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 Amendment
Applicant amended claims 1, 9, 13-15, 19 and 21, and added new claims 25-27; claims 6, 8, 12, 16, 18, and 23-24 are cancelled.
Claims 1-5, 7, 9-11, 13-15, 17, 19-23, and 25-27 are pending and considered in the present Office action.
The 103 rejections are withdrawn. However, upon further consideration a new ground of rejection is necessitated by amendment.
Response to Arguments
Applicant’s argument that Kazacos fails to suggest both the molar concentration of sulfonic acid and the redox metal is not persuasive. The concentration of the sulfonic acid was addressed under the rejection of claim 19, see e.g., page 12 of the last Office action. In short, Kazacos suggests the molar concentration of sulfonic acid is 0.01M-10M, see e.g., col. 12. Further, Kazacos discloses the concentration of the redox metal ions (vanadium species) as well in col. 12-13; specifically, the concentration of the redox metal ions is 0.001M-15M, thereby allowing high discharge capacity.
Applicant’s comments regarding the rejection of Claim 19 and Peng are moot because this reference was not used in the rejection.
Applicant’s conclusion Clark (specifically, claim 21) teaches away from the presence of sulfuric acid, as recited in instant claims 3 and 19, is not persuasive because disclosed examples and preferred embodiments (e.g., claim 21 of Clark) do not constitute a teaching away from a broader disclosure or nonpreferred embodiments, see MPEP 2123. First, Kazacos suggests the use of both methanesulfonic acid and sulfuric acid, and the concentration of each compound, see e.g., col. 12, where the molar concentration of sulfonic acid is 0.01M-20M and the molar concentration of sulfuric acid is 1.5M-10M; thus, Kazacos alone suggest the features of instant claims 3 and 19. Second, Clark supports the use of both methanesulfonic acid and sulfuric provided both acids offer acidity to the electrolyte and improved solubility of the redox metal ions in the electrolyte, see e.g., [0023-0024, 0031-0032].
Applicant’s arguments with respect to claim 13 are not persuasive. Claim 13 lists the compounds as ammonium salts, i.e., ammonium sulfate, ammonium phosphate, ammonium oxalate, ammonium hypophosphate, ammonium phosphate, ammonium asparate, ammonium hydrogen phosphate, ammonium acetate, ammonium nitrate, ammonium tartarate; that is, the cation of each compound is “ammonium” (NH4+). However, claim 13 also suggests the compounds may be sodium or potassium salts; that is, the cation of each compound is either “sodium” or “potassium” (instead of ammonium). In other words, the compounds may also be selected from sodium sulfate, sodium phosphate, sodium oxalate, sodium nitrate, potassium sulfate, potassium phosphate, potassium nitrate, etc.
Applicant’s argument that claims 14 and 15 are allowable because the references fail to disclose the sulfonic acid is methanesulfonic acid is not persuasive because Kazacos suggests the sulfonic acid is methanesulfonic acid, see e.g., col 12.
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.
A broad range or limitation together with a narrow range or limitation that falls within the broad range or limitation (in the same claim) may be considered indefinite if the resulting claim does not clearly set forth the metes and bounds of the patent protection desired. See MPEP § 2173.05(c). In the present instance, claim 27 recites the broad recitation “at least one inorganic additive”, and the claim also recites “a mixture of potassium phosphate and sodium hexametaphosphate” which is the narrower statement of the range/limitation. The claim(s) are considered indefinite because there is a question or doubt as to whether the feature introduced by such narrower language is (a) merely exemplary of the remainder of the claim, and therefore not required, or (b) a required feature of the claims. Examiner assumes “an inorganic additive… comprising a mixture of potassium phosphate and sodium hexametaphosphate”.
Claim Rejections - 35 USC § 103
Claim(s) 1-5, 7, 9-11, 13, 17, and 25-26 is/are rejected under 35 U.S.C. 103 as being unpatentable over Kazacos et al. (US 6,143,443, of record).
