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 .
Status of Claims
Claims 1-4 and 6-13 are amended. Claim 5 is cancelled. Claims 14-15 are withdrawn from further consideration pursuant to 37 CFR 1.142(b) as being drawn to a nonelected groups II and III, there being no allowable generic or linking claim. Claims 1-4 and 6-13, as filed 22 September 2025, are examined herein. No new matter is included.
Response to Arguments
The claim objection is withdrawn.
The rejection under 35 USC 112(b) of claims 1-13 is withdrawn in light of Applicants amendments and arguments.
Regarding the rejection under 35 USC 103, Applicant argues:
(1) That Yuan does not disclose a molar ratio of sodium atoms in the sodium salt to metal atoms in the transition metal salt does not exceed 1, and is not less than 0.5;
(2) That Yuan does not disclose weighing and tableting powder, wherein a pressure applied is not greater than 100 MPa, and the pressure is maintained for 3~5 minutes, to obtain a precursor sheet with a thickness not more than 3 mm; and
(4) That there is no motivation to modify Yuan with the molten salt ion exchange of Yang.
Applicant specifically argues that the features of claim 1 have resolved the technical problems of improving the room-temperature ionic conductivity of the polymer solid-state electrolyte. “The objective is an inorganic crystal material having a diffusion channel penetrating through the frame. The diffusion of ions in the channel is driven by the migration of thermal defects in loaded ion sublattice, and the diffusion activation energy is generally low, therefore, a higher room- temperature ionic conductivity is provided compared with the structure-driven ion conductor. Although a stable structural framework constitutes an ion diffusion channel, the widespread grain boundaries are also introduced into the structure, which severely hinders the diffusion of ions between the grains, then it is critical to regulate the grain boundaries. …”
“In the above process of preparing the precursor, the addition amount of sodium salt is quite critical. When the molar ratio of sodium atoms in the sodium salt to metal atoms in the transition metal salt is 1-2, the product is in a crystalline state, and when the molar ratio of sodium atoms in the sodium salt to metal atoms in the transition metal salt is lower than 1, the product is in an amorphous state. … it is determined through theoretical speculation and repeated test verification that to enable the performance of product to be optimized, the addition amount of sodium salt should satisfy that the molar ratio of the sodium atoms therein to the metal atoms in the transition metal salt does not exceed 1 and is not lower than 0.5.”
Applicant further argues:
“The abovementioned distinguishing feature "a molar ratio of sodium atoms in the sodium salt to metal atoms in the transition metal salt does not exceed 1, and is not less than 0.5" as defined in claim 1 has resolved the technical problem of improving the ionic conductivity of the material.
In sharp contrast, it is clearly disclosed in Paragraph 0011 of Yang "the anode material according to the present invention has a better potential plateau, better cycle performance, and better magnification properties, than a conventional titanium-based anode material having a delithiation potential of 0.8 to 1.2 V". Thus, the technical problem addressed by the technical solution of Yang with the abovementioned feature "a molar ratio of sodium atoms in the sodium salt to metal atoms in the transition metal salt does not exceed 1, and is not less than 0.5" is to provide a better potential plateau, better cycle performance, and better magnification properties, which is completely irrelevant and different from the technical problem of improving the ionic conductivity of the material in the instant application. Consequently, from the perspective of technical problem, those of ordinary skill in the art would have no motivation to combine Yuan with Yang to arrive at the technical solution of claim 1 to resolve the technical problem of improving the ionic conductivity of the material.”
