DETAILED ACTION
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 .
Priority
Receipt is acknowledged of certified copies of papers required by 37 CFR 1.55.
Information Disclosure Statement
The information disclosure statement (IDS) submitted on 10/28/2022 are in compliance with the provisions of 37 CFR 1.97. Accordingly, the information disclosure statements are being considered by the examiner.
Drawings
The drawings received on 10/28/2022 were reviewed and are acceptable.
Specification
The specification filed on 10/28/2022 was reviewed and is acceptable.
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.
Claim(s) 27 is/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 27 recites the limitation “the metal support” in line 3. There is insufficient antecedent basis for this limitation in the claim.
Claim Rejections - 35 USC § 102
In the event the determination of the status of the application as subject to AIA 35 U.S.C. 102 and 103 (or as subject to pre-AIA 35 U.S.C. 102 and 103) is incorrect, any correction of the statutory basis (i.e., changing from AIA to pre-AIA ) for the rejection will not be considered a new ground of rejection if the prior art relied upon, and the rationale supporting the rejection, would be the same under either status.
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.
(a)(2) the claimed invention was described in a patent issued under section 151, or in an application for patent published or deemed published under section 122(b), in which the patent or application, as the case may be, names another inventor and was effectively filed before the effective filing date of the claimed invention.
Claim(s) 12-13 is/are rejected under 35 U.S.C. 102(a)(1) as being anticipated by Lu et al. (“Effects of Fluorine Doping on Structural and Electrochemical Properties of Li6.25Ga0.25La3Zr2O12 as Electrolytes for Solid-State Lithium Batteries,” hereinafter Lu).
Regarding Claim 12, Lu discloses the limitations regarding a garnet-type inorganic compound based on the elements Li, La, Zr, A, O, wherein A denotes at least one element selected from the group consisting of Ga; (Lu, garnet-type solid electrolyte having the composition Li6.05Ga0.25La3Zr2O11.8F0.2, Table 1). The Examiner notes that Claim 12 is directed towards a garnet-type inorganic compounds, which is read upon by Lu, regardless of the process of claim 1. Thus, claim 12 is rejected based by Lu.
Regarding Claim 13, Lu discloses all of the claim limitations as set forth above. Lu discloses the limitations regarding an inorganic compound having a garnet-type structure based on the elements O, Li, Zr, A (Lu, garnet-type solid electrolyte having the composition Li6.05Ga0.25La3Zr2O11.8F0.2, Table 1), the relative proportions of which are those of the formula (I)
LixLa3ZrzAW (I)
wherein:
A denotes at least one element selected from the group consisting of Al, Ga, Nb, Fe, W and Ta;
x, z and w denote real numbers;
1.20 < z ≤ 2.10;
0 < w ≤ 0.80
4.00 ≤ x ≤ 10.50 (Lu, garnet-type solid electrolyte having the composition Li6.05Ga0.25La3Zr2O11.8F0.2, Table 1;
Li = Li, and x = 6.05, meeting the claimed range of 4.00 ≤ x ≤ 10.50;
La = La, and 3 = 3;
Zr = Zr, and z = 2, meeting the claimed range of 1.20 < z ≤ 2.10;
A = Ga, and w = 0.25, meeting the claimed range of 0 < w ≤ 0.80;
x, z, and w are all real numbers).
this compound also comprising the element F (Lu, garnet-type solid electrolyte having the composition Li6.05Ga0.25La3Zr2O11.8F0.2, Table 1).
With respect to the limitations the compound having at least one of the following characteristics:
a signal located between -125.0 and -129.0 ppm, on a (19F) solid- state NMR spectrum, the reference at δ=0 ppm being that of the compound CF3COH;
it is submitted that such limitations are simply measurements of, and thus descriptions of, inherent properties of the recited garnet-type solid electrolyte.
Applicant discloses a signal located between -125.0 and -129.0 ppm, on a (19F) solid- state NMR spectrum, the reference at δ=0 ppm being that of the compound CF3COH is generally attributed to a fluorine involved in an Li-F bond (see Instant Specification Page 13, lines 10-15).
