites the “polymer has a melting point or glass transition temperature higher than 300°C or a thermal decomposition temperature higher than 400°C”. This limitation is interpreted to encompass a first thermally stable polymer having a melting point (no specific melting temperature is required by the claim).
Regarding claim 9, the claim is directed toward a hybrid separator. The lithium salt is dispersed in the hybrid separator [0025] but does not appear to be part of the structure of the claimed hybrid separator. Claim 9 has not been given patentable weight as the claim appears to recite an intended use limitation (i.e., requires the use in a battery containing a lithium salt electrolyte).
Regarding claim 16, the claimed lithium salt concentration of 2.0 M or higher is only limiting the claimed quasi-solid electrolyte. The lithium salt concentration is not limiting the claimed liquid electrolyte, solid electrolyte, inorganic solid electrolyte or a composite electrolyte.
Regarding claim 19, an alkaline solution is defined as a solution having a pH greater than 7 and an acidic solution is defined as a solution having a pH less than 7.
Claims Objections
In claim 2, line 10, the first listed polymer contains a typographical error. Examiner suggests “1,2,3-“. See also claim 4.
In claim 3, line 2, the period should be removed from the middle of the claim. Examiner suggests “Ga,”. See also claims 5 and 6.
Claim Rejections - 35 USC § 112
The following is a quotation of 35 U.S.C. 112(b):
(b) CONCLUSION.—The specification shall conclude with one or more claims particularly pointing out and distinctly claiming the subject matter which the inventor or a joint inventor regards as the invention.
The following is a quotation of 35 U.S.C. 112 (pre-AIA ), second paragraph:
The specification shall conclude with one or more claims particularly pointing out and distinctly claiming the subject matter which the applicant regards as his invention.
Claims 1-23 are rejected under 35 U.S.C. 112(b) or 35 U.S.C. 112 (pre-AIA ), second paragraph, as being indefinite for failing to particularly point out and distinctly claim the subject matter which the inventor or a joint inventor (or for applications subject to pre-AIA 35 U.S.C. 112, the applicant), regards as the invention.
Claim 1 recites the limitation "the ceramic coating or shell" in line 7. There is insufficient antecedent basis for this limitation in the claim. Examiner suggests “the ceramic coating”.
The claims recite improper group language creating confusion as to the list of alternatively useable members. The format of the claimed groups should clearly recite the alternative members of the group (e.g., alternatives may be set forth as "a material selected from the group consisting of A, B, and C" or "wherein the material is A, B, or C"). See MPEP 2117 and MPEP 2173.05(h). See at least the last three lines of claim 2. See the first three and last two lines of claim 3. See the first two and last three lines if claim 4. See lines 2-5 of claim 5. See lines 2-5 of claim 6. See claim 12 that recites “or” in the middle of the claim and at the end of the claim.
Claim 3 recites the limitation "said ceramic" in line 1. There is insufficient antecedent basis for this limitation in the claim. Examiner suggests “said ceramic coating”. All recitations of “said ceramic” in claims 3-23 require correction.
The term “type” in claim 8 is a relative term which renders the claim indefinite. The term “type” is not defined by the claim, the specification does not provide a standard for ascertaining the requisite degree, and one of ordinary skill in the art would not be reasonably apprised of the scope of the invention. For example, it is unclear what encompasses an “oxide type” or a “hydride type” of an inorganic solid electrolyte material. See also claim 17 that recites “type”.
Claim 10 recites the limitation "said lithium salt" in line 1. There is insufficient antecedent basis for this limitation in the claim.
Claim 11 recites “preferably from 30% to 85%”, which is indefinite. A broad range or limitation together with a narrow range or limitation that falls within the broad range or limitation (in the same claim) may be considered indefinite if the resulting claim does not clearly set forth the metes and bounds of the patent protection desired. See MPEP § 2173.05(c). The claim(s) are considered indefinite because there is a question or doubt as to whether the feature introduced by such narrower language is (a) merely exemplary of the remainder of the claim, and therefore not required, or (b) a required feature of the claims.
Claim 16 recites the limitation "the secondary battery" in line 1. There is insufficient antecedent basis for this limitation in the claim. Claim 15 recites “a lithium secondary battery” or “sodium secondary battery”.