Regarding Claims 1-5, 7, 10-11, 17, and 25-26, Kazacos suggests an electrochemical cell (i.e., a vanadium redox flow battery, e.g., col. 12 lines 40-44) including a negative electrode, a positive electrode, and an electrolyte composition (see e.g., title, cols. 6-7, col. 11) comprising: 0.08M to 8M (e.g., 0.01M-10M, col. 12) of a sulfonic acid of formula R-SO3H, in which R represents a (C1-C4) alkyl or a (C6-C14) aryl optionally substituted with a (C1-C4) alkyl (e.g., alkyl sulfonic acid, methyl sulfonic acid, ethyl sulfonic acid, aryl sulfonic acid, benzene sulfonic acid, naphthalene sulfonic acid, toluene sulfonic acid), optionally sulfuric acid (i.e., H2SO4, see e.g., col. 12 lines 45-62, col. 103 lines 21-35, where sulfonic acid and sulfuric acid are considered as a mixture), 0.1 M to 15 M (e.g., 0.001M – 15M) of redox metal ions (i.e., various species of vanadium, e.g., V(II), V(III), etc., col. 12 line 63 to col. 13 line 55, col. 104 lines 57-58), at least one inorganic additive (A) comprising at least one phosphorus atom whose oxidation state is less than or equal to +5 (i.e., stabilizing agent, e.g., orthophosphoric acid, sodium hexametaphosphate, phosphoric acid, pyrophosphate, polyphosphoric acid, ammonium phosphate, etc., see e.g., col. 13 lines 41-42, 57-60, claims 1, 6, 11, 12-18) in an amount of 0.5% to 5 % (or 0.5% to 3 %) by weight relative to the total weight of the electrolyte composition (e.g., 0.5-3 % by weight overlaps with that claimed, col. 97 line 37 to col. 98 line 14, col. 110 line19, claims 17-18), and water (i.e., “aqueous solution”), see col. 12-14, 102-104, Tables, and claims. The concentration values and amount of A suggested in the prior art overlaps with that claimed, or is close, thus a prima facie case of obviousness exists. See MPEP 2144.05.
Regarding Claim 9, Kazacos suggests a corrosion inhibitor having a general formula (1) or (2): NO2X (1) or NO3X (2) in which X is chosen from: K or NH4 (see e.g., claim 13 where NH4NO3 (ammonium nitrate) and KNO3 (potassium nitrate) are explicitly disclosed).
Regarding Claim 13, the positively recited features of the electrolyte composition in the method claim overlaps with that of claim 1; considering the features have already been addressed under the rejection of claim 1, they are not repeated here for brevity. The preamble of claim 13 (e.g., “for stabilizing … between 0 °C and 60°C) appears to recite purpose or intended use, thus not considered a limitation and is of no significance to claim construction, see MPEP 2111.02. In the alternative, Kazacos suggest the intended purpose set forth in the preamble of claim 13, see e.g., abstract, col. 2, and 11-12, which suggests a method for stabilizing an electrolyte composition at a temperature between 0 °C and 60 °C, see also tables (and discussions thereof), claim 1, col. 105 lines 1-15, col. 118 lines 53-67.
Claim(s) 14, and 21-22 is/are rejected under 35 U.S.C. 103 as being unpatentable over Kazacos (cited earlier) in view of Peng et al. (Int. J. Electrochem. Sci., 7 (2012) 643 – 649, of record), hereinafter Peng.
Regarding Claims 14, and 21-22, Kazacos suggests an electrochemical cell (i.e., a vanadium redox flow battery, e.g., col. 12 lines 40-44) including a negative electrode, a positive electrode, and an electrolyte composition as set forth under the rejection of claims 1 and 3. Further, Kazacos suggests a mixture of sulfonic acid and sulfuric acid, where the sulfonic acid is methanesulfonic acid, see e.g., col. 12. Kazacos does not suggests a specific mole ratio of the sulfonic acid to sulfuric acid. However, Peng uses a methanesulfonic acid/sulfuric acid mixed solution in the electrolyte of a vanadium redox flow battery; a molar ratio of the methanesulfonic acid to the sulfuric acid of 1.5M/1.5M (see experimental page 644) improved electrochemical activity of the electrolyte by increasing the kinetics of the redox reaction and reducing mass transport resistance, and improved the energy density of the cell, see conclusions on page 648, and page 647. It would be obvious to one having ordinary skill in the art the molar ratio of methanesulfonic acid to sulfuric acid in Kazacos is 1/1, with the expectation of improving the electrochemical activity of the electrolyte, as suggested by Peng.
