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 .
Specification
Applicant is reminded of the proper language and format for an abstract of the disclosure.
The abstract should be in narrative form and generally limited to a single paragraph on a separate sheet within the range of 50 to 150 words in length. The abstract should describe the disclosure sufficiently to assist readers in deciding whether there is a need for consulting the full patent text for details.
The language should be clear and concise and should not repeat information given in the title. It should avoid using phrases which can be implied, such as, “The disclosure concerns,” “The disclosure defined by this invention,” “The disclosure describes,” etc. In addition, the form and legal phraseology often used in patent claims, such as “means” and “said,” should be avoided.
The abstract of the disclosure is objected to because it contains phrases which can be implied ("The present invention" in line 1). A corrected abstract of the disclosure is required and must be presented on a separate sheet, apart from any other text. See MPEP § 608.01(b).
Claim Objections
Claim 1 is objected to because claim 1 does not indent each step that is recited. Claims that set forth a plurality of elements or steps should have each element be separated by a line indentation. See MPEP § 608.01(m).
Claim 10 is objected to because claim 10 recites two sets of temperature ranges, heating rates, and time period for two separate heating steps (lines 3 – 4 for the first set and lines 5 -6 for the second set) and does not indent each step. Claims that set forth a plurality of elements or steps should have each element be separated by a line indentation. See MPEP § 608.01(m).
Appropriate correction is required.
Claim Rejections - 35 USC § 112
The following is a quotation of 35 U.S.C. 112(b):
(b) CONCLUSION.—The specification shall conclude with one or more claims particularly pointing out and distinctly claiming the subject matter which the inventor or a joint inventor regards as the invention.
The following is a quotation of 35 U.S.C. 112 (pre-AIA ), second paragraph:
The specification shall conclude with one or more claims particularly pointing out and distinctly claiming the subject matter which the applicant regards as his invention.
Claims 1 - 10 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.
Claims 1 – 10 recite the limitation “a polyanion type” in line 1. The addition of the word “type” to an otherwise definite expression extends the scope of the expression so as to render it indefinite. Therefore, it is unclear what “type” is intended to convey in the phrase “polyanion type.” Ex parte Attig, 7 USPQ2d 1092 (Bd. Pat. App. & Inter. 1986). See MPEP §2173.05 (b)(III).
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 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.
Claims 1 – 7 are rejected under 35 U.S.C. 103 as being unpatentable over Zhang, et. al. 2020 (CN 111162256 A), referred to as Zhang from herein, in view of Pang, et. al. 2019 (CN 109860572 A), referred to as Pang from herein, and in view of Wu, et. al. 2016 (Sol-Gel Synthesis of Na4Fe3(PO4)2(P2O7)/C Nanocomposite for Sodium Ion Batteries and New Insights into Microstructural Evolution during Sodium Extraction. Journal of Power Sources 2016, 327, 666 – 674), referred to as Wu from herein.
Regarding claim 1, Zhang teaches a method for preparing a polyanion type sodium battery positive electrode material ([0002]) on the basis of an organic acid dissolution method ([0014] describes adding oxalic acid, an organic acid, to dissolve Fe(NO3)3 • 9H2O, sodium acetate (CH3COONa), and ammonium dihydrogen phosphate [NH4H2PO4]), comprising the following steps:
preparing a mixture of a transition metal source, a sodium source, and a polyanion source, and putting the mixture into a reactor ([0014] describes mixing Fe(NO3)3 • 9H2O, a transition metal source, sodium acetate, a sodium source, and ammonium dihydrogen phosphate, a polyanion source; also see [0025])
adding a carbon source stirring ([0019] describes adding graphene oxide in the step wherein Fe(NO3)3 • 9H2O, sodium acetate, and ammonium dihydrogen phosphate are mixed together and before the addition of oxalic acid), and drying to obtain precursor powder ([0015]);
adding organic acid into the reactor and continuously stirring until the transition metal source is completely dissolved ([0014])
heating the precursor powder in an inert gas atmosphere to obtain the polyanion type sodium battery positive electrode material ([0016])
While Zhang adds the carbon source before adding the organic acid, one of ordinary skill in the art would not expect the order in which the carbon source is added to impact the end result and would therefore not expect different results despite differences in the selection of the order of steps between Zhang and the present invention. It is noted that the courts have held that the selection of any order of performing process steps is prima facie obvious in the absence of new or unexpected results. See Ex parte Rubin 128 USPQ 440 (Bd. App. 1959), In re Burhans, 154 F.2d 690, 69 USPQ 330 (CCPA 1946) and In re Gibson, 39 F.2d 975, 5 USPQ 230 (CCPA 1930). See also MPEP § 2144.04.IV.C. It would have been obvious to one of ordinary skill in the art at the time of filing of the invention to perform the method as taught by Zhang comprising adding the carbon source in any order before drying and heating including after adding the organic acid as claimed as a mere difference in the selection of performing process steps absent new and unexpected results.