Claim 17 recites the limitation "the secondary battery" in line 1. There is insufficient antecedent basis for this limitation in the claim. Claim 15 recites “a lithium secondary battery” or “sodium secondary battery”.
Claims 18 and 20 recite multiple limitations having insufficient antecedent basis in the claim. For example, “multiple fibers of a first thermally stable polymer” and “a ceramic layer”. Examiner notes claims 18 and 20 each depend from claim 1.
To the extent the claims are understood in view of the 35 USC 112 rejections above, note the following prior art rejections.
Claim Rejections - 35 USC § 102
The following is a quotation of the appropriate paragraphs of 35 U.S.C. 102 that form the basis for the rejections under this section made in this Office action:
A person shall be entitled to a patent unless –
(a)(1) the claimed invention was patented, described in a printed publication, or in public use, on sale, or otherwise available to the public before the effective filing date of the claimed invention.
Claim(s) 1-19 and 22 is/are rejected under 35 U.S.C. 102(a)(1) as being anticipated by Pascaly et al., US 2008/0190841 A1.
Pascaly teaches a flexible, ceramic membrane useful as a separator for batteries, especially lithium batteries. The membrane containing a polymeric non-woven; a ceramic coating on and in the non-woven; wherein the ceramic coating comprises at least one oxide selected from the group consisting of Al2O3, TiO2, ZrO2, BaTiO3, SiO2, and mixtures thereof [abstract]. The polymeric fibers of the non-woven preferably comprise non-electroconductive fibers of polymers which are preferably selected from polyacrylonitrile (PAN), polyester, for example polyethylene terephthalate (PET), polyamide (PA), for example nylon 12 or polyolefins, for example polypropylene (PP) or polyethylene (PE). More preferably, the non-woven comprises polymeric fibers composed of polyester, especially PET, and/or polyamide, especially nylon 12, or consists fully of these polymeric fibers. The polymeric fibers of the non-wovens are preferably from 0.1 to 10 mm and more preferably from 1 to 5 mm in diameter [0079]. The membranes preferably comprise polymeric non-wovens which are flexible and preferably less than 50 mm in thickness and have a porosity of 50-97% [0076-0078]. The ceramic coating has a layer thickness of preferably less than 100 nm [0075].
The non-woven is preferably less than 30 mm in thickness. It may be preferable for the polymeric fibers to be from 0.1 to 10 mm and preferably from 1 to 5 mm in diameter. It is particularly preferable to use a polymeric non-woven which comprises fibers selected from polyacrylonitrile, polyester, polyimide, polyamide, polytetrafluoroethylene and/or polyolefin [0105]. The separator may comprise an adhesion promoter which is based on an alkylalkoxysilane [0030;0099]. The separator may contain an electrolyte comprising lithium salts having large anions in carbonate solvents. Examples of lithium salts include LiClO4, LiBF4 and LiPF6. Solvents include ethylene carbonate and propylene carbonate[0134].
The separator is very saft in the event of internal short circuiting as the separator has no meltdown effect [0059-0066]. The separator may contains shut down particles or a layer of shutdown particles, such as waxes and polyolefins [0087].
Regarding process claims 18, 19 and 22, see at least [0027-0036], [0042-0044], [0056-0057], [0074] and [0090-0133]. The process of Pascaly may include admixing adhesion promoters, particularly amine-functional and glycidyl-functionalized silanes [0102;0118]. The process of Pascaly comprises heat treating to form the ceramic coating on the polymeric non-woven [0028]. The solvent may include an anhydrous solvent such as an alcohol. See also the Examples of Pascaly. Thus, the claims are anticipated.
*
Claim(s) 1-4, 8-11, 13-19 and 22 is/are rejected under 35 U.S.C. 102(a)(1) as being anticipated by Smith et al., US 2021/0167463 A1.
Smith teaches polymer-ceramic hybrid membranes, as well as processes for manufacturing such membranes. In particular, polymer-ceramic hybrid membranes are non-flammable and thermally stable and may be used in batteries, such as lithium ion batteries [abstract].
