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 Application
Claims 1-18, 20-31 are currently pending. Claim 19 is cancelled. Claims 1, 7-9 are currently amended. Claim 31 is new.
Response to Arguments
Applicant's arguments filed 02/26/2026 have been fully considered but they are not persuasive.
Firstly, Examiner notes that Jin is relied upon to teach the step of pressurizing and is not relied upon to teach the sintering step, as Wang already discloses the step of sintering.
Regarding the argument that the method disclosed by Jin involves calcination rather than the claimed sintering, Examiner notes that “calcining” and “sintering” are often used interchangeably in the art, thus it appears necessary to compare the actual conditions of the claimed “sintering” and calcination of Jin.
The instant specification discloses wherein sintering temperature may be in a range of about 850° C. to about 950° C and the pellet may be sintered for at least about 10 hours [PG Pub 0044-0045] (e.g., 900°C for 10 h in Example 1).
In this regard, Jin also teaches wherein the pellet is heat-treated at 980°C for 20 hours, then heat-treated at 900°C for 5 hours [0057] which is “at least about 10 hours”. Jin further discloses that the heat treatment temperature may range from 500 to 1,500°C. [0034] which encompasses the temperature range of the instant specification (i.e., “about 850° C. to about 950° C”). Thus, a person having ordinary skill in the art would reasonably understand the “sintering” of the instant application and heat-treating or calcination of Jin are held at substantially similar conditions (i.e., temperature and time) and further envisage the pellets to have formed similar structures (i.e., single crystal) absent evidence contrary.
Further, Zhang (Single-Crystalline Ni-Rich LiNixMnyCo1−x−yO2 Cathode Materials: A Perspective, copy attached) recognizes that sintering temperature as one of the most critical factors for forming single-crystal NMC (SC-NMC), wherein synthesis of SC-NMC is typically conducted at 900–1020 °C. Zhang further discloses that longer sintering time at higher temperature is generally required for the growth of large single crystals (See pg 3, first paragraph). Since Jin discloses wherein the NCM pellet is “heat-treated at 980°C for 20 hours, then heat-treated at 900°C for 5 hours” [Jin 0057] (i.e., high temperature and long sintering time), a person having ordinary skill in the art would reasonably envisage the pellet to have formed a single crystal morphology.
Applicant further appears to argue that Sloop does not teach a separate step of relithiating and purifying prior to admixing with nickel (claim 2).
Examiner notes that Sloop teaches wherein spent positive electrode material is harvested (step 12) and thrashed in basic medium comprising LiOH to separate the electrode material from binder and break each of the components down to a manageable particle size (Step 14; [0026]), followed by further relithiating with LiOH and a relithiation solution comprising dilute nickel [0035, 0038] (e.g., step 28).
As such, it would have been obvious for a person having ordinary skill in the art before the effective filing date to have added a step of relithiating and purifying, such as step 14 of Sloop, prior to admixing with nickel (i.e., step 28), with a reasonable expectation to separate different components of the spent positive electrode material and prepare for subsequent mechanical and chemical processes [0026 Sloop].
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.
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) 1,3-16,20-21,23-24 and 26 is/are rejected under 35 U.S.C. 103 as being unpatentable over Wang (US20240079580A1, previously cited), in view of Jin (WO2020111807A1, previously cited).
Regarding claim 1, 7-10, 23, Wang discloses a method for direct upcycling of lithium-ion battery cathodes, the method comprising:
providing delithiated NCM particles from spent lithium-ion battery cathodes (i.e., 5.207 mmol spent NMC111 [0048]);
admixing the delithiated NCM particles with a Ni-containing precursor (i.e., 3.468 mmol NiO [0048]) to form a combination;
admixing the combination with a supplementary lithium source (i.e., 20 mol % excess of LiOH [0048]) to form a mixture,
wherein the supplementary lithium source comprises a single lithium salt (i.e., LiOH [0048]) and
the mixture comprises a molar excess of the lithium salt (i.e., “20 mol % excess of LiOH” [0048])
sintering at 900° C [Wang 0045] the mixture to produce single-crystal NCM particles with increased nickel content (i.e., Single-Crystal NCM 622 [0048-0049]) (i.e., “between 850°C and about 950°C” of claim 10).