Zhang does not teach the transition metal source as a transition metal simple substance or a transition metal oxide, heating the dissolution step described in step S2, and cooling the precursor powder to room temperature along with a furnace after the heating treatment.
Pang teaches the transition metal source as a transition metal simple substance or transition metal oxide (Example 2 [0049] – [0053] and Example 3 [0054] – [0058] demonstrate obtaining lithium iron phosphate using iron powder as the transition metal source while Example 4 [0059] – [0063] demonstrates using both iron powder and ferric oxide).
Zhang and Pang are analogous to the present invention as both are in the same field of preparing alkali battery electrode material.
Since both Zhang and Pang both teach methods for preparing polyanion type alkali battery electrode material which includes a transition metal source, it would be obvious for one of ordinary skill in the art before the effective filing date to substitute Fe(NO3)3 • 9H2O in Zhang with iron powder or ferric oxide in Pang. One of ordinary skill in the art would reasonably expect successful results if an iron salt was replaced with iron powder or iron oxide (i.e. ferric oxide). While, Pang demonstrates this with a polyanion type lithium electrode material instead of a polyanion type sodium electrode material, one of ordinary skill in the art would recognize that both sodium and lithium are alkali metals and share very similar properties would reasonably expect successful results for sodium electrode materials if one substituted Fe(NO3)3 • 9H2O with iron powder or ferric oxide, as taught by Pang.
Pang further teaches cooling the precursor powder to room temperature along with a furnace after the heating treatment (described in [0016]).
It would be obvious for one of ordinary skill in the art before the effective filing date to modify the method in Zhang with cooling the precursor to room temperature along with a furnace after the heating treatment, as taught by Pang. While, Pang demonstrates this with a polyanion type lithium electrode material instead of a polyanion type sodium electrode material, one of ordinary skill in the art would recognize that both sodium and lithium alkali metals and share very similar properties and would reasonably expect successful results for sodium electrode materials if the precursor was cooled in the furnace after heating as taught by Pang.
Zhang in view of Pang still does not teach heating the dissolution step described in step S2.
Wu teaches a method for preparing a polyanion type sodium battery material comprising of similar steps to the claimed invention including preparing a mixture of iron metal powder, citric acid, and sodium dihydrogen phosphate dihydrate while heating and stirring; adding ethylene glycol while stirring the mixture and then drying; and calcining (Section titled “Synthesis of Na4Fe3(PO4)2(P2O7)/C nanocomposite” on Pages 667 – 668 describes the synthesis of the polyanion sodium battery material). Wu further discloses heating the mixture comprising of iron metal powder, citric acid, and sodium dihydrogen phosphate dihydrate until dissolved (see Section titled “Synthesis of Na4Fe3(PO4)2(P2O7)/C nanocomposite” on Pages 667 – 668; while not explicitly disclosed, one of ordinary skill in the art would recognize “the solution still remained transparent” implies that the components have dissolved). While Wu does not explicitly use the same terms as the present invention, one of ordinary skill in the art would recognize iron metal as a transition metal source, citric acid as an organic acid, and sodium dihydrogen phosphate dihydrate as both a sodium source and a polyanion source.
Wu is analogous to the present invention as both are in the field of preparing polyanion type sodium battery material.