Smith teaches a thermally stable, flame-resistant polymer-ceramic battery separator membrane. In specific embodiments, the separator membrane comprising a nanofiber mat, the nanofiber mat comprising one or more shelled nanofiber(s). In more specific embodiments, the one or more shelled nanofiber comprises a continuous core material and a continuous shell material (e.g., that runs along the entire length or a part of the length of the nanofiber), the continuous core material comprising a polymer, and the continuous shell material comprising a ceramic [0076-0079; 0129].
The nanofiber, nanofiber mats, separators, or other membranes may comprise a polyimide (glass transition temperature >300°C) and a ceramic (e.g., of a coated fiber mat and/or a ceramic-polymer hybrid fiber mat prepared directly from electrospinning a combination of polymer (e.g., polyimide) and ceramic precursor) being treated to a temperature of at least 250°C, more preferably, at least 275°C, and still more preferably about 300°C or more. As demonstrated in the examples, untreated products or products treated at lower temperatures have a greatly reduced resistance to flammability compared to those that are treated at higher temperatures [0097].
The membrane has any suitable thickness. The membrane (e.g., separator membrane) has an average thickness of about 1 micron to about 25 micron (e.g., about 5 micron to about 15 micron, or about 5 micron to about 10 micron). In preferred embodiments, the average thickness is about 8 to about 20 micron, such as about 12 to about 15 micron [0093]. The nanofiber mat or precursor membrane described herein comprising ceramic precursor and/or partially cured ceramic precursor can be thicker than a separator membrane described herein (e.g., as the membrane may be calendered to achieved the thickness desired in the separator membrane). The nanofiber mat or precursor membrane has a thickness of about 1 micron to about 50 micron, such as about 5 micron to about 50 micron or about 10 micron to about 50 micron. In some embodiments, the thickness is about 1 micron to about 25 micron, such as about 10 micron to about 25 micron. In certain embodiments, the nanofiber mat has a thickness variation of less than 20%, less than 10%, less than 5% or the like [0108].
Table 1 discloses nanofiber diameters within the diameter range of at least claim 1. Smith teaches, in certain instances, a continuous material is a material that runs continuously along a length (such as from a few microns in length (e.g., >5 micron, >10 micron, >20 micron, or the like), to several microns in length, to the entire length of the fiber) of a nanofiber or nanofiber segment (e.g., at least 5% the length of the nanofiber, at least 10% the length of the nanofiber, at least 25% the length of the nanofiber, at least 50% the length of the nanofiber, at least 75% the length of the nanofiber, or the like), rather than being formed in isolated domains along or within the fiber. In some instances, a continuous material or matrix runs uninterrupted and/or without break along a length of a nanofiber or nanofiber segment herein. In certain instances, a continuous material or matrix is a high aspect ratio material, such as having an aspect ratio of at least 10, at least 20, at least 50, at least 100, at least 200, or the like (e.g., wherein the aspect ratio of the material is the length or the greatest longitudinal dimension divided by the diameter or the greatest lateral dimension) [0077].
Smith teaches a material (e.g., fiber) comprises a polymer matrix with a ceramic coating. The ceramic coating has any suitable thickness to impart a beneficial characteristic(s) to the material, such as one of the many described. In some embodiments, the material has a (e.g., average) thickness (e.g., diameter of a fiber), the polymer matrix (e.g., including any ceramic embedded therein) having a first thickness and the coating having a second thickness. In some instances, such as wherein a fiber is coated all the way around the fiber, a material has a polymer thickness, a first coating thickness and a second coating thickness. In some embodiments, the (e.g., average) thickness of a ceramic coating is about 30% or less of the (e.g., average) thickness of material (e.g., fiber). In specific embodiments, the (e.g., average) thickness of a ceramic coating is about 20% or less of the (e.g., average) thickness of material. In more specific embodiments, the (e.g., average) thickness of a ceramic coating is about 20% or less of the (e.g., average) thickness of material. In still more specific embodiments, the (e.g., average) thickness of a ceramic coating is about 15% or less of the (e.g., average) thickness of material. In yet more specific embodiments, the (e.g., average) thickness of a ceramic coating is about 8% to about 12% (e.g., about 10%) of the (e.g., average) thickness of material. In certain embodiments, the (e.g., average) thickness of the ceramic coating is at least 1% (e.g., at least 2%, at least 3%, at least 5%, or the like) of the overall (e.g., average) thickness of the material [0177].