Applicant's arguments are not persuasive. (1) Applicant has argued that the selection of a molar ratio between 0.5 and 1 is critical for regulating the grain boundaries to obtain excellent room-temperature ionic conductivity. Yuan teaches this feature at [0038], therefore the argument that this range is critical is moot. (2) Applicant has argued that Yuan does not disclose weighing and tableting powder, wherein a pressure applied is not greater than 100 MPa, and the pressure is maintained for 3~5 minutes, to obtain a precursor sheet with a thickness not more than 3 mm. Yuan discloses weighing and “using a film press”, to obtain a sheet with a thickness of 1 mm (as set forth below). Examiner notes that while Yuan does not disclose the claimed pressure range of the tableting press, most commercially available tableting pressed (film pressed) provide a pressure less than 100 MPa. See for example Nogami (US 20160204466 A1) disclosing [0120] “The complex hydride solid electrolyte powder was put into a 10-mm diameter powder tableting machine and was press-formed at a pressure of 28 MPa.” Further, Applicant has not provided evidence for the criticality of the tableting pressure or time. (3) Applicant has argued there is no motivation to modify Yuan with the molten salt ion exchange of Yang. The person of ordinary skill is motivated to attempt the molten salt ion exchange process as taught by Yang on the silicate compound of modified Yuan, in order solve the problem of Li volatilizing during high temperature treatment, with a reasonable expectation of successfully creating a desirable lithium silicate compound.
Claim Interpretation
Regarding claim 4 “wherein in step 1) …. a product is in a crystalline state, …” “A product” likely refers to “the transition metal silicate sodium ion conductor obtained in step 2) of claim 2.” The clarity of this claim can be improved.
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.
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) 1-4 and 6-13 is/are rejected under 35 U.S.C. 103 as being unpatentable over Yuan (CN105819461A, with paragraph numbering to the provided English translation) in view of Barker (US 20040197654 A1) and Yang (US 20180151878 A1).
Regarding claim 1, Yuan teaches a preparation method of a transition metal silicate ion conductor ([0007] “doped sodium silicate positive electrode material”, ([0010])the transition metal including iron, Fe, [0027] “sodium ion migration … significantly improved),
wherein the preparation method is performed by sintering using a solid phase method, ([0015], [0023,0025] sintering at temperatures lower than melting points of the transition metals) specifically comprising following steps:
1) wherein the precursor is prepared with a transition metal salt, a sodium salt, and ethyl orthosilicate as raw materials ([0013], [0019] ferrous acetate, [0017] sodium acetate, [0020] tetra ethyl orthosilicate) as raw materials,
wherein a molar ratio of sodium atoms in the sodium salt to metal atoms in the transition metal salt does not exceed 1, and is not less than 0.5. ([0038] 0.98 mol sodium oxalate to 0.02 mol of magnesium oxalate and 1.0 mol of ferrous oxalate.) This creates a molar ratio of 0.98: (0.02 + 1.0) = 0.98:1.02 = 0.96: 1.0, which is between 0.5 and 1, which falls within the claimed range,
a molar ratio of sodium atoms in the sodium salt to silicon atoms in the ethyl orthosilicate does not exceed 2; ([0038] 0.98 mol sodium oxalate to 1 mol of TEOS) This creates a molar ratio of 0.98: 1.0 = 0.98, which falls within the claimed range;
2) making a solid phase sintered transition metal silicate sodium ion conductor, ([0014]) pre-sintering the precursor in a vacuum tubular furnace protected by an inert gas at 300~500 ˚C for more than 5 hours ([0014],[0023] pre-firing … 350-500˚C for 2-6 hours in an inert atmosphere, which overlaps the range of the instant limitation, establishing a prima facie case of obviousness [MPEP 2144.04(I)]); milling a resultant to refine powder particles ([0024] the solid pre-burned in step b is crushed and mixed with the carbon source compound in a mass ratio of 1: (0.1-1))
weighing and tableting the powder, wherein a pressure applied is not greater than 100 MPa, … to obtain a precursor sheet with a thickness not more than 3 mm. ([0013] accurately weighing, [0040] “pressing into a film with a thickness of about 1 mm using a film press”. Examiner notes that a film press is likely to apply less than 100MPa of pressure.)
finally sintering the precursor sheet in the vacuum tubular furnace protected by an inert gas for more than 8 hours, at a sintering temperature of 500-900 ˚C, ([0015],[0025] “sinter the precursor at 600-900˚C for 2-10 hours in an inert atmosphere”) which overlaps the range of the instant claim limitation.