It would be obvious for one of ordinary skill in the art before the effective filing date to modify the method of Zhang in view of Pang and heat the dissolution step described in step S2, as taught by Wu. The rationale to support a conclusion that the claim would have been obvious is that all the claimed elements were known in the prior art and one skilled in the art could have combined the elements as claimed by known methods with no change in their respective functions, and the combination yielded nothing more than predictable results to one of ordinary skill in the art (MPEP 2143.A.). The simple substitution of one known element for another is likely to be obvious when predictable results are achieved. See KSR International Co. v. Teleflex Inc., 550 U.S. 398, 415-421, USPQ2d 1385, 1395 - 97 (2007) (see MPEP § 2143, B.). Further, one would have a reasonable expectation of success when heating the dissolution step described in step S2, as taught and demonstrated by Wu.
Regarding claim 2, Zhang in view of Pang and in view of Wu teaches a method for preparing a polyanion type sodium battery positive electrode material on the basis of an organic acid dissolution according to claim 1, and Pang further teaches the transition metal source is iron or iron oxides thereof (Example 2 [0049] – [0053] and Example 3 [0054] – [0058] demonstrate obtaining lithium iron phosphate using iron powder as the transition metal source while Example 4 [0059] – [0063] demonstrates using both iron powder and ferric oxide).
Regarding claim 3, Zhang in view of Pang and in view of Wu teaches a method for preparing a polyanion type sodium battery positive electrode material on the basis of an organic acid dissolution according to claim 1, and Zhang further teaches the sodium source is sodium acetate ([0014]).
Regarding claim 4, Zhang in view of Pang and in view of Wu teaches a method for preparing a polyanion type sodium battery positive electrode material on the basis of an organic acid dissolution according to claim 1, and Pang further teaches the polyanion source as phosphoric acid ([0017] provides a list of phosphorus sources which includes phosphoric acid; Example 2 [0049] – [0053] and Example 3 [0054] – [0058] demonstrate obtaining lithium iron phosphate using phosphoric acid as the phosphorus source).
Regarding claim 5, Zhang in view of Pang and in view of Wu teaches a method for preparing a polyanion type sodium battery positive electrode material on the basis of an organic acid dissolution according to claim 1, and Zhang further teaches the organic acid comprising of oxalic acid ([0014] describes adding oxalic acid).
Regarding claim 6, Zhang in view of Pang and in view of Wu teaches a method for preparing a polyanion type sodium battery positive electrode material on the basis of an organic acid dissolution according to claim 1. Zhang further teaches the usage amounts of the transition metal source, the sodium source and the polyanion source comply with the stoichiometric ratio in the chemical formula of the prepared polyanion type sodium battery positive electrode material ([0017] describes using a molar ratio of Fe3+:Na+:PO43- is 2:3:3, which complies with the stoichiometric ratio of the final product, Na3Fe2(PO4)2(P2O7)) and a usage amount of the organic acid is 1-5 times of the molar amount of the added transition metal source ([0018] describes the molar ratio of oxalic acid to Fe(NO3)3 • 9H2O is 2.5 – 3.5: 1, which is within the range in the present invention).
Wu further teaches a usage amount of ethylene glycol is 1 times of the molar amount of added iron powder (see Section titled “Synthesis of Na4Fe3(PO4)2(P2O7)/C nanocomposite” on Pages 667 – 668; 0.01 moles of ethylene glycol and iron powder are mixed together), which is within the recited range of 1 – 3 times. While Wu does not explicitly use the same terms as the present invention, one of ordinary skill in the art would recognize ethylene glycol as a carbon source and iron powder as a transition metal source.
Regarding claim 7, Zhang in view of Pang and in view of Wu teaches a method for preparing a polyanion type sodium battery positive electrode material on the basis of an organic acid dissolution according to claim 1. Wu further teaches step S2 having a heating temperature of 80 ºC (describes heating the mixture to 80 ºC to remove excess water in Section titled “Synthesis of Na4Fe3(PO4)2(P2O7) particles on Page 9).
