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 .
Response to Amendment
This is a final Office action in response to Applicant’s remarks and amendments filed on 06/18/2026. Claims 1, 3 and 13 are amended. Claims 6 and 7 are canceled. Claims 1, 3 – 5, 8- 13, and 18 are pending in the current Office action.
The 35 U.S.C 103 rejections set forth in the previous Office action are withdrawn. A new grounds of rejection, necessitated by applicants amendment, is presented below.
Response to Arguments
Applicant’s arguments with respect to claim(s) 1 and 13 have been considered but are moot because the arguments do not apply to the combination of references used in the current rejection. Specifically, in addition to the previously cited art, the new grounds of rejection relies on a new teaching reference: Zhou et al. (Solvent-engineered design of argyrodite Li6PS5X (X= Cl, Br, I) solid electrolytes with high ionic conductivity. ACS Energy Letters, 4(1), pp.265-270) to address the new limitation.
Claim Objections
Claims 11 – 12 are objected to because of the following informalities: By reciting “the halide-containing crystalline argyrodite” it is unclear which of the claimed halide-containing crystalline lithium argyrodites established in claim 1 is being further limited by claims 11 and 12. That is claim 1 appears to claim the solid electrolyte comprising a solid, halide-containing crystalline argyrodite and a halide-containing crystalline argyrodite structure represented as xLiX·Li6PS5X . Appropriate correction is required. For the purpose of this Office action, the examiner is interpreting “the halide-containing crystalline argyrodite” to mean the solid, halide-containing crystalline argyrodite which is an interpretation that appears to be supported by [0139];[0156] of the instant specification.
Claim Rejections - 35 USC § 112
The following is a quotation of the first paragraph of 35 U.S.C. 112(a):
(a) IN GENERAL.—The specification shall contain a written description of the invention, and of the manner and process of making and using it, in such full, clear, concise, and exact terms as to enable any person skilled in the art to which it pertains, or with which it is most nearly connected, to make and use the same, and shall set forth the best mode contemplated by the inventor or joint inventor of carrying out the invention.
The following is a quotation of the first paragraph of pre-AIA 35 U.S.C. 112:
The specification shall contain a written description of the invention, and of the manner and process of making and using it, in such full, clear, concise, and exact terms as to enable any person skilled in the art to which it pertains, or with which it is most nearly connected, to make and use the same, and shall set forth the best mode contemplated by the inventor of carrying out his invention.
Claims 1, 3 – 5, 8 – 13, and 18 rejected under 35 U.S.C. 112(a) or 35 U.S.C. 112 (pre-AIA ), first paragraph, as failing to comply with the written description requirement. The claim(s) contains subject matter which was not described in the specification in such a way as to reasonably convey to one skilled in the relevant art that the inventor or a joint inventor, or for applications subject to pre-AIA 35 U.S.C. 112, the inventor(s), at the time the application was filed, had possession of the claimed invention.
Specifically, Claims 1 and 13 recite “wherein the interphase layer comprises a uniform distribution of P, S, and X”. Applicant has indicated (Remarks Pg. 7) that support for the amendments can be found in [0127], [0132] and [0174] of the instant specification. Examiner notes that although [0127] provides support for “a uniform distribution of P, S, and X”; there does not seem to be support in the instant specification for the interphase layer to comprise the uniform distribution of P, S, and X. That is the subject matter of cited section of the instant specification are directed to the atomic structure/distribution within the Li6PS5X electrolyte NOT the interphase layer, e.g. [0127] recites “In addition, the EDX maps of the Li6PSSX {emphasis added} (see Fig. 23) show uniform distribution of P, S, and X (Cl, Br, and I) atoms, suggesting a homogeneity in the final product after the liquid synthesis method…”; [0132] recites “…due to the distribution of disorder of CI ions over the 4a and 4c sites together, which provides both high Li* intercage jump rates and doublet jump rates in the Li6PS5CI structure {emphasis added}”. The examiner further notes that [0174] recites “The elemental mapping images of the cross-section {emphasis added} by EDS illustrated in FIG. 42 [panel (e)], demonstrate the uniform distribution of phosphorous (P), sulfur (S) and chloride (Cl), which indicates that adding PC only influences the surface and the majority of Li6PS5Cl—LiCl remains unchanged”. With respect to the additional support recited by the applicant {i.e. Figs. 45 and 54 and [0186] of the instant specification}, the examiner notes that, with respect to the interphase layer and figure 45, figure 54 and [0086], based on the recitation “shows the detailed XPS spectra and peak fits of S 2p, C 1s, and O1s obtained from the SE of the LTO∥Li6PS5Cl—LiCl/PC-III∥Li cell before (top) and after cycling (bottom)” data of the figures also do not appear to be specific to the interphase layer {i.e. instead directed to SE as a whole} and thus also does not appear to provide support for the claimed limitation “wherein the interphase layer comprises a uniform distribution of P, S, and X”. Therefore, this limitation is interpreted as introducing new matter.
