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 .
Claim Objections
Claims 1 and 2 are objected to because of the following informalities:
Claim 1 recites the limitation, “to obtain the composite adhesive, namely the VC composite adhesive,” in line 12. The phrasing appears redundant as throughout the claims only VC composite adhesive is used, and it is suggested for clarity that the limitation is simplified to read as, “to obtain the VC composite adhesive.”
Claim 2 recites the limitation, “the lithium source is any one or more selected from a group consisting of lithium hydroxide, lithium bicarbonate, lithium sulfate, and lithium hydroxide” in lines 5-7. The recitation of lithium hydroxide twice is redundant and appears to have been a typographical error.
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.
The claims are generally narrative and indefinite, failing to conform with current U.S. practice. They appear to be a literal translation into English from a foreign document and are replete with grammatical and idiomatic errors. A non-exhaustive list of said errors are provided herein:
Claim 1 recites the limitation, “after reaction,” in line 7. There is insufficient antecedent basis for this limitation in the claim as it is unclear to if “reaction” refers to the raising of the pH or another step after the alkali liquor is added to the mixed salt solution.
Claim 1 recites the limitation, “the sieved granulated particles,” in line 18. There is insufficient antecedent basis for this limitation in the claim.
Claim 1 recites the term “high” in line 15, which is a relative term and renders the claim indefinite. The term “high” is not defined by the claim, the specification does not provide a standard for ascertaining the requisite degree, and one of ordinary skill in the art would not be reasonably apprised of the scope of the invention. As a result, it is unclear what stirring speeds would be considered high speed for the purpose of homogenizing the mixture of lithium-intercalated salt precursor slurry and VC composite adhesive in step 2B.
Claim 3 recites the limitation, “the addition amount,” in lines 1-2. There is insufficient antecedent basis for this limitation in the claim.
Claim 3 recites the limitation, “the molar ratio of aluminum to lithium,” in lines 2-3. There is insufficient antecedent basis for this limitation in the claim.
Claim 4 recites the limitation, “the mass concentration,” in line 4. There is insufficient antecedent basis for this limitation in the claim.
Claim 4 recites the limitation, “the addition amount,” in line 7. There is insufficient antecedent basis for this limitation in the claim.
Claim 4 recites the limitation, “the addition amount of the adjuvant is controlled as 0%-10% by mass,” in line 7. However, claim 1 appears to require an adjuvant. Therefore, it is not clear whether the adjuvant in step 2A is an optional ingredient or is required by the claims.
Claim 5 recites the limitation, “the mass concentration,” in line 3. There is insufficient antecedent basis for this limitation in the claim.
Claim 5 recites the limitation, “the mass ratio,” in line 4. There is insufficient antecedent basis for this limitation in the claim.
Claim 5 recites the limitation, “the ratio,” in line 5. There is insufficient antecedent basis for this limitation in the claim.
Claim 5 recites the limitation, “in molded material,” in line 6. There is insufficient antecedent basis for this limitation in the claim.
Claim 6 recites the limitation, “the ultrasonic frequency is 20KHZ-60KHZ,” in lines 2-3. There is a lack of clarity as to whether, “the ultrasonic frequency,” refers only to the frequency of ultrasonic stirring in step 2B), to ultrasonic stirring in step 1, or both.
Claim 8 recites the limitation, “the mass concentration,” in line 3. There is insufficient antecedent basis for this limitation in the claim.
Claim 8 recites the limitation, “the crosslinking time,” in line 4. There is insufficient antecedent basis for this limitation in the claim.
Claims 2, 7, 9 and 10 are rejected via their dependence from rejected claim 1.
Claim Rejections - 35 USC § 103
The following is a quotation of the appropriate paragraphs of 35 U.S.C. 102 that form the basis for the rejections under this section made in this Office action:
A person shall be entitled to a patent unless –
(a)(1) the claimed invention was patented, described in a printed publication, or in public use, on sale, or otherwise available to the public before the effective filing date of the claimed invention.
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.
Claims 1-3, 6-7, and 9-10 are rejected under 35 U.S.C. 103 as being unpatentable over Chinese Patent Pub. No. CN113926419A (Provided machine translation cited here) in view of Zheng et al. (Nanomaterials, 2021, 11, 2668) Ding et al. (Chemical Engineering Journal, 2021, 426, 131689).