While Wu does not teach the recited temperature value, one of ordinary skill would recognize that temperature effects the rate of a reaction. Therefore, it would have been obvious to one of ordinary skill in the art before the effective filing date of the claimed invention to optimize the temperature of dissolution described in step S2 to decrease the amount of time it takes for the dissolution to be completed, thereby arriving at the instantly claimed invention. The courts have found that “where the general conditions of a claim are disclosed in the prior art, it is not inventive to discover the optimum or workable ranges by routine experimentation.” In re Aller, 220 F.2d 454, 456, 105 USPQ 233, 235 (CCPA 1955). See MPEP 2144.05 II. Therefore, the claimed value of 90 ºC merely represents an obvious variant and/or routine optimization of the temperature of dissolution.
Furthermore, generally, differences in concentration or temperature will not support the patentability of subject matter encompassed by the prior art unless there is evidence indicating such concentration or temperature is critical. "[W]here the general conditions of a claim are disclosed in the prior art, it is not inventive to discover the optimum or workable ranges by routine experimentation." In re Aller, 220 F.2d 454, 456, 105 USPQ 233, 235 (CCPA 1955)
Claim 8 is rejected under 35 U.S.C. 103 as being unpatentable over Zhang in view of Pang and in view of Wu as applied in claim 1, and in further view of Deng, et. al. 2016 (CN 105845974 A), referred to as Deng from herein.
Regarding claim 8, Zhang in view of Pang and in view of Wu teaches a method for preparing a polyanion type sodium battery positive electrode material on the basis of an organic acid dissolution according to claim 1, and Deng teaches the carbon source as graphene, citric acid, sucrose, or glucose ([0037] lists all potential carbon sources; Examples 1 and 2 from [0053] – [0063] use sucrose as the carbon source; Examples 3 and 4 [0064] – [0074] use graphene as the carbon source; Example 5 [0074] – [0079] uses glucose as the carbon source; Example 6 [0080] – [0084] uses citric acid as the carbon source) where the purpose of the carbon source in is to coat the surface of the NaFePO4 particles to improve the overall electrical conductivity of the material ([0042]).
Deng is analogous to the present invention as both are in the field of preparing polyanion type sodium battery positive electrode material.
Therefore, it would be obvious for one of ordinary skill in the art before the effective filing date to modify the method of Zhang in view of Pang and in view of Wu with the carbon source as taught by Deng to ensure that the carbon source used is able to successfully coat the polyanion type sodium material to improve the overall electrical conductivity. Since Deng provides examples of graphene, citric acid, sucrose, and glucose, it would be reasonable for one of ordinary skill in the art to expect successful results with each disclosed carbon source, as demonstrated by Examples 1 – 5 disclosed in Deng.
Claim 9 is rejected under 35 U.S.C. 103 as being unpatentable over Zhang in view of Pang and in view of Wu as applied in claim 1.
Regarding claim 9, Zhang in view of Pang and in view of Wu teaches a method for preparing a polyanion type sodium battery positive electrode material on the basis of an organic acid dissolution according to claim 1, and Zhang further teaches the inert gas atmosphere in step S4 is argon-hydrogen mixed gas ([0016] describes calcining under Ar-H2 atmosphere)
Claim 10 is rejected under 35 U.S.C. 103 as being unpatentable over Zhang in view of Pang and in view of Wu as applied in claim 1, and in further view of Deng.
Regarding claim 10, Zhang in view of Pang and in view of Wu teaches a method for preparing a polyanion type sodium battery positive electrode material on the basis of an organic acid dissolution according to claim 1, and Deng teaches the heating treatment process in step S4 is as follows:
a temperature is increased to 300ºC – 400ºC ([0014] describes the temperature range of the first sintering step) at a heating rate of 1 – 10 ºC/min ([0019] describes heating rate range for both sintering steps) and then maintained for 3 – 5 hours ([0014] describes the length of time the temperature is held for the first sintering step)
and the temperature is further increased to 500ºC – 800ºC ([0014] describes the temperature range of the second sintering step) at a heating rate of 1 – 10 ºC/min ([0019] describes heating rate range for both sintering steps) and then maintained for 4 – 20 hours ([0014] describes the length of time the temperature is held for the second sintering step).