Yuan does not explicitly teach (A) the pressure is maintained for 3-5 minutes, (B) transferring the precursor sheet into a porcelain boat, and (C) wherein the heating and cooling rates do not exceed 2˚C per minute, so as to obtain a crystalline or amorphous transition metal silicate sodium ion conductor with high ionic conductivity.
Pertaining to (A) while modified Yuan is silent on the pressure applied and the time of the pressure being applied, absent persuasive evidence that the applied pressure and time to form the tablet is significant, a person of ordinary skilled in the art would have found it obvious to have selected a pressure of not greater than 100 MPa, the pressure being maintained for 3-5 minutes in order to form a tablet (i.e., pellet) having good grain-to-grain contact, without undue experimentation and with a reasonable expectation of success [MPEP 2144.05(II)].”
Pertaining (B) above, Barker (in the field of electroactive materials, see Abstract and [0168]) discloses at ([0319]) Barker that the pelletized material is “transfer[red] to a temperature-controlled tube furnace and heated at a preferred ramp rate of about 2˚C/minute to an ultimate temperature of about 800°C”, which falls within the instant temperature ramp rate limitation. At ([0321]) Barker contemplates that the pellet may be placed inside a nickel crucible or other suitable container such as a ceramic crucible (the claimed alumina boat is a type of ceramic crucible). A person of ordinary skill in the art would have been motivated, as of before the effective filing date of the instant invention, to select a ceramic crucible as contemplated by Barker, for the pellet of modified Yuan, with a reasonable expectation of successful sintering, based on Barker’s teaching of suitability.
At ([0312]) Barker contemplates that “the cooling may be conducted at a rate similar to the earlier ramp rate. Such a cooling rate has been found to be adequate to achieve the desired structure of the final product”, which falls within the instant claim limitation.
A person of ordinary skill in the art would have been motivated, as of before the effective filing date of the instant invention, to heat and cool the pellet of modified Yuan at the 2˚C/minute rate as contemplated by Barker, with a reasonable expectation of achieving the desired structure of the final product, thus obtaining a crystalline or amorphous transition metal silicate sodium ion conductor with high ionic conductivity.
Yuan and Barker do not explicitly teach step 3):
performing ion exchange, comprising using an ion exchange method to replace Na in an obtained transition metal silicate sodium ion conductor with other metal ions, so as to prepare other alkali metal or alkaline earth metal ion conductors, wherein ion exchange can be performed by a method comprising electrochemical exchange, molten salt exchange, and solution exchange,
wherein the electrochemical exchange is achieved by charging or discharging the obtained sodium ion conductor with different metal anodes, so that other metal ions replace Na sites; the molten salt exchange is achieved by to immersing the obtained sodium ion conductor into a molten salt containing different metal ions, and carrying out ion exchange with different chemical potentials; and the solution exchange method comprises immersing the obtained sodium ion conductor into a solution of different metal ions, and carrying out ion exchange by concentration differences.
Yang, in a similar field of endeavor, teaches ([0033]) ion exchange using molten salt which allows for the production of a compound containing the easily volatilizable the Li element, without losing the Li during the sintering process. Specifically, Yang teaches replacing Na in a NaEuTi04 compound with Li, to create LiEuTi04, which solves the problem of Li volatilizing during high temperature treatment.
A person of ordinary skill in the art would have been motivated, as of before the effective filing date of the instant invention, to attempt the molten salt ion exchange process as taught by Yang on the silicate compound of modified Yuan, in order solve the problem of Li volatilizing during high temperature treatment, with a reasonable expectation of successfully creating a desirable lithium silicate compound.
Regarding claim 2, Yuan in view of Barker and Yang teaches all of the limitations as considered above, and Yuan further teaches wherein the transition metal salt is [0019] ferrous acetate, oxalate, or nitrate. These candidates are within the scope of the claimed list of alternatives.