In regard to claim 1, CN113926419A, herein referred to as CN ‘419A, teaches a method of making an aluminum-based lithium adsorbent comprising ultrasonically mixing an aluminum source (polymerized aluminum salt), a lithium source (soluble lithium salt), and water to form a mixed salt solution [n0015]-[n0016], combining an alkaline liquor with the mixed salt solution to form an intermediate slurry with a final pH between 3-12 [n0017]-[n0018]. The instantly claimed final pH value range of 6-9 is encompassed by the range taught in CN ’419A, and one of ordinary skill in the art at the time of invention would have found it obvious to select the portion of the prior art’s range which is within the range of the applicants’ claims because it has been held prima facie case of obviousness to select a value in a known range by optimization for the results. In re Aller, 105 USPQ 233. Additionally, the subject matter as a whole would have been obvious to one of ordinary skill in the art at the time invention was made to have selected the overlapping portion of the range disclosed by the reference because overlapping ranges have been held to be a prima facie case of obviousness. In re Malagari, 182 USPQ. CN ‘419A also teaches washing the adsorbent material, vacuum drying the adsorbent material, activating the material by heating to 50°C in DI water, and a second vacuum drying step [n0043]. These steps read to the instantly claimed limitations of step 3. While CN ‘419A does not explicitly describe dehydrating the material, the vacuum drying taught by CN ‘419A leads to a loss of water, i.e. dehydration of the material. It is the examiner’s position that the taught vacuum drying step reads to the, “dehydrating” instantly claimed in claim 1, line 21.
CN ‘419A does not teach steps 2a-d. However, Zheng et al. teaches the preparation of a graphene oxide/chitosan/PVA nanofiber composite film for use as a lithium adsorbent comprising the steps of forming an initial modified graphene oxide adsorbent material, preparing an adhesive solution by dissolving a biological polysaccharide (chitosan) and an adjuvant (acetic acid) in room temperature water, dissolving an aqueous additive (polyvinyl alcohol; PVA) in hot (60°C) water, combining the two mixtures and mixing to form a single homogenous CS-PVA solution, adding a slurry of prepared lithium adsorbent (modified graphene oxide) to the CS-PVA mixture and stirring for 1 hour, cooling to room temperature, and using ultrasound to remove bubbles and obtain a blended slurry (pp. 4, Section 2.2.3). The recited treatment steps read to the instantly claimed steps 2A and 2B. Zheng et al. further teaches molding the slurry into a specific shape, treating with 1% NaOH solution to coagulate the slurry into a gel film, washing with distilled water, freezing, and freeze-drying the material to obtain a lithium adsorbent material (pp. 4, Section 2.2.3). The recited treatment steps read to parts of instantly claimed step 2C (use of a receptor fluid) and step 3 (drying, dehydrating, & washing). CN ‘419A forms a solid, powdered aluminum salt lithium extraction adsorbent. Zheng et al. teaches that such solid adsorbents suffer from poor fluidity and permeability, and low dissolution rate during acid elution regeneration, limiting their industrial applicability (pp. 2, lines 8-13). As a solution, Zheng et al. teaches that formation of a composite can increase the available adsorption sites and improve stability over time. Therefore, it would have been obvious to one of ordinary skill in the art at the relevant time to modify the taught aluminum salt adsorbent by embedding it in a chitosan-PVA matrix as taught by Zheng et al. in order to improve the physical properties of the adsorbent. In combining the processes of CN ‘419A and Zheng et al., it would have been obvious to one of ordinary skill in the art based on the introduction of the modified graphene oxide as a dispersed slurry to the other ingredients, to simply use the intermediate slurry of CN ‘419A for the subsequent steps laid out in Zheng et al. instead of separating and drying the material as taught in CN ‘419.
The combined teaches of CN ‘419 and Zheng et al.’s process differs from the instantly recited preparation method in that it does not employ a granulating step (step 2C) or a cross-linking step (step 2D). However, Ding et al. teaches a granulating process and cross-linking strategy for a solid adsorbent and chitosan material for lithium adsorption from aqueous media. To form stable granules, Ding et al. teaches forming a slurry of a Li4Mn5O12 (LMO, i.e. a lithium adsorbent material), chitosan (i.e. biological polysaccharide), and acetic acid (i.e. adjuvant), dropping the blended slurry into a receptor fluid (1 M NaOH) via a dropper/burette (granulating device for molding), and conducting a cross-linking reaction by adding the formed granules into DI water and mixing with ethylene glycol diglycidyl ether (EDGE), and finally drying the material (pp. 2, right col., lines 14-21, and pp. 3, Fig. 1). The described process reads to the instantly claimed limitations of step 2C and 2D.