Accordingly, it is reasonably interpreted that the fluorine involved in an Li-F bond is critical to the recited signal located between -125.0 and -129.0 ppm such that it would fulfil the recited measurements and necessarily possess the inherent properties.
Lu discloses atoms are more tightly bound in the fluorinated structure, and in the case of F, this may be more motion for Li motion, since the windows they have to cross are less impeded, as the thermal displacements of the anionic sublattice is significantly smaller and is more favorable for Li diffusion (Lu, Page 2045-2046, paragraph starting with “The unit-cell parameter…”).
It is submitted that the garnet-type solid electrolyte of Lu is substantially similar to the instant inorganic compound such that the garnet-type solid electrolyte of Lu would reasonably possess the same properties and exhibit the same results.
Therefore, based upon such substantial similarities, it appears reasonable that the garnet-type solid electrolyte of Lu would inherently possess physical properties, e.g. a signal located between -125.0 and -129.0 ppm, on a (19F) solid- state NMR spectrum, the reference at δ=0 ppm being that of the compound CF3COH, such that the garnet-type solid electrolyte of Lu would necessarily fulfill the recited limitations, i.e. a signal located between -125.0 and -129.0 ppm, on a (19F) solid- state NMR spectrum, the reference at δ=0 ppm being that of the compound CF3COH.
Assuming, arguendo, that such properties are not inherent, it is submitted that before the effective filing date of the current invention, one having ordinary skill in the art would find such properties obvious over the claimed inorganic compound. The skilled artisan would reasonably find that the disclosed garnet-type solid electrolyte of Lu is so similar to the instant inorganic compound that the prior art garnet-type solid electrolyte would also exhibit a signal located between -125.0 and -129.0 ppm, on a (19F) solid- state NMR spectrum, the reference at δ=0 ppm being that of the compound CF3COH.
Regarding Claims 16-17, Lu discloses all of the claim limitations as set forth above. Lu discloses the limitations regarding an inorganic compound (Lu, garnet-type solid electrolyte having the composition Li6.05Ga0.25La3Zr2O11.8F0.2, Table 1), the crystalline structure of which consists of a skeleton of LaO8 dodecahedra (La of coordination number 8) (Claim 16), and more specifically 24c site (Claim 17) (Lu, La are located at 24c (1/8, 0, ¼) sites, Page 2045, paragraph starting with “To reveal the effects of doping F…”) and
of ZrO6 octahedra (Zr of coordination number 6) (Claim 16), and more specifically 16a site (Claim 17) (Lu, Zr at 16a (0, 0, 0), Page 2045, paragraph starting with “To reveal the effects of doping F…”).
Regarding Claim 18, Lu discloses all of the claim limitations as set forth above. Lu discloses the limitations regarding an inorganic compound (Lu, garnet-type solid electrolyte having the composition Li6.05Ga0.25La3Zr2O11.8F0.2, Table 1), wherein some Li atoms are present at the 24d tetrahedral sites or 48g and 96h octahedral sites (Lu, Li1 atoms were located at 24d (3/8, 0, 1/4) sites and Li2 at 96h (x, y, z) positions, Page 2045, paragraph starting with “To reveal the effects of doping F…”).
Regarding Claim 19, Lu discloses all of the claim limitations as set forth above. Lu discloses the limitations regarding an inorganic compound (Lu, garnet-type solid electrolyte having the composition Li6.05Ga0.25La3Zr2O11.8F0.2, Table 1), comprising La-F and/or Zr-F bonds (Lu, it seems that the introduction of 1.67% of F in the anionic sublattice gives rise to stronger La-(O,F) and Zr-(-F) chemical bonds, even if a more ionic character could be forecasted from the higher electronegativity of F versus O, Page 2045-2047, paragraph starting with “The unit-cell parameter…”).
Regarding Claim 20, Lu discloses all of the claim limitations as set forth above. Lu discloses the limitations regarding an inorganic compound (Lu, garnet-type solid electrolyte having the composition Li6.05Ga0.25La3Zr2O11.8F0.2, Table 1).
