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 .
Response to Arguments
Applicant's arguments filed 04/24/2026 have been fully considered but they are not persuasive.
Applicant amended claim 1 to include the subject matter of cancelled claim 7. Ling and Jing are differently combined to teach amended claim 1. Specifically, regarding the claimed structure represented by: Li1+xMi2-yMiiy(PO4)3 wherein 0≤x≤1, 0.0≤y≤0.3; Mi is at least one selected from the group consisting of Al, Ga, Fe, Zr, Ca, and In; and Mii is at least one selected from the group consisting of Ti, V, Co, and Fe, secondary reference Jing is applied to teach the formula as claimed.
Jing discloses Li1.5Al0.5Ge1.5(PO4)3, which is the same LAGP formula as disclosed by Ling, that is doped with TiO2 undergoing a sintering process to form a new composite material of LAGP-TiO2 (see e.g., Jing; 2.1 Preparation and Characterization of Solid Electrolyte). Jing discloses that TiO2 may be included in weight% of 0, 2.5, 7.5, and 10, and shows in table 1 the atomic ratios of the sample provided with a weight% of 7.5 TiO2. In this sample, Al, Ti, and Ge have atomic% at the grain of 3.40, 2.37, and 8.68, respectively, and atomic% at the grain boundary of 4.83, 3.06, and 14.42, respectively. Therefore, in the sample having 7.5 wt% of TiO2 added, the ratio of transition metal Ti to all metal elements at the grain is about 16.4%, and about 13.7% at the grain boundary. Although Jing does not explicitly show the atomic ratio of the 2.5 wt% TiO2 sample, the approximate atomic ratios of this sample may be found through proportional calculation, which results Al, Ti, and Ge of 3.57%, 0.79%, and 9.12% at the grain, respectively, and Al, Ti, and Ge of 4.96%, 1.02%, and 15.56% at the grain boundary, respectively. The TiO2 doped LAGP provided by Jing overlaps with the claimed formula of Li1+xMi2-yMiiy(PO4)3 wherein 0≤x≤1, 0.0≤y≤0.3; Mi is at least one selected from the group consisting of Al, Ga, Fe, Zr, Ca, and In; and Mii is at least one selected from the group consisting of Ti, V, Co, and Fe; in this case, Mi is Ge and Mii is Ti. It would have been obvious for one of ordinary skill in the art before the effective filing date of the claimed invention to have modified the LAGP component of Ling by doping with TiO2 in low weight% of 2.5, 5, 7.5, because the TiO2-doped LAGP material results in higher bulk conductivity, grain boundary conductivity, total conductivity, and lower activation energy (see e.g., Jing; Table 2). These material improvements are even apparent in the low doping of Ti-2.5 as shown in table 2.
Therefore, amended claim 1 is taught by Ling and Jing.
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) 1-4, 9-12 is/are rejected under 35 U.S.C. 103 as being unpatentable over Ling (Shi-Gang Ling et al 2018 Chinese Phys. B 27 038201. Enhanced ionic conductivity in LAGP/LATP composite electrolyte), and in further view of Jing (Jing Yang, Zhen Huang, Peng Zhang, Gaozhan Liu, Xiaoxiong Xu, and Xiayin Yao ACS Applied Energy Materials 2019 2 (10), 7299-7305 DOI: 10.1021/acsaem.9b01268).
Regarding claim 1, Ling discloses a composite electrolyte comprising LAGP and LATP, wherein the LATP may be Li1.4Al0.4Ti1.6(PO4)3 (see e.g., Ling; abstract), which corresponds with the claimed plurality of solid electrolyte particles having a second portion in which a second constituent ratio of a transition metal element to all metal elements, excluding lithium, is more than 15%, because transition metal Ti is included in a molar amount of 1.6 compared to the molar amount of all metals excluding lithium of 2.0.