Claims, 3 – 5, 8 – 12, and 18 are also rejected for introducing new matter due to their dependency on independent claim 1.
Claim Rejections - 35 USC § 103
The text of those sections of Title 35, U.S. Code not included in this action can be found in a prior Office action.
Claim(s) 1, 3 – 5, 8 – 13, and 18 are rejected under 35 U.S.C. 103 as being unpatentable over An (CN107394272A – cited in previous Office action mailed 12/12/2024) in view of Utsuno (WO 2018/092366 A1, US PG Pub. 2019/0319305 A1 used as English translation – cited in previous Office action mailed 12/12/2024) and Zhou (Solvent-engineered design of argyrodite Li6PS5X (X= Cl, Br, I) solid electrolytes with high ionic conductivity. ACS Energy Letters, 4(1), pp.265-270, annotated NPL provided).
Regarding Claims 1, 11 – 12 and 18, An discloses an electrochemical energy storage device (solid-state lithium ion battery; [0010]) comprising a solid electrolyte ([0010];[0015]) and a wetting agent (organic solvent; [0010 – 0012]).
The organic solvent disclosed by An reads on the claimed wetting agent, because, like the claimed wetting agent, the organic solvent functions to reduce contact impedance between the electrolyte and electrode in the battery and ultimately allow for improved performance of the solid-state lithium ion battery (An: [0022]; Instant Specification: [0164 – 0165]). Furthermore, materials listed/exemplified to be used as the organic solvent in An, such propylene carbonate, are claimed and disclosed by the applicant to be wetting agents (An: [0022];[0046 – 0050]; Instant Specification: [0164]).
In Example 1 of An, the organic solvent is propylene carbonate and the solid electrolyte is a solid polymer electrolyte composed of polyethylene carbonate, poly(vinylidene fluoride-hexafluoropropylene), and lithium bis (trifluoromethylsulfonyl imide) ([0046]). The negative electrode of the example battery is a lithium metal electrode and the positive electrode is a lithium iron phosphate electrode ([0047 – 0048]).
As an alternative to polymer electrolytes, An also teaches using inorganic solid electrolytes for the solid-state lithium ion battery ([0015]). Inorganic solid electrolytes taught by An include materials such as Li7La3ZrO12, Li10GeP2S12, Li3OCl0.5Br0.5, Li3xLa(2/3)-xTiO3, Li5La3Ta2O12, Li5La3Nb2O12, Li5.5La3Nb1.74In0.25O12, Li3N-LiCl, Li3N-LiBr, Li3N-LiI, Li14Zn(GeO4)4, LiZr2(PO4)3, Li3OCl, LiPON, and Li2S-MaSb wherein 0.04 < x < 0.14, M = Al, Si, or P, and the values of a and b are 1 – 3, respectively.
An does not explicitly disclose wherein the solid electrolyte composition comprises a solid, halide-crystalline lithium argyrodite represented as xLiX·Li6PS5X wherein X is a halide or wherein the halide-containing crystalline lithium argyrodite is represented by a formula chosen from the group consisting of LimPSnXo and LimPSn, where m is a number in the range of 4-8, n is a number in the range of 3-6, X represents at least one halide, and o is a number in the range of 0-3 (Claim 11).