Ding et al. posits that while chitosan is an effective and appropriate support material for powdery lithium adsorbent materials, it suffers from its inherent sensitivity to acidic conditions due to the reaction between acidic molecules and the available -OH sites along the chitosan chain (pp. 2, left col., lines 27-30). Ding et al. states that particles with a small diameter can provide higher surface areas, providing more effective adsorption sites (pp. 4, right col., line 12 – pp. 5, left col., line 2). Ding et al. further states that the granulating and cross-linking strategy employed improves both acidity and alkalinity resistance in the prepared adsorbent materials (pp. 5., right col., line 14 – pp. 6, left col., line 2). Therefore, it would have been obvious to modify the combined teachings of CN ‘419 and Zheng et al. further to granulate the slurry and treat the resulting granules with a cross-linking solution as suggested by Ding et al., instead of the thin film preparation taught by Zheng et al., to produce a material more resilient to the operating conditions of lithium extraction.
The combined teachings of CN ‘419A, Zheng et al., and Ding et al. does not teach a sieving step between granulating and cross-linking the material as instantly claimed. However, a person of ordinary skill in the art would be capable of implementing a sieving step in order to tightly control the particle size of the resulting granular adsorbent material. As taught by Ding et al., particle size/diameter is related to the effective specific area of the adsorbent material and affects the available adsorption sites (pp. 4, right col., line 12 – pp. 5, left col., line 2). Therefore, a person of ordinary skill would have been motivated to optimize the formed adsorbent granules for a specific particle diameter, and could achieve so through the routine process of sieving, which eliminates particles of an unwanted size.
As all limitations of steps 1, 2a-d, and 3 are taught or made obvious over the combined teachings of CN ‘419A (steps 1 & 3), Zheng et al. (steps 2a-b), and Ding et al. (steps 2c-d), claim 1 would have been obvious to a person of ordinary skill at the time of filing.
In regard to claim 2, CN ‘419A teaches that the aluminum source of step 1 may be polyaluminum chloride or polyaluminum ferric chloride [n0024], the lithium source may be lithium hydroxide or lithium sulfate [n0025], and the alkali liquor may be an aqueous solution of sodium hydroxide or potassium hydroxide with a concentration of 0.5-20 mol/L, which encompasses the instantly claimed concentration range of 1-5 mol/L ([n0018] & [n0026]). With respect to the quality of the aluminum source, CN ‘419A does not disclose that the polyaluminum chloride or polyaluminum ferric chloride is of food- or drinking water-grade, but it also does not limit the aluminum sources to exclusively be waste products. However, it would have been obvious to a person of ordinary skill in the art to utilize food- or drinking water-grade aluminum sources, i.e. not contaminated with toxic substances, in any instance wherein the lithium extracted using the adsorbent material is for human consumption. With respect to the encompassing and overlapping ranges previously discussed, the subject matter as a whole would have been obvious to one of ordinary skill in the art at the time of invention to select the portion of the prior art’s range which is within the range of the applicants’ claims because it has been held prima facie case of obviousness to select a value in a known range by optimization for the results. In re Aller, 105 USPQ 233. Additionally, the subject matter as a whole would have been obvious to one of ordinary skill in the art at the time invention was made to have selected the overlapping portion of the range disclosed by the reference because overlapping ranges have been held to be a prima facie case of obviousness. In re Malagari, 182 USPQ.