With respect to the limitations the compound having at least one of the following characteristics:
having, by (19F) solid-state NMR spectroscopy, the reference at δ=0 ppm being that of the compound CF3COOH, a signal between -98.0 and -102.0 ppm, and/or a signal between - 58.0 and -62.0 ppm,
it is submitted that such limitations are simply measurements of, and thus descriptions of, inherent properties of the recited garnet-type solid electrolyte.
Applicant discloses a signal between -98.0 and -102.0 ppm, and/or a signal between - 58.0 and -62.0 ppm, on a (19F) solid-state NMR spectrum, the reference at δ=0 ppm being that of the compound CF3COH is generally attributed to the formation of La-F and Zr-F bonds, respectively (see Instant Specification Page 13, lines 23-29).
Accordingly, it is reasonably interpreted that the presence of La-F and Zr-F bonds are critical to the recited signal located between -98.0 and -102.0 ppm, and/or a signal between - 58.0 and -62.0 ppm such that it would fulfil the recited measurements and necessarily possess the inherent properties.
Lu discloses that the introduction of 1.67% of F in the anionic sublattice gives rise to stronger La-(O,F) and Zr-(-F) chemical bonds, even if a more ionic character could be forecasted from the higher electronegativity of F versus O (Lu, Page 2045-2047, paragraph starting with “The unit-cell parameter…”).
It is submitted that the garnet-type solid electrolyte of Lu is substantially similar to the instant inorganic compound such that the garnet-type solid electrolyte of Lu would reasonably possess the same properties and exhibit the same results.
Therefore, based upon such substantial similarities, it appears reasonable that the garnet-type solid electrolyte of Lu would inherently possess physical properties, e.g. a signal located between -125.0 and -129.0 ppm, on a (19F) solid- state NMR spectrum, the reference at δ=0 ppm being that of the compound CF3COH, such that the garnet-type solid electrolyte of Lu would necessarily fulfill the recited limitations, i.e. a signal between -98.0 and -102.0 ppm, and/or a signal between -58.0 and -62.0 ppm, on a (19F) solid- state NMR spectrum, the reference at δ=0 ppm being that of the compound CF3COH.
Assuming, arguendo, that such properties are not inherent, it is submitted that before the effective filing date of the current invention, one having ordinary skill in the art would find such properties obvious over the claimed inorganic compound. The skilled artisan would reasonably find that the disclosed garnet-type solid electrolyte of Lu is so similar to the instant inorganic compound that the prior art garnet-type solid electrolyte would also exhibit a signal between -98.0 and -102.0 ppm, and/or a signal between - 58.0 and -62.0 ppm, on a (19F) solid- state NMR spectrum, the reference at δ=0 ppm being that of the compound CF3COH.
Regarding Claim 21, Lu discloses all of the claim limitations as set forth above. Lu discloses the limitations regarding an inorganic compound (Lu, garnet-type solid electrolyte having the composition Li6.05Ga0.25La3Zr2O11.8F0.2, Table 1), of which the proportion of fluorine in the compound expressed by weight of the element fluorine relative to the total weight, is less than or equal to 10.0% and is greater than or equal to 0.01% (Lu, it seems that the introduction of 1.67% of F in the anionic sublattice gives rise to stronger La-(O,F) and Zr-(-F) chemical bonds, even if a more ionic character could be forecasted from the higher electronegativity of F versus O, Page 2045-2047, paragraph starting with “The unit-cell parameter…”; the disclosed F amount of 1.67% falls within the claimed range of 0.01% to 10%)
Regarding Claims 23-24, Lu discloses all of the claim limitations as set forth above. Lu discloses the limitations regarding an inorganic compound (Lu, garnet-type solid electrolyte having the composition Li6.05Ga0.25La3Zr2O11.8F0.2, Table 1), having a cubic crystal structure (Claim 23), and more specifically, the crystal structure belongs to the Ia3̅d space group (Claim 24) (Lu, it can be concluded that the F anions are successfully doped into LLZO lattice, and dense garnet type pellets are obtained with the same Ia3̅d structure, Page 2044-2045, Paragraph starting with “To gain insight…”).