Ling discloses the composite electrolyte is developed within the context of lithium ion batteries (see e.g., Ling; Introduction), but in this study Ling does not explicitly disclose the composite electrolyte in a solid state battery comprising at least one battery constituent unit including a positive electrode layer, a negative electrode layer, and the solid electrolyte layer interposed between the positive electrode layer and the negative electrode layer.
However, Jing discloses an all-solid-state battery assembled with a lithium metal anode, polymer buffer layer and LAGP-TiO2 glass-ceramics sheet corresponding to a solid electrolyte layer, and LiFePO4 composite cathode (see e.g., Jing; 2.2 Preparation and Characterization of All-Solid-State Batteries). Therefore, it would have been obvious for one of ordinary skill in the art before the effective filing date of the claimed invention to have used the electrolyte disclosed by Ling in an all solid state battery with a positive electrode, negative electrode, and solid electrolyte interposed between as disclosed by Jing in order to enhance safety and improve the energy density of lithium batteries (see e.g., Ling; Introduction).
Ling discloses that the electrolyte may be a composite electrolyte with LAGP/LATP, and the LAGP may correspond with the claimed plurality of solid electrolyte particles having a first portion. Ling discloses that the LAGP may be of formula Li1.5Al0.5Ge1.5(PO4)3 (see e.g., Ling; abstract), which corresponds with the plurality of solid electrolyte particles contain a lithium-containing phosphate compound having a NASICON structure.
Ling does not disclose that this first portion having a transition metal and having a first constituent ratio of transition metal element to all metal elements, excluding lithium, of 0.5% to 15%, and wherein the structure is represented by: Li1+xMi2-yMiiy(PO4)3 wherein 0≤x≤1, 0.0≤y≤0.3; Mi is at least one selected from the group consisting of Al, Ga, Fe, Zr, Ca, and In; and Mii is at least one selected from the group consisting of Ti, V, Co, and Fe.
However, Jing discloses Li1.5Al0.5Ge1.5(PO4)3, which is the same LAGP formula as disclosed by Ling, that is doped with TiO2 undergoing a sintering process to form a new composite material of LAGP-TiO2 (see e.g., Jing; 2.1 Preparation and Characterization of Solid Electrolyte). Jing discloses that TiO2 may be included in weight% of 0, 2.5, 7.5, and 10, and shows in table 1 the atomic ratios of the sample provided with a weight% of 7.5 TiO2. In this sample, Al, Ti, and Ge have atomic% at the grain of 3.40, 2.37, and 8.68, respectively, and atomic% at the grain boundary of 4.83, 3.06, and 14.42, respectively. Therefore, in the sample having 7.5 wt% of TiO2 added, the ratio of transition metal Ti to all metal elements at the grain is about 16.4%, and about 13.7% at the grain boundary. Although Jing does not explicitly show the atomic ratio of the 2.5 wt% TiO2 sample, the approximate atomic ratios of this sample may be found through proportional calculation, which results Al, Ti, and Ge of 3.57%, 0.79%, and 9.12% at the grain, respectively, and Al, Ti, and Ge of 4.96%, 1.02%, and 15.56% at the grain boundary, respectively. Therefore, TiO2 included at 2.5 wt% may have transition metal Ti to all metal elements at the grain of about 5.9%, and transition metal Ti to all metal elements at the grain boundary of about 4.7%. Therefore, the inclusion of TiO2 with the LAGP of 2.5 wt% and 7.5 wt% results in a LAGP-TiO2 particles that fall within the claimed first constituent ratio of a transition metal element to all metal elements, excluding lithium, of 0.5% to 15%. Moreover, the TiO2 doped LAGP provided by Jing overlaps with the claimed formula of Li1+xMi2-yMiiy(PO4)3 wherein 0≤x≤1, 0.0≤y≤0.3; Mi is at least one selected from the group consisting of Al, Ga, Fe, Zr, Ca, and In; and Mii is at least one selected from the group consisting of Ti, V, Co, and Fe; in this case, Mi is Ge and Mii is Ti. It would have been obvious for one of ordinary skill in the art before the effective filing date of the claimed invention to have modified the LAGP component of Ling by doping with TiO2 in low weight% of 2.5, 5, 7.5, because the TiO2-doped LAGP material results in higher bulk conductivity, grain boundary conductivity, total conductivity, and lower activation energy (see e.g., Jing; Table 2). These material improvements are even apparent in the low doping of Ti-2.5 as shown in table 2. The resulting modification of Jing to Ling provides an LAGP-TiO2 and LATP composite electrolyte.