Claim(s) 15 is/are rejected under 35 U.S.C. 103 as being unpatentable over Kazacos and Peng in view of He et al. (Electrochimica Acta 106 (2013) 556– 562, of record), hereinafter He.
Regarding Claim 15, as set forth under the rejection of claim 14 Kazacos as modified by Peng suggests the molar ratio of methanesulfonic acid to sulfuric acid (i.e., 1.5M/1.5M (which is equivalent to the claimed 50/50, which simplifies to 1/1 or 1)); the modification does not suggest the molar ratio of methanesulfonic acid to sulfuric acid is between 5/95 to 15/85 (i.e., ~0.05 to ~0.18). However, Peng has recognized larger molar ratios of methanesulfonic acid to sulfuric acid (e.g., 1.5M/1.5M (i.e., 50/50)) results in improved electrochemical activity, see e.g., conclusions. He discloses the combination of methanesulfonic acid and sulfuric acid in the electrolyte of vanadium redox flow batteries; the amount of methanesulfonic acid to sulfuric acid, even at a very small molar ratio (i.e., 0.0004 M/3M (0.0001)), results in improved thermal stability and electrochemical performance, see e.g., page 557. It would be obvious to one having ordinary skill in the art to utilize a small molar amount of methanesulfonic acid with respect to sulfuric acid with the expectation of improving electrochemical performance, as suggested by Peng and He. Further, the prior art (Peng and He) has recognized that molar ratio of sulfonic acid and sulfuric acid (between 0.0004M/3 M to 1.5M/1.5M, i.e., 0.0001 to 1) is a result effective variable for electrochemical performance. The presence of a known result-effective variable would be motivation for a person of ordinary skill in the art to experiment to reach another workable product or process (i.e., thereby reaching the claimed molar ratio between 0.05 to 0.17). 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). MPEP 2144.05, II.
Claim(s) 19 is/are rejected under 35 U.S.C. 103 as being unpatentable over Kazacos in view of Clark et al. (US 2006/0063065, of record), hereinafter Clark.
Regarding Claims 19, Kazacos suggests the sulfonic acid is methanesulfonic acid and the molar concentration thereof is between 0.1 M and 4 M (e.g., 0.01M to 10M), and the sulfuric acid molar concentration is between 0.1 M and 4 M (e.g.,1.5M to 10M), see e.g., col. 12. Further, Clark contemplates sulfuric and sulfonic acids for the vanadium redox couples; methane sulfonic acid (MSA) is suitable at a molar concentration range of 0.1 M to 4M, see e.g., [00120021, 0031-0031], thereby allowing the metal ions to dissolve, [0024]. It would be obvious to one having ordinary skill in the art to utilize a molar concentration of 0.1M to 4M for each of the sulfuric acid and the sulfonic acid with the expectation of dissolving the vanadium ions into the electrolyte, as suggested by Kazacos and Clark.
Claim(s) 20 is/are rejected under 35 U.S.C. 103 as being unpatentable over Kazacos (cited earlier) in view of Rahman et al. (Journal of Power Sources 340 (2017) 139–149, of record), hereinafter Rahman.