Regarding Claims 25-26, Lu discloses all of the claim limitations as set forth above. Lu discloses the limitations regarding an inorganic compound (Lu, garnet-type solid electrolyte having the composition Li6.05Ga0.25La3Zr2O11.8F0.2, Table 1)
With respect to the limitations the compound having at least one of the following characteristics:
having a ratio R less than or equal to 50%, R being the ratio between the intensity of the vibrational band of the C-O bond of the carbonate groups (symmetric stretching v) located around 1090 cm-1 to the intensity of the stretching band of the bonds in the ZrO6 octahedra located around 648 cm-1, these two intensities being determined by Raman spectroscopy and R being determined after storing the inorganic compound in an air-filled sealed flask for a period of at least two months, in particular of two months (Claim 25);
characterized in that the intensity of the vibrational mode v3 and/or of the vibrational mode v2 of the carbonate groups, these modes being respectively located between 1350 and 1600 cm-1 and between 890 and 1350 cm-1, is less than or equal to 50%, this intensity being determined by infrared spectroscopy in total attenuated reflectance mode (Claim 26),
it is submitted that such limitations are simply measurements of, and thus descriptions of, inherent properties of the recited garnet-type solid electrolyte.
Applicant discloses that it is generally considered that the C-O vibrational band of the carbonate groups is located at 1090±20 cm-1. This band is generally located between 1080 and 1100 cm-1 (see Instant Specification Page 14, lines 6-9). Further, Applicant discloses that it is observed that the fluorination process has the effect of reducing the amount of carbonate groups which are present, in particular at the surface of the solid, or even of making them disappear (see Instant Specification Page 16, lines 22-28).
Accordingly, it is reasonably interpreted that Applicant is directed towards minimizing the intensity of the C-O vibrational bands, and making the carbonate group disappear is desirable, such that it would fulfil the recited measurements and necessarily possess the inherent properties.
Lu discloses that as observed from the high quality of XRD patterns, no impurity phases, such as Li2CO3, especially F contained compounds, were detected under the limitation of XRD instrument (Lu, Page 2044, paragraph starting with “The crystal structures…”). The Examiner notes that since Li2CO3 was not present in the garnet of Lu, so the claimed ratio R (Claim 25) and the carbonate vibrational band intensity (Claim 26) would be 0%, which falls within the claimed range of less than or equal to 50%.
It is submitted that the garnet-type solid electrolyte of Lu is substantially similar to the instant inorganic compound such that the garnet-type solid electrolyte of Lu would reasonably possess the same properties and exhibit the same results. Therefore, based upon such substantial similarities, it appears reasonable that the garnet-type solid electrolyte of Lu would inherently possess physical properties, e.g.
having a ratio R less than or equal to 50%, R being the ratio between the intensity of the vibrational band of the C-O bond of the carbonate groups (symmetric stretching v) located around 1090 cm-1 to the intensity of the stretching band of the bonds in the ZrO6 octahedra located around 648 cm-1, these two intensities being determined by Raman spectroscopy and R being determined after storing the inorganic compound in an air-filled sealed flask for a period of at least two months, in particular of two months (Claim 25);
characterized in that the intensity of the vibrational mode v3 and/or of the vibrational mode v2 of the carbonate groups, these modes being respectively located between 1350 and 1600 cm-1 and between 890 and 1350 cm-1, is less than or equal to 50%, this intensity being determined by infrared spectroscopy in total attenuated reflectance mode (Claim 26),
such that the garnet-type solid electrolyte of Lu would necessarily fulfill the recited limitations, i.e.
having a ratio R less than or equal to 50%, R being the ratio between the intensity of the vibrational band of the C-O bond of the carbonate groups (symmetric stretching v) located around 1090 cm-1 to the intensity of the stretching band of the bonds in the ZrO6 octahedra located around 648 cm-1, these two intensities being determined by Raman spectroscopy and R being determined after storing the inorganic compound in an air-filled sealed flask for a period of at least two months, in particular of two months (Claim 25);
characterized in that the intensity of the vibrational mode v3 and/or of the vibrational mode v2 of the carbonate groups, these modes being respectively located between 1350 and 1600 cm-1 and between 890 and 1350 cm-1, is less than or equal to 50%, this intensity being determined by infrared spectroscopy in total attenuated reflectance mode (Claim 26).