Utsuno, also directed to solid-state lithium ion batteries ([0130 – 0131]), teaches a sulfide solid electrolyte with an argyrodite-crystal structure represented by LiaPSbClc wherein 5.0 ≤ a ≤ 6.5, 6.1 ≤ a + c ≤ 7.5 {i.e. 0.4 ≤ c ≤ 2.5}, 0.5 ≤ a - b ≤ 1.5 {i.e. 3.5 ≤ b ≤ 6}, b > 0, and c > 1.0 are satisfied ([0035];[0055 – 0057]). Utsuno further teaches that the electrolyte material has improved ion conductivity due to the inclusion of chlorine, and is compatible with negative electrodes including elemental metals like metal lithium and positive electrodes including transition metal oxides like LiFePO4 ([0015];[0026];[0107];[0122]).
Since An already teaches using inorganic sulfide solid electrolytes that include Li, S, and P, it would have been obvious to one with ordinary skill in the art, before the effective filing date of the claimed invention, to modify the battery of Example 1, to include the sulfide solid electrolyte taught by Utsuno, and thus obtain a solid electrolyte composition that comprises a solid, halide-containing crystalline lithium argyrodite, with a reasonable expectation of success in obtaining a solid electrolyte with improved conductivity and suitable for An’s solid-state lithium ion battery.
By including a sulfide solid electrolyte represented by LiaPSbClc wherein 5.0 ≤ a ≤ 6.5, 6.1 ≤ a + c ≤ 7.5 {i.e. 0.4 ≤ c ≤ 2.5}, 0.5 ≤ a - b ≤ 1.5 {i.e. 3.5 ≤ b ≤ 6}, b > 0, and c > 1.0 are satisfied (Utsuno: [0035];[0055 – 0057]), modified An’s solid electrolyte composition includes halide-containing crystalline lithium argyrodites such as Li6PS5Cl·0.5LiCl and Li6PS5Cl. Therefore, modified An includes within its scope halide-containing crystalline lithium argyrodites having a chloride content overlapping the claimed chloride content range expressed as Li6PS5Cl·xLiCl where x is 0 – 2 (Claim 12); halide-containing crystalline lithium argyrodites represented as xLiX·Li6PS5X wherein X is a halide (Claim 1 cont.); and further provides halide-containing crystalline lithium argyrodites represented by LimPSnXo, where m is 5 – 6.5, which is within the claimed range of 4 – 8, n is 3.5 – 6, which is within the claimed range of 3 – 6, X represents at least one halide {i.e. Cl}, and o is 0.4 to 2.5 which is within the claimed range of 0 – 3 (Claim 11) and further overlaps the claimed range of 0.5 – 3 inclusive of end points (Claim 18).
Utsuno’s taught ranges for the molar ratios of Li, S, and Cl in LiaPSbClc provide the advantageous effects of stable crystal structure and improved ion conductivity ([0005];[0026];[0047 – 0053]). Furthermore, Utsuno teaches that increasing the Cl content reduces the lattice constant of the argyrodite crystal structure and ultimately allows for improvements in ion conductivity ([0026]).
Therefore, selection of halide-containing crystalline lithium argyrodites with chloride contents within the overlapping portion of the taught range and the claimed range, such as Li6PS5Cl·0.5LiCl {x = 0.5} and o = 0.5 – 2.5, would have been obvious to one with ordinary skill in the art to optimize the crystal structure and conductivity of the sulfide solid electrolyte material of modified An, with a reasonable expectation of success and without undue experimentation [MPEP 2144.05(II)].
Modified An does not explicitly disclose the halide-containing crystalline lithium argyrodite forming a solid electrolyte, halide containing interphase layer between the solid electrolyte composition and an electrode or further wherein the interphase layer comprises a uniform distribution of P, S, and X atoms.