Regarding claim 2, modified Ling teaches the solid state battery according to claim 1. Ling discloses the composite electrolyte of LAGP and LATP particles (see e.g., Ling; abstract), which are both ceramic materials that are electron conduction path blocking materials.
Regarding claim 3, modified Ling teaches the solid state battery according to claim 1. Ling discloses wherein the solid electrolyte layer is a single layer, and the plurality of the solid electrolyte particles are randomly arranged in the single layer (see e.g., Ling; 2.1 regarding LAGP and LATP powders combined and pressed into sheets corresponding to a single layer).
Regarding claim 4, modified Ling teaches the solid state battery according to claim 1. Ling discloses wherein the first portion is a plurality of a first solid electrolyte particles, and the second portion is a plurality of second solid electrolyte particles (see e.g., Ling; abstract, Experimental details, wherein LAGP may be the first portion have a plurality of first solid electrolyte particles and LATP may be the second portion having a plurality of second solid electrolyte particles), and the plurality of second solid electrolyte particles are interspersed and arranged so as to be separated from each other in a main part of the solid electrolyte layer in which the plurality of first solid electrolyte particles are arranged in a matrix form (see e.g., Ling; 2.1, regarding LAGP and LATP mixed into weight ratios of 80:20, 50:50, and 20:80 and pressed into sheets to be sintered, which corresponds to forming the matrix).
Regarding claim 9, modified Ling teaches the solid state battery according to claim 1. As described above regarding claim 1, modified Ling teaches wherein TiO2 included at 2.5 wt% may have transition metal Ti to all metal elements at the grain of about 5.9%, and transition metal Ti to all metal elements at the grain boundary of about 4.7%, which falls within the claimed first constituent ratio having a range of 0.5% to 10%.
Regarding claim 10, modified Ling teaches the solid state battery according to claim 1. As described above regarding claim 1, modified Ling teaches wherein TiO2 included at 2.5 wt% may have transition metal Ti to all metal elements at the grain of about 5.9%, and transition metal Ti to all metal elements at the grain boundary of about 4.7%, which falls within the claimed first constituent ratio having a range of 1% to 10%.
Regarding claim 11, modified Ling teaches the solid state battery according to claim 1. As above regarding claim 1, modified Ling with Jing teaches wherein the positive electrode layer is LiFePO4 and the negative electrode layer is a metal anode layer (see e.g., Jing; 2.2 Preparation and Characterization of All-Solid-State Batteries), which corresponds with the claimed layers that insert and extract lithium ions.
Regarding claim 12, modified Ling teaches the solid state battery according to claim 1. As described above regarding claim 1, modified Ling teaches wherein TiO2 included at 2.5 wt% may have transition metal Ti to all metal elements at the grain of about 5.9%, and transition metal Ti to all metal elements at the grain boundary of about 4.7%. Therefore, in the sample of 2.5 wt%, the grain boundary of the particles may correspond with the claimed first portion having a first constituent ratio of transition metal elements to all metal elements, excluding lithium, of 4.7%, which falls within the claimed ratio having a range of 0.5% to 5%.