Regarding claim 3, Yuan in view of Barker and Yang teaches all of the limitations as considered above, and Yuan further teaches wherein the sodium salt is ([0017]) sodium acetate, which is a candidate within the scope of the claimed list of alternatives.
Regarding claim 4, Yuan in view of Barker and Yang teaches all of the limitations as considered above. Regarding the limitation wherein in step 1), when the molar ratio of sodium atoms in the sodium salt to metal atoms in the transition metal salt is 1-2, a product is in a crystalline state, and when the molar ratio of sodium atoms in the sodium salt to metal atoms in the transition metal salt is less than 1, a product is in an amorphous state. Modified Yuan as set forth above teaches the chemistry and processing steps of the claimed material, therefore the claimed material at a molar ratio of 0.98 will necessarily possess the claimed amorphous state.
Regarding claim 6, Yuan in view of Barker and Yang teaches all of the limitations as considered above, and Yang further teaches wherein in step 1), a ratio of a mole number of metal atoms to a mole number of sodium atoms is 1:0.5- 1:2. ([0038] 0.98 mol sodium oxalate to 0.02 mol of magnesium oxalate and 1.0 mol of ferrous oxalate) This creates a molar ratio of 0.98: (0.02 + 1.0) = 0.98:1.02 = 0.96: 1.0, which falls within the claimed range.
Regarding claim 7, Yuan in view of Barker and Yang teaches all of the limitations as considered above, and Yang further teaches wherein in step 1), a ratio of a mole number of silicon atoms to a mole number of sodium atoms is 1:0.5- 1:2. ([0038] 0.98 mol sodium oxalate to 0.02 mol of magnesium oxalate and 1.0 mol of ferrous oxalate) This creates a molar ratio of 0.98: (0.02 + 1.0) = 0.98:1.02 = 0.96: 1.0, which falls within the claimed range.
Regarding claim 8, Yuan in view of Barker and Yang teaches all of the limitations as considered above, and Yuan further teaches wherein in step 2), the inert gas is ([0038]) nitrogen, which is a candidate within the scope of the claimed list of alternatives.
Regarding claim 9, Yuan in view of Barker and Yang teaches all of the limitations as considered above, and Yuan further teaches wherein in step 2), a pre- sintering temperature is ([0038]) 400 ˚C, which is a candidate within the scope of the claimed list of alternatives.
Regarding claim 10, Yuan in view of Barker and Yang teaches all of the limitations as considered above, and Yuan further teaches wherein in step 2), the sintering temperature is ([0038]) 650 ˚C which is a candidate within the scope of the claimed list of alternatives.
Regarding claim 11, Yuan in view of Barker and Yang teaches all of the limitations as considered above, and Yuan further teaches wherein other metal ions in step 3) are ([0038]) Mg, which is a candidate within the scope of the claimed list of alternatives.
Regarding claim 12, Yuan in view of Barker and Yang teaches all of the limitations as considered above. Yuan does not explicitly teach wherein the molten salt in step 3) is a salt capable of dissociating desired metal ions in a molten state.
Yang teaches ([0033]) the use of LiNO3, which meets the instant claim limitation. A person of ordinary skill in the art would have been motivated, as of before the effective filing date of the instant invention, to use LiNO3 molten salt exchange for the reasons set forth in claim 1.
Regarding claim 13, Yuan in view of Barker and Yang teaches all of the limitations as considered above, and Yuan further teaches wherein the solution in step 3) is a solution capable of ionizing desired metal ions in a solvent. ([0040]) disclosing a sodium ion battery having a solvent-based electrolyte. The battery achieved a charge and discharge current of 0.1C and a charge and discharge voltage range of 4.2V to 1.5V (vs. Na), therefore metal ions are ionized.
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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CLAIRE A. RUTISER
Examiner
Art Unit 1751
/C.A.R./Examiner, Art Unit 1751
/JONATHAN G LEONG/Supervisory Patent Examiner, Art Unit 1751 1/5/2026