However, based on [0127];[0159];[0163 – 0164] of the instant specification, the presence of the interphase layer and further an interphase layer comprises a uniform distribution of P, S, and X atoms appears to be dependent on the (1) the inclusion of an excess amount of Cl and trace amounts of carboxylic acid ester; (2) the use of a metal anode in the battery; and (3) the method of in which the halide-containing crystalline lithium argyrodite is formed {i.e. in [0127] it is suggested the liquid synthesis of the electrolyte material allows for uniform distribution of P, S, and X atoms}. Furthermore, the examiner notes that the recitation “to form a solid electrolyte, halide containing interphase layer between the solid electrolyte composition and an electrode….wherein the interphase layer comprises a uniform distribution of P, S, and X atoms” establishes an intended use/inherent function for the solid electrolyte composition. Regarding product and apparatus claims, when the structure recited in the reference is substantially identical to that of the claims, claimed properties or functions are presumed to be inherent.
The examiner acknowledges that Utsuno does not teach forming their taught halide-containing lithium sulfide electrolyte via a liquid synthesis method, rather Utsuno teaches a production method having a step of applying mechanical stress {e.g. ball milling} to a mixture of the raw materials as described later to cause reaction to prepare an intermediate and a step of applying heat treatment to the intermediate to cause crystallization ([0072];[0087]).
Zhou teaches solvent-engineered lithium argyrodites represented by Li6PS5X where X is Cl, Br, I (Refer to highlighted text in second paragraph of left column and first paragraph of right column on pg. 266). In the method of preparation, Zhou teaches using Li2S, Li3PS4·3THF, and LiX (X = Cl, Br, I) as the precursors and THF and ethanol as the solvents (Refer to highlighted text in second paragraph of the left column on pg. 266). Furthermore, Zhou’s taught method of preparation includes a drying step at 140°C for 20 hours and an annealing step at 500°C for 6 hours (Refer to highlighted text in second paragraph of left column; highlighted text in first paragraph of right column on pg. 266; and Experimental section in Supporting Information, pg. S2). The Li6PS5Cl is further taught by Zhou to be applied as a solid electrolyte material in a TiS2/Li11Sn6 all-solid-state battery (Refer to highlighted text in second paragraph of right column on pg. 268). Zhou further teaches the traditional methods of preparing lithium argyrodite electrolytes {i.e. milling reactants followed by heat treatment} consumes much energy and is difficult to scale up, making such methods impractical for solid-state batteries and that their solution-engineered method solves such issues while also reducing subsequent heat treatment temperature and/or time and further provides a fully crystallized Li6PS5X where X is Cl and/or Br with comparable electrochemical performance to that of an argyrodite Li6PS5Cl solid electrolyte synthesized by a typical ball-milled solid-state route (Refer to highlighted text in last paragraph on pg. 265; highlighted text in first paragraph of left column on pg. 266; and highlighted text in last paragraph on pg. 269).
Since Utsuno’s taught method utilizes a mechanical method involving milling to prepare their taught lithium sulfide electrolyte which is a lithium argyrodite solid electrolyte including Cl, it would have been obvious to one with ordinary skill in the art, before the effective filing date of the claimed invention, to prepare the electrolyte of Utsuno, and thus modified An’s electrolyte, using a solvent-based method, as taught by Zhou, with a reasonable expectation of success in obtaining the desired electrolyte through a more practical, scalable means.
Therefore, since modified An renders obvious the claimed solid electrolyte composition and structure {i.e. propylene carbonate wetting agent and halide-containing crystalline lithium argyrodite solid electrolyte}, including electrode materials {i.e. lithium metal negative electrode and lithium transition metal positive electrode} disclosed in the instant specification: [00169], and further renders obvious a solvent-based method of making similar to the method of making taught by the applicant to provide a solid electrolyte with uniform distribution of P, S, and X atoms (Instant Specification; [0081];[0086 – 0087];[0127]), a skilled artisan would reasonably expect, the battery of modified An to form the claimed solid electrolyte, halide containing interphase layer between the solid electrolyte composition and an electrode with the claimed uniform distribution of P, S, and X atoms.
Regarding Claims 3 – 5, modified An discloses all limitations as set forth above. In the battery embodiment of modified An, the organic solvent, which corresponds to the claimed wetting agent, is disclosed to be propylene carbonate (An: Example 1; [0046 – 0050]), thus, modified An further discloses wherein the wetting agent is a carboxylic acid ester (Claim 3) and wherein the carboxylic acid ester is propylene carbonate (Claim 5), which is a carboxylic acid ester included in the claimed group consisting of ethylene carbonate, dimethyl carbonate, ethyl-methyl carbonate, and propylene carbonate (Claim 4).