However, Wang does not disclose wherein the method comprises:
treating the mixture at a pressure of at least 1 MPa to form a pressurized mixture prior to the sintering.
In this regard, Jin also teaches a method for manufacturing a cathode active material from a lithium secondary battery from a recovered cathode active material (abstract), wherein degraded NCM is mixed with a lithium source and a nickel source [Jin 0056], followed by a pelletizing step (i.e., “treating the mixture at a pressure” as claimed) at a pressure of 30 MPa, followed by heat treatment step [Jin 0057].
Thus, it would have been obvious for a person having ordinary skill in the art before the effective filing date to have modified the method for upcycling lithium-ion battery cathodes such that the mixture is pelletized at a pressure of 30 MPa, which is “at least 1 MPa” (claim 1), “at least 5 MPa” (claim 8), and “at least about 15 MPa” (claim 9) prior to the heat treatment step, as Jin teaches that pressurizing (i.e., pelletizing) the cathode improves the charge density characteristics and charge/discharge characteristics of a battery [Jin 0045].
Regarding claim 3, modified Wang discloses the method of claim 1, wherein the single-crystal NCM particles (i.e., Single-Crystal NCM622 [Wang 0048]) have a nickel content of at least 60% (see Table 1 wherein Ni content ranges from 0.603-0.610).
Regarding claim 4, modified Wang discloses the method of claim 1, wherein a source of the delithiated NCM particles is D-NCM 111 (“Spent NCM111” [Wang 0048]).
Regarding claim 5, modified Wang discloses the method of claim 1, wherein the delithiated NCM particles (spent NMC111) are ball milled with the Ni-containing precursor (NiO) to produce NCM single-crystal particles (i.e., in agate jar with agate balls [Wang 0045], [Wang 0048]).
Regarding claim 6, modified Wang discloses the method of claim 5, wherein the Ni-containing precursor comprises NiO (in Example 1 [Wang 0045]), but does not disclose wherein the Ni-containing precursor comprises Ni(OH)2, as claimed.
In this regard, Jin teaches wherein the Ni-containing precursor may be at least one selected from a list comprising NiO, Ni(OH)2 [Jin 0039]. Thus, it would have been obvious for a person having ordinary skill in the art to have used Ni(OH)2 as an alternative Ni-containing precursor to the NiO, with a reasonable expectation to adjust nickel amount in the upcycled cathode [Jin 0055].
Regarding claims 11, modified Wang discloses the method of claim 10, wherein the pellet is sintered at 900°C for 10 hours [Wang 0045]. Examiner notes that the instant specification does not provide any special definition of the term “about”. Thus, absent special definition of “about”, the claimed limitation of “about 850 °C” is considered met since Wang teaches a sintering temperature of 900°C.
Regarding claim 12, modified Wang discloses the method of claim 10, wherein a ramping rate during sintering is about 10 °C/min [Wang 0045].
Regarding claim 13, modified Wang discloses the method of claim 10, wherein the pellet is sintered under pure oxygen (“under oxygen atmosphere” [Wang 0045]).
Regarding claims 14-15, modified Wang discloses the method of claim 10, wherein the pellet is sintered for 10 h [Wang 0045], which is “at least about 10 h” (claim 14) and “between about 10 h and about 15 h” (claim 15).
Regarding claim 16, modified Wang discloses the method of claim 15, wherein the pellet is sintered for 10 h [Wang 0045]. Examiner notes that the instant specification does not provide any special definition of the term “about”. Therefore, the claimed limitation of “wherein the pellet is sintered for about 12 h” is considered met since Wang discloses the sintering time of 10 h absent persuasive evidence to the contrary [Wang 0045].
Regarding claims 20-21, modified Wang discloses the method of claim 1, wherein the mixture comprises 20 mol% excess of LiOH [Wang 0048], which is “at least about a 5% molar excess of the lithium salt” (claim 20) and “at least about a 10% molar excess of the lithium salt” (claim 21).