The ceramic thickness of a shelled nanofiber or nanofiber segment is any suitable thickness. The average thickness of the shell is about 20% or less of the overall average diameter of the shelled nanofiber or segment thereof [0091]. See also [0095] and [0116-0117].
Thus, the claims are anticipated.
Regarding at least claims 2 and 4, any suitable polymer is utilized in the separators, membranes, fibers, mats, and the like described herein. In preferred embodiments, the polymer is a polymer compatible with one or more battery electrolyte, such as a lithium ion battery electrolyte. In certain embodiments, the polymer is polyvinyl alcohol (PVA), polyacrylonitrile (PAN), polyvinylidene difluoride (PVDF), polyvinylpyrrolidone (PVP), polyimide (PI), or a combination thereof. In specific embodiments, the polymer is PAN or PVDF [0178]. See also [0058-0072].
Regarding at least claims 3 and 4, any suitable ceramic is utilized in the separators, membranes, fibers, mats, and the like described herein. In certain embodiments, the ceramic is a precursor derived ceramic, such as a ceramic derived from a ceramic precursor that is liquid or soluble in or (e.g., at least partially) miscible with water, aqueous solutions, alcohol, dimethylformamide (DMF), combinations thereof, or the like. In certain embodiments, the ceramic is a silicon based ceramic, such as a silicon-oxycarbonnitride (SiCNO) ceramic, a silicon-oxycarbide (SiCO) ceramic, a silicon-carbonnitride (SiCN) ceramic, a silicon-oxynitride (SiNO) ceramic, a silicon oxide (SiOx) ceramic, a silicon nitride (SiNx) ceramic, a silicon carbide (SiCx) ceramic, combinations thereof, or the like [0197]. See also [0073-0074].
Regarding claims 9-10, the battery comprises a positive electrode, a negative electrode and a lithium ion battery electrolyte [0202]. The separator membrane is soaked with a battery electrode comprising 1 M LiPF6 in EC:DMC:DEC [0253]. See also [0198]. Regarding claim 11, the membrane has a porous structure with a porosity of about 10% to about 70% [0092; 0107]. Note also [0179-0196]. The polymer liquid medium comprises water, alcohol or a combination [0235].
Claim Rejections - 35 USC § 103
The following is a quotation of 35 U.S.C. 103 which forms the basis for all obviousness rejections set forth in this Office action:
A patent for a claimed invention may not be obtained, notwithstanding that the claimed invention is not identically disclosed as set forth in section 102, if the differences between the claimed invention and the prior art are such that the claimed invention as a whole would have been obvious before the effective filing date of the claimed invention to a person having ordinary skill in the art to which the claimed invention pertains. Patentability shall not be negated by the manner in which the invention was made.
Claim(s) 1-17 is/are rejected under 35 U.S.C. 103 as being unpatentable over Smith et al., US 2021/0167463 A1 in view of Joo et al., US 2019/0207186 A1.
Smith teaches polymer-ceramic hybrid membranes, as well as processes for manufacturing such membranes. In particular, polymer-ceramic hybrid membranes are non-flammable and thermally stable and may be used in batteries, such as lithium ion batteries [abstract].
Smith teaches a thermally stable, flame-resistant polymer-ceramic battery separator membrane. In specific embodiments, the separator membrane comprising a nanofiber mat, the nanofiber mat comprising one or more shelled nanofiber(s). In more specific embodiments, the one or more shelled nanofiber comprises a continuous core material and a continuous shell material (e.g., that runs along the entire length or a part of the length of the nanofiber), the continuous core material comprising a polymer, and the continuous shell material comprising a ceramic [0076-0079; 0129].
The nanofiber, nanofiber mats, separators, or other membranes may comprise a polyimide (glass transition temperature >300°C) and a ceramic (e.g., of a coated fiber mat and/or a ceramic-polymer hybrid fiber mat prepared directly from electrospinning a combination of polymer (e.g., polyimide) and ceramic precursor) being treated to a temperature of at least 250°C, more preferably, at least 275°C, and still more preferably about 300°C or more. As demonstrated in the examples, untreated products or products treated at lower temperatures have a greatly reduced resistance to flammability compared to those that are treated at higher temperatures [0097].