Furthermore, in modified An, X is Cl, which is within the claimed selection of F, Cl, Br, and I (Claim 3 cont.).
Regarding Claims 8 – 9, modified An discloses all limitations as set forth above. Fig 2 of An shows the charge and discharge curve of the battery of Example 1 at 50°C ([0044][0080]). The specific capacity of the example battery, based on Fig. 2, is shown to be about 160 mAh g-1.
Modified An does not explicitly disclose wherein the device when cycling at a C-rate of 0.2 C is characterized by a specific capacity of at least 170 mAh g-1 after cycle 1 of charge/discharge (Claim 8), and further, wherein the device when cycling at a C-rate of 1 C is characterized by a specific capacity of at least 116 mAh g1 after at least 200 cycles of charge/discharge (Claim 9).
However, since An already exemplifies obtaining capacities as high as 160 mAh g-1 (Refer to Fig. 2 in An), and modified An renders obvious the claimed battery composition and structure {i.e. propylene carbonate wetting agent and halide-containing crystalline lithium argyrodite solid electrolyte within the claimed/taught scope of the instant application}, including electrode materials {i.e. lithium metal negative electrode and lithium transition metal positive electrode} disclosed in the instant specification: [00169], a skilled artisan would reasonably expect, given the same test/operating conditions, the battery of modified An to, provide the claimed cycling characteristics.
Regarding Claim 10, modified An discloses all limitations as set forth above. An teaches, with respect to example 1, that the combination of solid electrolyte and organic solvent at the interface of the electrolyte and electrode in the solid-state battery allows for improved interface impedance and good charge/discharge cycle characteristics ([0023];[0080]).
Modified An does not explicitly disclose wherein the device when under a current density of 0.2 mA cm-2 exhibits a flat polarization voltage marked by a variance in voltage of no greater than 10% over a period of time of at least 1000 hours
However, since modified An renders obvious the claimed battery composition and structure {i.e. propylene carbonate wetting agent and halide-containing crystalline lithium argyrodite solid electrolyte within the claimed/taught scope of the instant application }, including electrode materials {i.e. lithium metal negative electrode and lithium transition metal positive electrode} disclosed in the instant specification: [00169], a skilled artisan would reasonably expect, given the same test/operating conditions, the battery of modified An to, provide the claimed flat polarization voltage.
Regarding Claim 13, An discloses an electrochemical energy storage device (solid-state lithium ion battery; [0010]) comprising a solid electrolyte ([0010];[0015]) and a wetting agent (organic solvent; [0010 – 0012]).
The organic solvent disclosed by An reads on the claimed wetting agent, because, like the claimed wetting agent, the organic solvent functions to reduce contact impedance between the electrolyte and electrode in the battery and ultimately allow for improved performance of the solid-state lithium ion battery (An: [0022]; Instant Specification: [0164 – 0165]). Furthermore, materials listed/exemplified to be used as the organic solvent in An, such propylene carbonate, are claimed and disclosed by the applicant to be wetting agents (An: [0022];[0046 – 0050]; Instant Specification: [0164]).
An further teaches an embodiment of the solid-state lithium ion battery where the organic solvent is particularly propylene carbonate (Example 1; [0046]), which, as one with ordinary skill in the art would recognize is a carboxylic acid ester.
Example 1 of An further includes a lithium metal negative electrode, a lithium iron phosphate positive electrode, and a solid electrolyte that is a solid polymer electrolyte composed of polyethylene carbonate, poly(vinylidene fluoride-hexafluoropropylene), and lithium bis (trifluoromethylsulfonyl imide) ([0046 – 0048]); therefore, An does not further explicitly disclose wherein the solid electrolyte composition comprises a solid, halide-crystalline lithium argyrodite represented by a formula chosen from the group consisting of LimPSnXo and LimPSn, where m is a number in the range of 4-8, n is a number in the range of 3-6, X represents at least one halide, and o is a number in the range of 0-3.