Regarding claim 24, modified Wang discloses the method of claim 1, wherein the single-crystal NCM particles comprise NCM 611 (Example 4 [Wang 0048]). While Wang does not disclose wherein NCM111 is upcycled to NCM 811 in that embodiment, Wang further discloses in Example 2 wherein NCM111 is upgraded to a single-crystal NCM 811 (Example 2; [Wang 0022, 0046]), having a formula of approximately LiNi0.8Co0.1Mn0.1O2.
Thus, it would have been obvious for a person having ordinary skilled in the art to have used the method disclosed in claim 1 to produce an upcycled NCM 811, with a reasonable expectation to provide nickel rich cathode material with improved specific capacity and cycling stability [Wang 0019].
Regarding claim 26, modified Wang discloses the method of claim 1, wherein the single crystal NCM particles comprise NCM 622 (Example 4; [Wang 0048]), having a formula of approximately LiNi0.6Co0.2Mn0.2O2.
Claim(s) 2, 31 is/are rejected under 35 U.S.C. 103 as being unpatentable over Wang (US20240079580A1, previously cited), in view of Jin (WO2020111807, previously cited) and Sloop (US20170200989A1, IDS cited 09/06/2024, previously cited).
Regarding claim 2, modified Wang discloses the method of claim 1. However, Wang does not disclose the method “further comprising relithiating and purifying the delithiated NCM particles prior to admixing with the Ni-containing precursor”.
In this regard, Sloop teaches methods to recycle positive-electrode material of a lithium-ion battery (title), wherein spent positive electrode material (e.g., NMC [0025]) is suspended in basic medium comprising lithium hydroxide to delaminate the positive electrode material from the binder, and break each component down to a manageable particle size to facilitate subsequent mechanical and chemical processing [Sloop 0026]. Sloop further teaches that the medium may further include LiClO, lithium peroxide as an oxidizing agent [Sloop 0026].
As such, it would have been obvious for a person having ordinary skill in the art before the effective filing date to have added such step of purifying (i.e., delaminating) and relithiating (i.e., with lithium hydroxide) prior to admixing with the Ni-containing precursor, with a reasonable expectation to physically separate the positive-electrode material from the support, the binder, and break each of the components down to a manageable particle size to facilitate subsequent mechanical and chemical processing [Sloop 0026].
Regarding claim 31, Wang discloses a method for direct upcycling of lithium-ion battery cathodes, the method comprising:
providing delithiated NCM particles from spent lithium-ion battery cathodes (i.e., 5.207 mmol spent NMC111 [0048])
Wang does not disclose the step of:
relithiating and purifying the delithiated NCM particles prior to admixing with a Ni- containing precursor
In this regard, Sloop teaches methods to recycle positive-electrode material of a lithium-ion battery (title), wherein spent positive electrode material (e.g., NMC [0025]) is suspended in basic medium comprising lithium hydroxide to delaminate the positive electrode material from the binder, and break each component down to a manageable particle size to facilitate subsequent mechanical and chemical processing [Sloop 0026]. Sloop further teaches that the medium may further include LiClO, lithium peroxide [Sloop 0026]. Sloop further teaches wherein the delaminated positive electrode material is relithiated with a relithiation solution comprising dilute nickel ([0037-0038]; step 28).
As such, it would have been obvious for a person having ordinary skill in the art before the effective filing date to have added such step of purifying (i.e., delaminating) and relithiating (achieved by mixing with lithium hydroxide) prior to admixing with a Ni-containing precursor, with a reasonable expectation to physically separate the positive-electrode material from the support, the binder, and break each of the components down to a manageable particle size to facilitate subsequent mechanical and chemical processing [Sloop 0026].