Claim(s) 5 is/are rejected under 35 U.S.C. 103 as being unpatentable over Ling (Shi-Gang Ling et al 2018 Chinese Phys. B 27 038201. Enhanced ionic conductivity in LAGP/LATP composite electrolyte), and Jing (Jing Yang, Zhen Huang, Peng Zhang, Gaozhan Liu, Xiaoxiong Xu, and Xiayin Yao ACS Applied Energy Materials 2019 2 (10), 7299-7305 DOI: 10.1021/acsaem.9b01268), and in further view of Yi (US-20180123167-A1).
Regarding claim 5, modified Ling teaches the solid state battery according to claim 1. Ling does not explicitly disclose wherein the plurality of solid electrolyte particles have a core/shell structure in which a core portion thereof is the second portion, and a shell portion which surrounds the core portion is the first portion. However, Yi discloses a solid electrolyte with a core/shell structure wherein the core is LATP and the shell has high ionic conductivity (see e.g., Yi; [0006], regarding internal component corresponding to core having formula of Li1+x Mx Ti2−x (PO4 )3 wherein M is one or more elements selected from the group of Al, La, Cr, Ga, Y, and In, and 0.05≤x≤0.4, and external component corresponding to shell). The formula disclosed by Yi overlaps with the LATP formula of Ling. Therefore, Yi may further modify Ling and Jing such that the LAGP-TiO2 doped material is arranged as a shell around the LATP. It would have been obvious for one of ordinary skill in the art before the effective filing date of the claimed invention to have further modified the LAGP-TiO2 and LATP electrolyte of modified Ling with Jing such that the LAGP-TiO2 materials is provided as a shell around the LATP material because Yi discloses that an LATP material having a high ionic conductivity shell, which the modified LAGP-TiO2 material has (see e.g., Jing; abstract, regarding ionic conductivity of up to 1.07 x 10-3 S/cm-1), to increase the electrochemical window of the solid electrolyte and improve security (see e.g., Yi; [0004]-[0005]). In summary, the modification results in a LATP core corresponding to a second portion and a LAGP-TiO2 shell around the LATP core particles corresponding to a first portion.
Claim(s) 6 is/are rejected under 35 U.S.C. 103 as being unpatentable over Ling (Shi-Gang Ling et al 2018 Chinese Phys. B 27 038201. Enhanced ionic conductivity in LAGP/LATP composite electrolyte), and Jing (Jing Yang, Zhen Huang, Peng Zhang, Gaozhan Liu, Xiaoxiong Xu, and Xiayin Yao ACS Applied Energy Materials 2019 2 (10), 7299-7305 DOI: 10.1021/acsaem.9b01268), and in further view of Onouchi (JP2015060737A).
Regarding claim 6, modified Ling teaches the solid state battery according to claim 1. Ling does not explicitly disclose wherein at least one of the positive electrode layer and the negative electrode layer further contains the plurality of solid electrolyte particles. However, Onouchi discloses the positive electrode layer and the negative electrode layer further contains a plurality of solid electrolyte particles (see e.g., Onouchi; [0026], [0036], [0043], [0080]-[0081], [0092]-[0093]). Onouchi is further analogous art because Onouchi discloses NASICON electrolyte particles that may also have Ti and Ge (see e.g., Onouchi; [0040]). It would have been obvious for one of ordinary skill in the art before the effective filing date of the claimed invention to have modified Ling by having solid electrolyte particles of modified Ling in the electrode layers of modified Ling as disclosed by Onouchi. One of ordinary skill in the art would have been motivated to make this modification in order to obtain high ionic conductivity essential for operation of solid-state batteries (see e.g., Onouchi; [0043]).
Conclusion
THIS ACTION IS MADE FINAL. 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.
Any inquiry concerning this communication or earlier communications from the examiner should be directed to KEVIN SONG whose telephone number is (571)270-7337. The examiner can normally be reached Monday - Friday 9:00 am - 5:00 pm EST.
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/KEVIN SONG/Examiner, Art Unit 1728
/MATTHEW T MARTIN/Supervisory Patent Examiner, Art Unit 1728
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