Generally, An teaches using inorganic solid electrolytes for the solid-state lithium ion battery ([0015]). Inorganic solid electrolytes taught by An include materials such as Li7La3ZrO12, Li10GeP2S12, Li3OCl0.5Br0.5, Li3xLa(2/3)-xTiO3, Li5La3Ta2O12, Li5La3Nb2O12, Li5.5La3Nb1.74In0.25O12, Li3N-LiCl, Li3N-LiBr, Li3N-LiI, Li14Zn(GeO4)4, LiZr2(PO4)3, Li3OCl, LiPON, and Li2S-MaSb wherein 0.04 < x < 0.14, M = Al, Si, or P, and the values of a and b are 1 – 3, respectively.
Utsuno, also directed to solid-state lithium ion batteries ([0130 – 0131]), teaches a sulfide solid electrolyte with an argyrodite-crystal structure represented by LiaPSbClc wherein 5.0 ≤ a ≤ 6.5, 6.1 ≤ a + c ≤ 7.5 {i.e. 0.4 ≤ c ≤ 2.5}, 0.5 ≤ a - b ≤ 1.5 {i.e. 3.5 ≤ b ≤ 6}, b > 0, and c > 1.0 are satisfied ([0035];[0055 – 0057]). Utsuno further teaches that the electrolyte material has improved ion conductivity due to the inclusion of chlorine, and is compatible with negative electrodes including elemental metals like metal lithium and positive electrodes including transition metal oxides like LiFePO4 ([0015];[0026];[0107];[0122]).
Since An already teaches using inorganic sulfide solid electrolytes that include Li, S, and P, it would have been obvious to one with ordinary skill in the art, before the effective filing date of the claimed invention, to modify the battery of Example 1, to include the sulfide solid electrolyte taught by Utsuno, and thus obtain a solid electrolyte composition within the claimed scope, with a reasonable expectation of success in obtaining a solid electrolyte with improved conductivity and suitable for An’s solid-state lithium ion battery.
By including a sulfide solid electrolyte represented by LiaPSbClc wherein 5.0 ≤ a ≤ 6.5, 6.1 ≤ a + c ≤ 7.5 {i.e. 0.4 ≤ c ≤ 2.5}, 0.5 ≤ a - b ≤ 1.5 {i.e. 3.5 ≤ b ≤ 6}, b > 0, and c > 1.0 are satisfied (Utsuno: [0035];[0055 – 0057]), modified An’s solid electrolyte composition includes halide-containing crystalline lithium argyrodites such as Li6PS5Cl·0.5LiCl and Li6PS5Cl. Therefore, modified An provides a halide-containing crystalline lithium argyrodite represented by LimPSnXo, where m is 5 – 6.5, which is within the claimed range of 4 – 8, n is 3.5 – 6, which is within the claimed range of 3 – 6, X represents at least one halide {i.e. Cl}, and o is 0.4 to 2.5 which is within the claimed range of 0 – 3; and further includes within its scope halide-containing crystalline lithium argyrodites represented as xLiX·Li6PS5X.
Modified An does not explicitly disclose the halide-containing crystalline lithium argyrodite forming a solid electrolyte, halide containing interphase layer between the solid electrolyte composition and an electrode or further wherein the interphase layer comprises a uniform distribution of P, S, and X atoms.
However, based on [0127];[0159];[0163 – 0164] of the instant specification, the presence of the interphase layer and further an interphase layer comprises a uniform distribution of P, S, and X atoms appears to be dependent on the (1) the inclusion of an excess amount of Cl and trace amounts of carboxylic acid ester; (2) the use of a metal anode in the battery; and (3) the method of in which the halide-containing crystalline lithium argyrodite is formed {i.e. in [0127] it is suggested the liquid synthesis of the electrolyte material allows for uniform distribution of P, S, and X atoms}. Furthermore, the examiner notes that the recitation “to form a solid electrolyte, halide containing interphase layer between the solid electrolyte composition and an electrode….wherein the interphase layer comprises a uniform distribution of P, S, and X atoms” establishes an intended use/inherent function for the solid electrolyte composition. Regarding product and apparatus claims, when the structure recited in the reference is substantially identical to that of the claims, claimed properties or functions are presumed to be inherent.