Assuming, arguendo, that such properties are not inherent, it is submitted that before the effective filing date of the current invention, one having ordinary skill in the art would find such properties obvious over the claimed inorganic compound. The skilled artisan would reasonably find that the disclosed garnet-type solid electrolyte of Lu is so similar to the instant inorganic compound that the prior art garnet-type solid electrolyte would also exhibit
having a ratio R less than or equal to 50%, R being the ratio between the intensity of the vibrational band of the C-O bond of the carbonate groups (symmetric stretching v) located around 1090 cm-1 to the intensity of the stretching band of the bonds in the ZrO6 octahedra located around 648 cm-1, these two intensities being determined by Raman spectroscopy and R being determined after storing the inorganic compound in an air-filled sealed flask for a period of at least two months, in particular of two months (Claim 25);
characterized in that the intensity of the vibrational mode v3 and/or of the vibrational mode v2 of the carbonate groups, these modes being respectively located between 1350 and 1600 cm-1 and between 890 and 1350 cm-1, is less than or equal to 50%, this intensity being determined by infrared spectroscopy in total attenuated reflectance mode (Claim 26).
Regarding Claim 28, Lu discloses all of the claim limitations as set forth above. Lu discloses the limitations regarding an inorganic compound (Lu, garnet-type solid electrolyte having the composition Li6.05Ga0.25La3Zr2O11.8F0.2, Table 1), a solid electrolyte of a lithium ion battery comprising the inorganic compound (Lu, both sides of the ceramic electrolyte were coated with a solid polymer electrolyte, and the electrochemical behaviors of the electrolytes were measured by using CR2032 coin cells, Page 2044, Paragraph starting with “The electrochemical behaviors…”)
Claim Rejections - 35 USC § 103
In the event the determination of the status of the application as subject to AIA 35 U.S.C. 102 and 103 (or as subject to pre-AIA 35 U.S.C. 102 and 103) is incorrect, any correction of the statutory basis (i.e., changing from AIA to pre-AIA ) for the rejection will not be considered a new ground of rejection if the prior art relied upon, and the rationale supporting the rejection, would be the same under either status.
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.
The factual inquiries for establishing a background for determining obviousness under 35 U.S.C. 103 are summarized as follows:
1. Determining the scope and contents of the prior art.
2. Ascertaining the differences between the prior art and the claims at issue.
3. Resolving the level of ordinary skill in the pertinent art.
4. Considering objective evidence present in the application indicating obviousness or nonobviousness.
This application currently names joint inventors. In considering patentability of the claims the examiner presumes that the subject matter of the various claims was commonly owned as of the effective filing date of the claimed invention(s) absent any evidence to the contrary. Applicant is advised of the obligation under 37 CFR 1.56 to point out the inventor and effective filing dates of each claim that was not commonly owned as of the effective filing date of the later invention in order for the examiner to consider the applicability of 35 U.S.C. 102(b)(2)(C) for any potential 35 U.S.C. 102(a)(2) prior art against the later invention.
Claim(s) 3 is/are rejected under 35 U.S.C. 103 as being unpatentable over Liu et al. (US 20150118571 A1, hereinafter Liu), as evidenced by Neuber et al. (US 20110023908 A1, hereinafter Neuber).
Regarding Claim 3, Liu discloses the limitations regarding a fluorination process comprising bringing an atmosphere comprising difluorine gas (Liu, the precursor compounds can include one or more fluorine salts as a source of fluorine, wherein LiF or CaF2 may be used, [0009]) into contact with the oxide (Liu, lithium garnet-type oxide ceramics with the incorporation of fluorine, which may act as a sintering aid and promotes the formation of the cubic garnet phase, [0020]) of formula (II): [Lix1La3ZrzAWO12] (II) wherein:
A denotes at least one element selected from the group consisting of Al, Ga, Nb, Fe, W and Ta;
x1, z and w denote real numbers;
1.20 < z ≤ 2.10;
0 < w ≤ 0.80;
x1 is a positive real number which is such that the electroneutrality of the oxide is ensured (Liu, a cation-doped garnet-type oxide represented by the formula Li6.75La3Zr1.75Nb0.25O12 – 24 mol% LiF, and CaF2 may be used in place of LiF, [046-0048];
Li = Li, and x1 = 6.25, x1 is a positive real number which is such that the electroneutrality of the oxide is ensured;
La = La, and 3 = 3;
Zr = Zr, and z = 1.75, meeting the claimed range of 1.20 < z ≤ 2.10;
A = Nb, and w = 0.25, meeting the claimed range of 0 < w ≤ 0.80;
O = O, and 12 = 12).