The membrane has any suitable thickness. The membrane (e.g., separator membrane) has an average thickness of about 1 micron to about 25 micron (e.g., about 5 micron to about 15 micron, or about 5 micron to about 10 micron). In preferred embodiments, the average thickness is about 8 to about 20 micron, such as about 12 to about 15 micron [0093]. The nanofiber mat or precursor membrane described herein comprising ceramic precursor and/or partially cured ceramic precursor can be thicker than a separator membrane described herein (e.g., as the membrane may be calendered to achieved the thickness desired in the separator membrane). The nanofiber mat or precursor membrane has a thickness of about 1 micron to about 50 micron, such as about 5 micron to about 50 micron or about 10 micron to about 50 micron. In some embodiments, the thickness is about 1 micron to about 25 micron, such as about 10 micron to about 25 micron. In certain embodiments, the nanofiber mat has a thickness variation of less than 20%, less than 10%, less than 5% or the like [0108].
Table 1 discloses nanofiber diameters within the diameter range of at least claim 1. Smith teaches, in certain instances, a continuous material is a material that runs continuously along a length (such as from a few microns in length (e.g., >5 micron, >10 micron, >20 micron, or the like), to several microns in length, to the entire length of the fiber) of a nanofiber or nanofiber segment (e.g., at least 5% the length of the nanofiber, at least 10% the length of the nanofiber, at least 25% the length of the nanofiber, at least 50% the length of the nanofiber, at least 75% the length of the nanofiber, or the like), rather than being formed in isolated domains along or within the fiber. In some instances, a continuous material or matrix runs uninterrupted and/or without break along a length of a nanofiber or nanofiber segment herein. In certain instances, a continuous material or matrix is a high aspect ratio material, such as having an aspect ratio of at least 10, at least 20, at least 50, at least 100, at least 200, or the like (e.g., wherein the aspect ratio of the material is the length or the greatest longitudinal dimension divided by the diameter or the greatest lateral dimension) [0077].
Smith teaches a material (e.g., fiber) comprises a polymer matrix with a ceramic coating. The ceramic coating has any suitable thickness to impart a beneficial characteristic(s) to the material, such as one of the many described. In some embodiments, the material has a (e.g., average) thickness (e.g., diameter of a fiber), the polymer matrix (e.g., including any ceramic embedded therein) having a first thickness and the coating having a second thickness. In some instances, such as wherein a fiber is coated all the way around the fiber, a material has a polymer thickness, a first coating thickness and a second coating thickness. In some embodiments, the (e.g., average) thickness of a ceramic coating is about 30% or less of the (e.g., average) thickness of material (e.g., fiber). In specific embodiments, the (e.g., average) thickness of a ceramic coating is about 20% or less of the (e.g., average) thickness of material. In more specific embodiments, the (e.g., average) thickness of a ceramic coating is about 20% or less of the (e.g., average) thickness of material. In still more specific embodiments, the (e.g., average) thickness of a ceramic coating is about 15% or less of the (e.g., average) thickness of material. In yet more specific embodiments, the (e.g., average) thickness of a ceramic coating is about 8% to about 12% (e.g., about 10%) of the (e.g., average) thickness of material. In certain embodiments, the (e.g., average) thickness of the ceramic coating is at least 1% (e.g., at least 2%, at least 3%, at least 5%, or the like) of the overall (e.g., average) thickness of the material [0177].
The ceramic thickness of a shelled nanofiber or nanofiber segment is any suitable thickness. The average thickness of the shell is about 20% or less of the overall average diameter of the shelled nanofiber or segment thereof [0091]. See also [0095] and [0116-0117].