Wang further discloses:
admixing the delithiated NCM particles with the Ni-containing precursor (i.e., 3.468 mmol NiO [0048]) to form a combination;
admixing the combination with a supplementary lithium source (i.e., 20 mol % excess of LiOH [0048]) to form a mixture,
wherein the supplementary lithium source comprises a single lithium salt (i.e., LiOH [0048]) and
the mixture comprises a molar excess of the lithium salt (i.e., “20 mol % excess of LiOH” [0048])
sintering at 900° C [Wang 0045] the mixture to produce single-crystal NCM particles with increased nickel content (i.e., Single-Crystal NCM 622 [0048-0049]) (i.e., “between 850°C and about 950°C” of claim 10).
However, Wang does not disclose:
treating the mixture at a pressure of at least 1 MPa to form a pressurized mixture prior to the sintering
In this regard, Jin also teaches a method for manufacturing a cathode active material from a lithium secondary battery from a recovered cathode active material (abstract), wherein degraded NCM is mixed with a lithium source and a nickel source [Jin 0056], followed by a pelletizing step (i.e., “treating the mixture at a pressure” as claimed) at a pressure of 30 MPa, followed by heat treatment step [Jin 0057].
Thus, it would have been obvious for a person having ordinary skill in the art to have modified the method for upcycling lithium-ion battery cathodes such that the mixture is pelletized at a pressure of 30 MPa, which is “at least 1 MPa” (claim 1), “at least 5 MPa” (claim 8), and “at least about 15 MPa” (claim 9) prior to the heat treatment step, as Jin teaches that pressurizing (i.e., pelletizing) the cathode improves the charge density characteristics and charge/discharge characteristics of a battery [Jin 0045].
Claim(s) 17 is/are rejected under 35 U.S.C. 103 as being unpatentable over Wang (US20240079580A1, previously cited), in view of Jin (WO2020111807, previously cited) and Min (CN 112054265 A, previously cited).
Regarding claim 17, modified Wang discloses the method of claim 10, but does not disclose wherein during sintering, the pellet is held at about 480 °C for about 3 h.
In this regard, Min teaches methods for recycling and reusing cathode materials from waste ternary lithium-ion batteries (title), wherein the spent ternary positive electrode material, supplement lithium source, and lithium transition metal are mixed [0045], followed by calcination at pressurized condition [Min 0048], wherein pre-calcining occurs at 400-600℃ for 3-6 hours [Min 0048], which encompasses the claimed temperature and time of “about 480°C for about 3 h”.
It would have been obvious for a person having ordinary skill in the art to have modified the pellet sintering temperature and time within the taught range of “not higher than 550 °C for 2-6 hours” (e.g., “about 480°C for about 3 h”), as Min teaches that such ternary single-crystal cathode materials obtained by high-temperature and high-pressure sintering has excellent performance [Min 0026] and the internal cracks of the material disappear and the material becomes denser [Min 0068].
Claim(s) 18 is/are rejected under 35 U.S.C. 103 as being unpatentable over Wang (US20240079580A1, previously cited), in view of Jin (WO2020111807, previously cited), Min (CN 112054265 A, previously cited), and Cui (CN113582251A, previously cited).
Regarding claim 18, modified Wang discloses the method of claim 17, wherein the ramping rate is 10°C/min [Wang 0045]. Min teaches wherein the temperature is raised [Min 0048], but does not disclose a ramping rate.
Thus, modified Wang does not disclose wherein a ramping rate during sintering is about 5 °C/min.
In this regard, Cui also teaches a recycling and regenerating method of positive electrode material, wherein the spent positive electrode material and lithium source are mixed and transferred into a high pressure hydrothermal reactor at the temperature of 400-500 °C, wherein the ramping speed is 1-5°C/min [0018], which overlaps with the claimed range of “about 5°C/min”. A person having ordinary skill in the art before the effective filing date would have been motivated to control the ramping rate of modified Wang, such that it is in the overlapping range, as Cui teaches that cathode material calcined at such condition is restored to its state before failure [Cui 0018].
Claim(s) 22 is/are rejected under 35 U.S.C. 103 as being unpatentable over Wang (US20240079580A1, previously cited), in view of Jin (WO2020111807, previously cited), and Ji (CN112117507A, previously cited).