In regard to claim 3, CN ‘419A teaches that the aluminum source and lithium source may be added in a Li/Al ratio of 0.1-5:1, which overlaps the instantly claimed range of 1.5-6.5:1 Li/Al [n0016]. CN ‘419A also teaches that the aluminum source and lithium sources may be added to water so that the aluminum ion concentration is 0.1-10 M (equivalent to 2-72 wt% when source is polyaluminum chloride), and the lithium ion concentration is 0.1-15 M (equivalent to 0.4-29 wt% when source is lithium hydroxide) [n0016]. At minimum, the total solid content of an aluminum and lithium solution taught by CN ‘419A could be 2.4 wt% and is necessarily less than 100%. The broad disclosure of aluminum and lithium ion concentrations overlaps the instantly claimed solid content of the mixed salt solution. With respect to the encompassing and overlapping ranges previously discussed, the subject matter as a whole would have been obvious to one of ordinary skill in the art at the time of invention to select the portion of the prior art’s range which is within the range of the applicants’ claims because it has been held prima facie case of obviousness to select a value in a known range by optimization for the results. In re Aller, 105 USPQ 233. Additionally, the subject matter as a whole would have been obvious to one of ordinary skill in the art at the time invention was made to have selected the overlapping portion of the range disclosed by the reference because overlapping ranges have been held to be a prima facie case of obviousness. In re Malagari, 182 USPQ. It would have been obvious to one of ordinary skill in the art at the relevant time to adopt the operating parameters discussed by Zheng et al. in the combined teachings of CN ‘419A and Zheng et al. as the parameters have been demonstrated to effectively create a polymer matrix which supports the adsorbent material.
In regard to claim 7, CN ‘419A does not teach process parameters for step 2c. However, Ding et al. teaches the use of a receptor fluid that is an aqueous solution of sodium hydroxide as instantly claimed (pp. 2, right col., lines 16-17). The solution taught was 1.0 M NaOH, which has a pH of 14, and is outside the instantly claimed range of 10-13. However, Ding et al. shows experimentally that over time, the adsorbent material is degraded in strongly alkaline solutions (pp. 5, Fig. 6). Therefore, a person of ordinary skill in the art would understand that acidic and alkaline extremes would be damaging to the adsorbent material, and work to optimize the synthesis scheme to prevent unnecessary material loss before it can be used. However, a certain alkalinity is required in order to effectively granulate the material. Therefore, it would have been obvious to a person of ordinary skill in the art at the relevant time to choose the instantly claimed range of pH of the receptor fluid, 10-13, through process optimization, since it has been held that there the general conditions of a claim are disclosed in the prior art, discovering the optimum or workable ranges involves only routine skill in the art. See In re Boesch, 205 USPQ 215.
In regard to claim 9, CN ‘419A teaches that the adsorbent material is dried via vacuum drying [n0023]. CN ‘419A is silent to the water content of the lithium-intercalated aluminum slat adsorbent material after drying, and does not specify it is 20-80 wt%. However, CN ‘419A states that the lithium-intercalated aluminum salt adsorbent is a hydrate [n0005], meaning that even after drying it must contain a certain amount of water in the final material. It would have been obvious to one having ordinary skill in the art at the time the invention was made to choose the instantly claimed water content through process optimization, since it has been held that there the general conditions of a claim are disclosed in the prior art, discovering the optimum or workable ranges involves only routine skill in the art. See In re Boesch, 205 USPQ 215.
In regard to claim 10, the combined teachings of CN ‘419A, Zheng et al., and Ding et al. render obvious an adsorbent material containing a lithium-intercalated aluminum salt, a biological polysaccharide, an adjuvant, an aqueous additive with a crosslinked, polymeric, and granular structure. Therefore, the combined teachings of CN ‘419A, directed to an aluminum salt lithium extraction adsorbent, Zheng et al., drawn to an adsorbent-chitosan-PVA adsorbent material, and Ding et al., drawn to a cross-linked, granular adsorbent-chitosan material, render obvious claim 10, as all of the structural limitations of claim 1 have been addressed. See above rejection of claim 1.
Claim 6 is rejected under 35 U.S.C. 103 as being unpatentable over CN '419A, Zheng et al., and Ding et al., as applied to claim 1 above, and further in view of Builliard-Sauret et al. (Experimental Thermal and Fluid Science, 2019, 104, pp. 258-271).
The combined teachings of CN ‘419A, Zheng et al., and Ding et al., are silent to the stirring speed and the frequency employed for ultrasonic treatment (generically reported as stirring and ultrasound treatment; Zheng et al., pp. 4, Section 2.2.3). However, determination of an appropriate stirring speed to keep the solid materials dispersed, as stated by Zheng et al., is of routine skill in the art. Furthermore, it is understood by a person of ordinary skill in the art that low frequency ultrasound agitation (generally 20 kHz to 40 kHz) is a typical low frequency employed for optimal stirring via ultrasound agitation. As taught by Bulliard-Sauret et al., ultrasonic irradiation at 25 kHz was effective at generating acoustic cavitation (i.e. disturbance of a liquid via oscillating gas vapors) which is most often employed as a stirring technique in various industries (pp. 258, Abstract & pp. 259, left col., 2nd paragraph). Therefore, it would have been obvious to one of ordinary skill in the art at the relevant time to select a stirring speed between the instantly claimed 1000-2500 RPM in step 2b through process optimization, since it has been held that there the general conditions of a claim are disclosed in the prior art, discovering the optimum or workable ranges involves only routine skill in the art. See In re Boesch, 205 USPQ 215. In addition, it would have been obvious to one of ordinary skill in the art at the relevant time to select an operating frequency between 20 and 60 kHz to effectively homogenize the reaction of step 2b because the range described is of routine use in the art and higher frequencies may induce unwanted convection (pp. 269, right col., 5th paragraph).