Liu discloses that fluorine may be added to the lithium garnet-type oxide ceramic through the form of a fluoride salt, such as LiF or CaF2 (Liu, [0020]). Further, Liu discloses an example where a garnet-type oxide was prepared wherein CaF2 was used in place of LiF (Liu, [0046]).
Therefore, it would have been obvious to one of ordinary skill in the art before the effective filing date of the invention to recognize that LiF and CaF2 are obvious substitutions, and it would be obvious to try to use CaF2 instead of LiF when preparing a cation-doped garnet-type oxide represented by Li6.75La3Zr1.75Nb0.25O12 – 24 mol% LiF.
It is evidenced by Neuber that CaF2, as a high surface area solid can be used to form F2. Specifically, high surface area pellets of the CaF2 may be dried, such as by a dryer, and then fed to a controlled high temperature furnace to control the rate of F2 evolved from the CaF2 (Neuber, [0037]).
Liu discloses that starting materials including Li2CO3, La2O3, ZrO2, and LiF (which can be substituted for CaF2, as noted above) were mixed, dried, then calcined in an alumina crucible at 900 °C (Liu, [0037-0046]). Since the processes of Neuber and Liu are similar, one of ordinary skill in the art would recognize that the CaF2 of Liu formed F2, or an atmosphere comprising difluorine gas, as claimed.
Claim(s) 14 is/are rejected under 35 U.S.C. 103 as being unpatentable over Lu et al. (“Effects of Fluorine Doping on Structural and Electrochemical Properties of Li6.25Ga0.25La3Zr2O12 as Electrolytes for Solid-State Lithium Batteries,” hereinafter Lu), as applied to Claim 13 above, and further in view of Liu et al. (US 20150118571 A1, hereinafter Liu)
Regarding claim 14, Lu discloses all of the claim limitations as set forth above. Lu discloses the limitations regarding an inorganic compound (Lu, garnet-type solid electrolyte having the composition Li6.05Ga0.25La3Zr2O11.8F0.2, Table 1). Lu is silent regarding the element zirconium is partially replaced by the element hafnium.
Liu discloses an inorganic compound (Liu, lithium garnet-type oxide ceramics, generally represented by the formula Li7La3Zr2O12 with z mol % F, where 0 < z < 40, [0020]), wherein the element zirconium is partially replaced by the element hafnium (Liu, the oxide ceramics may comprise one or more cation (M) dopants, which includes Hf, which may be incorporated into the crystal lattice onto one or more of a Zr site, [0024]).
Liu teaches that doping may result in the lithium garnet-type oxide ceramic to exhibit a unique microstructure which can contribute to a higher ionic conductivity and achievable hermeticity in solid membranes (Liu, [0021]).
Lu and Liu are analogous to the current invention as they are all directed towards lithium garnet-type ceramics with fluoride.
Therefore, it would have been obvious to one of ordinary skill in the art before the effective filing date of the invention for the garnet-type solid electrolyte of Lu to incorporate Hf into the crystal lattice onto one or more of a Zr site, as taught by Liu, in order to achieve a higher ionic conductivity.
Claim(s) 27 and 29 is/are rejected under 35 U.S.C. 103 as being unpatentable over Lu et al. (“Effects of Fluorine Doping on Structural and Electrochemical Properties of Li6.25Ga0.25La3Zr2O12 as Electrolytes for Solid-State Lithium Batteries,” hereinafter Lu), as applied to Claim 12 above, and further in view of Engel et al. (US 20150295274 A1, hereinafter Engel)
Regarding Claim 27, Lu discloses the limitations regarding an inorganic compound (Lu, garnet-type solid electrolyte having the composition Li6.05Ga0.25La3Zr2O11.8F0.2, Table 1). Lu is silent regarding an electrode E comprising:
a metal support;
a layer of a composition (C) in contact with the metal substrate, said composition (C) comprising:
the inorganic compound
at least one electroactive compound (EAC);
optionally at least one material which conducts the Li ions other than the fluorinated oxide (LiCM);
optionally at least one electrically-conductive material (ECM),
optionally a lithium salt (LIS); and
optionally at least one polymer binder material (P).