Deng further teaches of the benefits of using a two-step heating process disclosing that the two-step process partially decomposes the carbon source to allow the carbon to uniformly coat the surface of the precursor, which is NaFePO4. This uniform film hinders the agglomeration of powder and the growth of NaFePO4 during the second heating step, resulting in product with high crystallinity, reduced particle size and uniform size distribution ([0026]) Deng further discloses a comparative example, demonstrating that a one-step heating process results in a product with more impurities and poorer electrochemical performance ([0090]).
It would be reasonable for one of ordinary skill in the art before the effective filing date to modify the method of Zhang in view of Pang and in view of Wu with the two-step heating process taught by Deng to obtain product with high crystallinity and uniform size distribution while avoiding the formation of impurities.
The temperature range and time range for the first step represented by Deng have overlapping endpoints. It is noted that the courts have stated where the claimed ranges “overlap or lie inside the ranges disclosed by the prior art” a prima facie case of obviousness exists (see In re Wertheim, 541 F.2d 257, 191 USPQ 90 (CCPA 1976); In re Woodruff, 919 F.2d 1575, 16 USPQ2d 1934 (Fed. Cir. 1990); Titanium Metals Corp. of America v. Banner, 778 F2d 775. 227 USPQ 773 (Fed. Cir. 1985) (see MPEP 2144.05.01). Therefore, the claimed range of 200ºC – 300ºC for the temperature range and 3 hours for the time maintained in step one merely represent obvious variants and/or routine optimization of the values of the cited prior art.
The temperature range for the second step represented by Deng overlaps with the present invention. It is noted that the courts have stated where the claimed ranges “overlap or lie inside the ranges disclosed by the prior art” a prima facie case of obviousness exists (see In re Wertheim, 541 F.2d 257, 191 USPQ 90 (CCPA 1976); In re Woodruff, 919 F.2d 1575, 16 USPQ2d 1934 (Fed. Cir. 1990); Titanium Metals Corp. of America v. Banner, 778 F2d 775. 227 USPQ 773 (Fed. Cir. 1985) (see MPEP 2144.05.01). Therefore, the claimed range of 400ºC – 550ºC for the temperature range for the second step and merely represent an obvious variant and/or routine optimization of the values of the cited prior art.
The heating rate range and the time range for the second step represented by Deng are broader than the present invention. It is noted that the courts have stated where the claimed ranges “overlap or lie inside the ranges disclosed by the prior art” a prima facie case of obviousness exists (see In re Wertheim, 541 F.2d 257, 191 USPQ 90 (CCPA 1976); In re Woodruff, 919 F.2d 1575, 16 USPQ2d 1934 (Fed. Cir. 1990); Titanium Metals Corp. of America v. Banner, 778 F2d 775. 227 USPQ 773 (Fed. Cir. 1985) (see MPEP 2144.05.01). Therefore, the claimed range of 2 – 5 ºC/min and the value of 2 ºC/min for the heating rates and the claimed value of 10 hours for the time maintained for the second step merely represent obvious variants and/or routine optimization of the values of the cited prior art.
Citation of Pertinent Prior Art
The prior art made of record and not relied upon is considered pertinent to applicant's disclosure.
Yuan, et. al. 2019 (3D Graphene Decorated Na4Fe3(PO4)2(P2O7) Microspheres as Low-Cost and High-Performance Cathode Materials for Sodium-Ion Batteries Nano Energy 2019, 56, 160 – 168) teaches the preparation of graphene oxide confined Na4Fe3(PO4)2(P2O7) and conducted electrochemical experiments to determine the potential of using this material as a cathode for a sodium-ion battery.
Chen, et. al. 2019 (NASICON-type air-stable and all-climate cathode for sodium-ion batteries with low cost and high-power density, Nature Communications 2019, 10, 1480) teaches the preparation and electrochemical characterization of Na4Fe3(PO4)2(P2O7)/C nanocomposites.
Conclusion
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/V.F.C./Examiner, Art Unit 1738
/MICHAEL FORREST/Primary Examiner, Art Unit 1738
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