Claim 8 is rejected under 35 U.S.C. 103 as being unpatentable over CN '419A, Zheng et al., and Ding et al., as applied to claim 1 above, and further in view of Marin et al. (in New Trends in Macromolecular and Supramolecular Chemistry for Biological Applications, Springer Nature Switzerland, 2021).
In regard to claim 8, CN ‘419A and Zheng et al. do not teach process parameters for the cross-linking modification of an adsorbent material. However, Ding et al. teaches that six grams of EDGE were added to 100 mL of solution for the cross-linking reaction, resulting in a 5.6 wt% mass concentration of cross-linking agent. The calculated mass concentration of the crosslinking solution is 0.6 wt% out of the instantly claimed mass concentration range of 0.5-5 wt%. The amount of crosslinking agent added to solution controls the degree to which the base polymer will become crosslinked, which is related to both rigidity and porosity. However, it would have been obvious to one having ordinary skill in the art at the time the invention was made to choose the instantly claimed range of crosslinking agent concentrations through process optimization to yield preferred physical properties of the final material, since it has been held that there the general conditions of a claim are disclosed in the prior art, discovering the optimum or workable ranges involves only routine skill in the art. See In re Boesch, 205 USPQ 215. The cross-linking reaction was carried out for 9 hours, which is within the instantly claimed crosslinking time of 0.5-24 hours.
Ding et al. does not teach that citral, cinnamyl aldehyde, cintronellal, anisaldehyde or genipin are used as crosslinking agents. However, Marin et al. teaches that crosslinking chitosan with genipin (pp. 346) or monoaldehydes, as they are naturally occurring, nontoxic, and have high biocompatibility (pp. 347, lines 1-5). Specifically, Marin et al. explored the efficacy of citral and cinnamyl aldehyde (structures in pp. 347, Scheme 1). Cinnamyl aldehyde was observed to create a chitosan-crosslinked hydrogel with high porosity, which would have been attractive to a person of ordinary skill for applications as an adsorbent (pp. 352, Section 4, lines 3-11). Therefore, it would have been obvious to modify the combined teachings of CN ‘419A, Zheng et al., and Ding et al., to substitute ethylene glycol diglycidyl ether with cinnamyl aldehyde as a crosslinking agent for the chitosan material as a biocompatible, nontoxic, cheaper ingredient that results in a highly porous hydrogel.
Allowable Subject Matter
Claims 4 and 5 are objected to as being dependent upon a rejected base claim, but would be allowable if rewritten in independent form including all of the limitations of the base claim and any intervening claims.
The following is a statement of reasons for the indication of allowable subject matter:
Claim 4 is directed to starting reagents and process parameters for step 2 of the preparation method. The indication that the starting material is a mixture of chitosan and either hydrochloride chitosan, carboxymethyl chitosan, and quaternary ammonium salt chitosan and that the adjuvant is citric acid, lactic acid, oxalic acid, gluconic acid, glycolic acid, malic acid, or tartaric acid is not fairly taught or suggested by the combined teachings of CN ‘419A, Zheng et al., Ding et al. Claim 5 is directed to process parameters for step 2 of the preparation method. While the prior art cited discloses the general preparation method of claim 1, the closest identified pieces of prior art do not fairly teach, suggest, or provide evidence for the optimization of the instantly claimed process parameters.
Conclusion
Any inquiry concerning this communication or earlier communications from the examiner should be directed to MORDECAI M LEAVITT whose telephone number is (571)272-6637. The examiner can normally be reached Monday-Friday 8AM-5PM.
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/MORDECAI M LEAVITT/Examiner, Art Unit 1742 /CHRISTINA A JOHNSON/Supervisory Patent Examiner, Art Unit 1742
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