Engel discloses an electrode E (Engel, battery cell comprising a cathode, Claim 12) comprising:
a metal support (Engel, cathode current collector is an aluminum film, [0020]);
a layer of a composition (C) in contact with the metal substrate, said composition (C) comprising:
the inorganic compound (Engel, garnet with cathode active material, the garnet serving as an ion conductor, [0065])
at least one electroactive compound (EAC) (Engel, the cathode active material is selected from a lithiated transition metal oxide, which is selected from Li(NiCoMn)O2, [0026]);
optionally at least one electrically-conductive material (ECM) (Engel, the cathode can furthermore encompass additives to improve conductivity, such as conductive carbon black, [0066]), and
optionally at least one polymer binder material (P) (Engel, the cathode may include a binder such as PVdF (polyvinylidene fluoride, [0024]).
Engel discloses that garnet can improve ion conductivity of a cathode (Engel, [0065]).
Lu and Engel are analogous to the current invention as they are all directed towards usage of a garnet in a battery.
Therefore, it would have been obvious to one of ordinary skill in the art before the effective filing date of the invention for the battery of Lu to include the cathode of Engel and to use the garnet of Lu as the ion conductor of the cathode, in order to improve the ion conductivity of the cathode.
Regarding Claim 29, modified Lu discloses the limitations regarding a method of preparing a lithium battery (Lu, cell assembly, Page 2044, Paragraph starting with “The electrochemical behaviors…”), the method comprising: preparing an electrode comprising the inorganic compound (Engel, garnet with cathode active material, and the garnet serving as an ion conductor, [0065]).
Allowable Subject Matter
Claims 1-2, and 4 are allowable.
The following is a statement of reasons for the indication of allowable subject matter:
The present invention is related to a fluorination process comprising:
(Claim 1), bringing an atmosphere comprising difluorine gas into contact with an inorganic compound M having a garnet-type structure, which is based on the elements Li, La, Zr, A and O and for which the relative composition of the Li, La, Zr and A cations corresponds to the formula (I): LixLa3ZrzAW (I) wherein:
A denotes at least one element selected from the group consisting of Al, Ga, Nb, Fe, W and Ta;
x, z and w denote real numbers;
1.20 < z ≤ 2.10;
0 < w ≤ 0.80;
4.00 ≤ x ≤ 10.50;
the duration of the contact between the solid and the fluorinated atmosphere is between 2 minutes and 4 hours; and
the temperature at which the fluorination is carried out is between 20°C and 300°C.
Liu et al. (US 20150118571 A1, hereinafter Liu) is considered to be the closest relevant prior art to independent claim 1. Liu discloses most of the claim limitations as set forth above.
However, Liu does not disclose, teach, fairly suggest, nor render obvious the above noted limitations for the following reasons:
(Claim 1) Liu discloses that a mixture comprising of Li2CO3, La2O3, ZrO2, and LiF (which can be substituted for CaF2, as noted above) were dried, calcined in an alumina crucible at 900 °C in air for 12 h, and then cooled down to 25 °C (Liu, [0037-0046]). Thus, there does not appear to be any reasonable basis for the skilled artisan to be directed towards the duration of the contact between the solid and the fluorinated atmosphere is between 2 minutes and 4 hours; and the temperature at which the fluorination is carried out is between 20°C and 300°C.
Conclusion
Any inquiry concerning this communication or earlier communications from the examiner should be directed to KEVIN NGUYEN whose telephone number is (703)756-1745. The examiner can normally be reached Monday-Thursday 9:50 - 7:50 ET.
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/K.N./Examiner, Art Unit 1752
/NICHOLAS A SMITH/Supervisory Primary Examiner, Art Unit 1752