The examiner acknowledges that Utsuno does not teach forming their taught halide-containing lithium sulfide electrolyte via a liquid synthesis method, rather Utsuno teaches a production method having a step of applying mechanical stress {e.g. ball milling} to a mixture of the raw materials as described later to cause reaction to prepare an intermediate and a step of applying heat treatment to the intermediate to cause crystallization ([0072];[0087]).
Zhou teaches solvent-engineered lithium argyrodites represented by Li6PS5X where X is Cl, Br, I (Refer to highlighted text in second paragraph of left column and first paragraph of right column on pg. 266). In the method of preparation, Zhou teaches using Li2S, Li3PS4·3THF, and LiX (X = Cl, Br, I) as the precursors and THF and ethanol as the solvents (Refer to highlighted text in second paragraph of the left column on pg. 266). Furthermore, Zhou’s taught method of preparation includes a drying step at 140°C for 20 hours and an annealing step at 500°C for 6 hours (Refer to highlighted text in second paragraph of left column; highlighted text in first paragraph of right column on pg. 266; and Experimental section in Supporting Information, pg. S2). The Li6PS5Cl is further taught by Zhou to be applied as a solid electrolyte material in a TiS2/Li11Sn6 all-solid-state battery (Refer to highlighted text in second paragraph of right column on pg. 268). Zhou further teaches the traditional methods of preparing lithium argyrodite electrolytes {i.e. milling reactants followed by heat treatment} consumes much energy and is difficult to scale up, making such methods impractical for solid-state batteries and that their solution-engineered method solves such issues while also reducing subsequent heat treatment temperature and/or time and further provides a fully crystallized Li6PS5X where X is Cl and/or Br with comparable electrochemical performance to that of an argyrodite Li6PS5Cl solid electrolyte synthesized by a typical ball-milled solid-state route (Refer to highlighted text in last paragraph on pg. 265; highlighted text in first paragraph of left column on pg. 266; and highlighted text in last paragraph on pg. 269).
Since modified An’s taught method utilizes a mechanical method involving milling to prepare their taught lithium sulfide electrolyte which is a lithium argyrodite solid electrolyte including Cl, it would have been obvious to one with ordinary skill in the art, before the effective filing date of the claimed invention, to prepare the electrolyte of Utsuno, and thus modified An’s electrolyte, using a solvent-based method, as taught by Zhou, with a reasonable expectation of success in obtaining the desired electrolyte through a more practical, scalable means.
Therefore, since modified An renders obvious the claimed solid electrolyte composition and structure {i.e. propylene carbonate wetting agent and halide-containing crystalline lithium argyrodite solid electrolyte}, including electrode materials {i.e. lithium metal negative electrode and lithium transition metal positive electrode} disclosed in the instant specification: [00169], and further renders obvious a solvent-based method of making similar to the method of making taught by the applicant to provide a solid electrolyte with uniform distribution of P, S, and X atoms (Instant Specification; [0081];[0086 – 0087];[0127]), a skilled artisan would reasonably expect, the battery of modified An to form the claimed solid electrolyte, halide containing interphase layer between the solid electrolyte composition and an electrode with the claimed uniform distribution of P, S, and X atoms.
Conclusion
Applicant's amendment necessitated the new ground(s) of rejection presented in this Office action. Accordingly, THIS ACTION IS MADE FINAL. See MPEP § 706.07(a). Applicant is reminded of the extension of time policy as set forth in 37 CFR 1.136(a).
A shortened statutory period for reply to this final action is set to expire THREE MONTHS from the mailing date of this action. In the event a first reply is filed within TWO MONTHS of the mailing date of this final action and the advisory action is not mailed until after the end of the THREE-MONTH shortened statutory period, then the shortened statutory period will expire on the date the advisory action is mailed, and any nonprovisional extension fee (37 CFR 1.17(a)) pursuant to 37 CFR 1.136(a) will be calculated from the mailing date of the advisory action. In no event, however, will the statutory period for reply expire later than SIX MONTHS from the mailing date of this final action.
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/A.Y.O./Examiner, Art Unit 1751
/JONATHAN G LEONG/Supervisory Patent Examiner, Art Unit 1751 8/31/2026
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