Regarding claim 22, modified Wang discloses the method of claim 1, wherein various examples include 20-50 mol% excess of LiOH were added [Wang 0045]. Thus, Wang does not disclose wherein the mixture comprises “about a 5% molar excess of the lithium salt”.
In this regard, Ji teaches a method for regenerating cathode materials from waste lithium ion- batteries (title), wherein spent NCM is mixed with 5% excess lithium source to regenerate and obtain a high performance ternary cathode active material [Ji 0049]. Thus, it would have been obvious for a person having ordinary skill in the art to have modified the amount of molar excess of the lithium salt, such that it is “about a 5% molar excess of the lithium salt” with a reasonable expectation to lithiate the spent cathode to obtain a high performance ternary positive electrode active material [Ji 0065].
Claim(s) 25 is/are rejected under 35 U.S.C. 103 as being unpatentable over Wang (US20240079580A1, previously cited), in view of Jin (WO2020111807, previously cited) and Holman (US20220223379A1, previously cited).
Regarding claim 25, modified Wang discloses the method of claim 24. Wang does not disclose the specific surface and does not disclose “wherein the NCM 811 particles have a surface area of approximately 1.74 m2/g” as claimed.
In this regard, Holman teaches a method for recycling used NMC materials powder to produce NCM 532, NMC 622, or NMC 811 having a surface area of 0.01 to 15m2/g [Holman 0041], which encompasses the claimed amount of “approximately 1.74m2/g”. Thus, it would have been obvious for a person having ordinary skill in the art to have modified the surface area of the NCM 811 particles of Wang, such that it is within the taught range of 0.01 to 15m2/g [Holman 0041] (e.g., “approximately 1.74m2/g” as claimed), with a reasonable expectation to provide sufficient surface for electrochemical reaction [Holman 0037]
Claim(s) 27-29 is/are rejected under 35 U.S.C. 103 as being unpatentable over Wang (US20240079580A1, previously cited), in view of Jin (WO2020111807, previously cited), and Peng (CN114843504, previously cited).
Regarding claim 27-29, modified Wang discloses the method of claim 1. However, Wang is silent to an average particle size of the single-crystal NCM particles.
In this regard, Peng teaches a ternary positive electrode material for lithium ion battery with single crystal morphology (title), wherein an average particle size of the ternary positive electrode material preferably ranges from 1-10 μm [Peng 0020], which encompasses the claimed ranges of “about 1.0 µm to about 5.0 µm” (claim 27), “about 1.6 µm to about 2.5 µm”(claim 28), and “about 1.8 µm” (claim 29).
It would have been obvious for a person having ordinary skill in the art to have modified the average particle size of the single-crystal NCM particles of Wang, such that it is in the overlapping range, as Peng teaches such cathode is easy to make [0019] and breakage of the material during the cycle can be avoided [Peng 0021].
Claim(s) 30 is/are rejected under 35 U.S.C. 103 as being unpatentable over Wang (US20240079580A1, previously cited), in view of Jin (WO2020111807, previously cited) and Zhang (CN113265704A, previously cited).
Regarding claim 30, modified Wang discloses the method of claim 1, but does not explicitly disclose the wherein an XPS I(003)/I(104) peak intensity ratio of the NCM particles is greater than 1.6.
In this regard, Zhang teaches a method for preparing single-crystal LiNi0.6Co0.2Mn0.2O2 or LiNi0.8Co0.1Mn0.1O2 ternary electrode materials from recycled waste (Examples 2,3) having I(003)/I(104) is 2.485 and 2.699 (see Table), which is “greater than 1.6” as claimed. A person having ordinary skill in the art would have been motivated to modify the NCM particles of Wang such that the I003/I104 it is “greater than 1.6” such as 2.485 and 2.699 of Zhang, as Zhang teaches that such cathode provides high charge-charge specific capacity and stable long cycle performance [Zhang 0053].
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.
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/T.S./Examiner, Art Unit 1751
/Haroon S. Sheikh/Primary Examiner, Art Unit 1751
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