Smith does not explicitly teach the ceramic coating may include the materials recited at least claim 5. However, Joo teaches a ceramic-polymer hybrid nanostructure wherein other materials may be admixed with the ceramic precursor and/or the polymer material such as surfactants, leveling agents, plasticizers and other materials known to be of benefit to fibers. Functional additives may also be added [0082]. In other embodiments metals may be included in the fluid stocks which provide conductivity or semi-conductivity, magnetic properties, piezoelectric properties and the like, to the nanofiber, such as, for example, carboxylate salts of Ag, Al, Co, Ni, Zn, Zr, Si, Cu, Fe, Pb, Au, Cd, Li, Ti, Mn, Cr, Be, Si, V, Hf, Sr, Ba, Ge and combination thereof. Oxides of various metals may be included, such as, for example, SiO2, Al2O3, V2O5, VO2, SnO, SnO2, CuO, NiO, B2O3, Na2O, K2O, CaO, Li2O, MgO, TiO2, ZnO, MnO, Fe2O3, CoO, CoO2, SrTiO3, BaSrTiO3, and combinations thereof. Metals with ligands, metal alloys, conductive materials and other materials may be included depending on the desired properties of the prepared morphologically controlled, ceramic-polymer nanofibers [0083]. Therefore, one of skill in the art at the time the invention was filed would have been motivated to include the other materials (metal oxides disclosed by Joo) admixed with the ceramic precursor and/or the polymer of Smith to provide benefits such as conductivity or semi-conductivity, magnetic properties, piezoelectric properties and the like, as taught by Joo. Both Smith and Joo are directed toward a ceramic-polymer hybrid material as a separator for batteries, particularly lithium ion batteries. See [0003; 0080; 0085] of Joo. Joo teaches other polymer materials such as polyethylene oxide and polyacrylonitrile [0052; 0080] may be included in the a ceramic-polymer hybrid nanostructure. Joo teaches the nanofibers may be from about 50 nm to about 2 microns in length and have an aspect ratio of above about 100. The aspect ratio is defined as the ratio between the length and the width of the material, so that, in a fiber, an aspect ratio of 100 means the length of the fiber is 100 times larger than the width of the fiber [0070]. Joo teaches the ceramic nanostructures have an average diameter of about 5 nm to about 50 nm, e.g., about 10 nm to about 40 nm [0080].
Regarding at least claims 2 and 4, Smith teaches any suitable polymer is utilized in the separators, membranes, fibers, mats, and the like described herein. In preferred embodiments, the polymer is a polymer compatible with one or more battery electrolyte, such as a lithium ion battery electrolyte. In certain embodiments, the polymer is polyvinyl alcohol (PVA), polyacrylonitrile (PAN), polyvinylidene difluoride (PVDF), polyvinylpyrrolidone (PVP), polyimide (PI), or a combination thereof. In specific embodiments, the polymer is PAN or PVDF [0178]. See also [0058-0072].
Regarding at least claims 3 and 4, Smith teaches any suitable ceramic is utilized in the separators, membranes, fibers, mats, and the like described herein. In certain embodiments, the ceramic is a precursor derived ceramic, such as a ceramic derived from a ceramic precursor that is liquid or soluble in or (e.g., at least partially) miscible with water, aqueous solutions, alcohol, dimethylformamide (DMF), combinations thereof, or the like. In certain embodiments, the ceramic is a silicon based ceramic, such as a silicon-oxycarbonnitride (SiCNO) ceramic, a silicon-oxycarbide (SiCO) ceramic, a silicon-carbonnitride (SiCN) ceramic, a silicon-oxynitride (SiNO) ceramic, a silicon oxide (SiOx) ceramic, a silicon nitride (SiNx) ceramic, a silicon carbide (SiCx) ceramic, combinations thereof, or the like [0197]. See also [0073-0074].
Regarding claims 9-10, Smith teaches the battery comprises a positive electrode, a negative electrode and a lithium ion battery electrolyte [0202]. The separator membrane is soaked with a battery electrode comprising 1 M LiPF6 in EC:DMC:DEC [0253]. See also [0198]. Regarding claim 11, the membrane has a porous structure with a porosity of about 10% to about 70% [0092; 0107]. Note also [0179-0196]. The polymer liquid medium comprises water, alcohol or a combination [0235].
Allowable Subject Matter
Claims 20, 21 and 23 would be allowable if rewritten to overcome the rejection(s) under 35 U.S.C. 112(b) or 35 U.S.C. 112 (pre-AIA ), 2nd paragraph, set forth in this Office action and to include all of the limitations of the base claim and any intervening claims. The specific method steps (A)-(E) are not taught or suggested by the prior art.
Conclusion
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/TRACY M DOVE/ Primary Examiner, Art Unit 1725