Regarding Claim 20, Kazacos suggests the additive is sodium hexametaphosptae (SHMP), but does not suggest the additive is a mixture of potassium phosphate and sodium hexametaphosphate; however, Rahman suggests an additive in the vanadium flow battery electrolyte comprising a mixture of potassium phosphate and sodium hexametaphosphate, e.g., KS11 showed the best performance with only a 2% decrease in the concentration of vanadium after 40 days, see e.g., page 146 and conclusions on page 148. Kazacos suggests the combination of potassium phosphate and sodium hexametaphosphate delays precipitation at various temperatures, see e.g., various samples and data in Tables. It would be obvious to one having ordinary skill in the art the additive is a mixture of potassium phosphate and sodium hexametaphosphate because there is an expectation of minimizing precipitation of highly saturated vanadium solution in vanadium flow battery applications, as suggested by Rahman.
Claim(s) 27 is/are rejected under 35 U.S.C. 103 as being unpatentable over Kazacos, Peng, and Rahman (all cited earlier).
Regarding Claim 27, Kazacos suggests an electrolyte composition (see e.g., title, cols. 6-7, col. 11) comprising: 0.08M to 8M (e.g., 0.01M-10M, col. 12, line 51-54) of a sulfonic acid comprising methane sulfonic acid (col. 12, line 49-54), sulfuric acid (i.e., H2SO4, see e.g., col. 12 lines 45-62, col. 103 lines 21-35), and redox metal ions selected from V2+, V3+ (i.e., various species of vanadium, e.g., V(II), V(III), etc., col. 12 line 63 to col. 13 line 55, col. 104 lines 57-58), an inorganic additive (A) comprising a phosphorus atom whose oxidation state is less than or equal to +5 (i.e., stabilizing agent, e.g., orthophosphoric acid, sodium hexametaphosphate, phosphoric acid, pyrophosphate, polyphosphoric acid, ammonium phosphate, etc., see e.g., col. 13 lines 41-42, 57-60, claims 1, 6, 11, 12-18) in an amount of 0.5% to 5 % by weight relative to the total weight of the electrolyte composition (e.g., 0.5-3 % by weight overlaps with that claimed, col. 97 line 37 to col. 98 line 14, col. 110 line19, claims 17-18), and water (i.e., “aqueous solution”), see col. 12-14, 102-104, Tables, and claims. The concentration value and amount of A suggested in the prior art overlaps with that claimed, or is close, thus a prima facie case of obviousness exists. See MPEP 2144.05.
Kazacos does not suggest the molar ratio of methanesulfonic acid to sulfuric acid. However, Peng uses a methanesulfonic acid/sulfuric acid mixed solution in the electrolyte of a vanadium redox flow battery; a molar ratio of the methanesulfonic acid to the sulfuric acid of 1.5M/1.5M (see experimental page 644) improved electrochemical activity of the electrolyte by increasing the kinetics of the redox reaction and reducing mass transport resistance, and improved the energy density of the cell, see conclusions on page 648, and page 647. It would be obvious to one having ordinary skill in the art the molar ratio of methanesulfonic acid to sulfuric acid in Kazacos is 1/1, with the expectation of improving the electrochemical activity of the electrolyte, as suggested by Peng.
Kazacos suggests the additive is sodium hexametaphosptae (SHMP), but does not suggest the additive is a mixture of potassium phosphate and sodium hexametaphosphate; however, Rahman suggests an additive in the vanadium flow battery electrolyte comprising a mixture of potassium phosphate and sodium hexametaphosphate, e.g., KS11 showed the best performance with only a 2% decrease in the concentration of vanadium after 40 days, see e.g., page 146 and conclusions on page 148. Kazacos suggests the combination of potassium phosphate and sodium hexametaphosphate delays precipitation at various temperatures, see e.g., various samples and data in Tables. It would be obvious to one having ordinary skill in the art the additive is a mixture of potassium phosphate and sodium hexametaphosphate because there is an expectation of minimizing precipitation of highly saturated vanadium solution in vanadium flow battery applications, as suggested by Rahman.
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.
Any inquiry concerning this communication or earlier communications from the examiner should be directed to ANNA KOROVINA whose telephone number is (571)272-9835. The examiner can normally be reached M-Th 7am - 6 pm.
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/ANNA KOROVINA/Examiner, Art Unit 1729
/ULA C RUDDOCK/Supervisory Patent Examiner, Art Unit 1729
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