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 Rejections - 35 USC § 103
The text of those sections of Title 35, U.S. Code not included in this action can be found in a prior Office action.
Claim(s) 1-2 and 7-9 and 12 is/are rejected under 35 U.S.C. 103 as being unpatentable over Chu et al. (US-6402795-B1) in view of Coowar et al. (US-20130069601-A1).
Regarding Claim 1, Chu discloses an anode (electrode precursor 17’, Fig. 2). The preamble recitation of an anode “for an all-solid-state battery” amounts to a recitation of the intended use of the claimed anode. The recitation of the intended use of the claimed invention must further limit the structure of the claimed invention in order to be given patentable weight (MPEP 2111.02, II). Since the recitation of “for an all-solid-state battery” does not further limit the structure of the claimed anode, the intended use limitation “for an all solid-state battery” is not given patentable weight, since the anode of the prior art is fully capable of being used in an all-solid-state battery.
Chu thereby discloses an anode for an all-solid-state battery, the anode comprising (Col. 2, lines 19- 66; Col. 3, lines 7-18, 41-48; Col. 5, lines 1-10):
an anode current collector (14, Fig. 2); and
a coating layer (wetting layer 15, Fig. 2) contacting the anode current collector (see Fig. 2) prior to an initial charging of the all-solid-state battery (Col. 2, line 58 – Col. 3, line 2; Col. 5, lines 4-10; Col. 8, lines 61-67).
Chu discloses that the coating layer (wetting layer 15) can be formed of various materials that lower the energy of plating (Col. 6, lines 45-46), such as materials that alloy with lithium and materials that intercalate lithium (Col. 6, lines 46-49). Examples of such materials include carbon and metal sulfides such as titanium sulfide and iron sulfide (Col. 6, lines 51-52).
Although Chu does not disclose a specific example where both carbon and a metal sulfide are used together, the Examiner notes that combining equivalents known for the same purpose represents a prima facie case of obviousness (MPEP 2144.06, I). It would have been obvious to one of ordinary skill in the art, before the effective filing date of the claimed invention, to have used a combination of carbon and a metal sulfide with a reasonable expectation that such a configuration would have resulted in a successful coating layer for use in an anode.
As laid out above, Chu renders obvious that the coating layer (wetting layer) consists of a combination of metal sulfide and carbon, and Chu discloses that the materials of the coating layer either alloy with lithium or intercalate lithium (Col. 6, lines 45-52). Chu does not teach that the coating layer comprises a magnesium-based particle.
Coowar teaches a lithium ion battery including an anode comprising an electroactive material [0056-0057]. Coowar teaches electroactive materials which are able to both incorporate and release metal ion charge carriers such as lithium [0070]. Coowar teaches specific examples of the electroactive materials include, from a list of potential candidates, MgS [0071]. The Examiner notes that this establishes MgS as a metal sulfide material which is able to intercalate lithium ions.
It would have been obvious to one of ordinary skill in the art, before the effective filing date of the claimed invention, to have selected the metal sulfide of the coating layer of Chu to be MgS with a reasonable expectation that such a metal sulfide would result in a successful coating layer, since the selection of a known material based on its suitability for its intended use supports a prima facie case of obviousness (MPEP 2144.07).
Therefore, modified Chu renders obvious that the coating layer consists of:
a carbon material (carbon; Chu: Col. 6, line 51); and
a magnesium-based particle including a magnesium compound comprising MgS.
Although Chu does not specifically teach the content of carbon and the content of magnesium-based particles (i.e. MgS), and therefore does not explicitly teach that the coating layer consists of “10% to 70% by weight of carbon material; and 30% to 90% by weight of magnesium-based particles”, the Examiner notes that the prior art necessarily possesses a certain amount of each material. In other words, since modified Chu renders obvious that the coating layer consists of a carbon material and magnesium sulfide particles, the carbon material is understood to inherently be present in a range of greater than 0% and less than 100%. Similarly, the MgS particles are understood to be present in a range of greater than 0% and less than 100%. These ranges overlap the claimed ranges. It would have been obvious to one of ordinary skill in the art, before the effective filing date of the claimed invention, to have selected any portion of the ranges rendered obvious by the prior art, including the overlapping portion of the ranges, with a reasonable expectation that such contents of carbon material and magnesium sulfide particles would result in a successful coating layer (MPEP 2144.05, I).
Chu discloses that the coating layer does not have any lithium prior to the initial charging of the all-solid-state battery (Col. 2, line 58 – Col. 3, line 2; Col. 5, lines 4-10; Col. 8, line 61 Col. 9, line 4), and that the coating layer is a monolayer structure (see Fig. 2).
Chu discloses that the coating layer can have a thickness between 50 and 1000 angstroms (Col. 6, lines 57-59). Therefore, although modified Chu does not explicitly teach that the coating layer has a thickness of 0.1 µm to 20 µm, it would have been obvious to one of ordinary skill in the art, before the effective filing date of the claimed invention, to have selected the coating layer to have a thickness of 1000 angstroms (i.e. 0.1 µm) with a reasonable expectation that such a configuration would result in a successful coating layer for an anode (MPEP 2144.05, I).
Regarding Claim 2, modified Chu renders obvious all of the limitations as set forth above. Chu further discloses that the anode current collector be selected from the group consisting of copper, nickel, stainless steel and zinc (Chu: Claim 12). Therefore, it would have been obvious to one of ordinary skill in the art, before the effective filing date of the claimed invention, to have selected the anode current collector to comprise nickel or stainless steel with a reasonable expectation that such a configuration would have resulted in a successful anode current collector.
Regarding Claim 7, modified Chu renders obvious all of the limitations as set forth above. Although modified Chu does not explicitly teach that the anode further comprises “a charge product containing lithium between the coating layer and the anode current collector when the all-solid-state battery is charged”, the Examiner notes that this limitation amounts to the intended use of the claimed anode. The recitation of intended use of a claimed invention must result in a structural difference between the claimed invention and the prior art in order to patentably distinguish the claimed invention from the prior art. If the prior art is capable of performing the intended use, then it meets the limitation of the claim. Here, modified Chu renders obvious the claimed configuration of the anode necessary to perform the intended use limitation. Specifically, modified Chu teaches an anode current collector, a coating layer contacting the anode current collector, wherein the coating layer consists of a carbon material and a magnesium-based particle including a magnesium compound comprising MgS. Therefore, the prior art has the structure necessary to perform the intended use limitation. Thus, the intended use limitation is met.
Additionally, since the structure rendered obvious by the prior art is substantially similar to the claimed structure (as laid out above), it is understood that the anode of the prior art necessarily and inherently undergoes the claimed transformation during charging, as evidenced by the instant specification [instant specification: 0054-0055, 0059-0060].
Regarding Claim 8, Chu discloses an electrode precursor wherein a protective layer (18, Fig. 2) is deposited onto the surface of a current collector (14, Fig. 2) with a wetting layer (15, Fig. 2) between the protective layer and the current collector (Col. 2, lines 19- 57; Col. 3, lines 7-18; Col. 5, lines 1-10). The electrode precursor can then be converted to an alkali metal electrode by an initial charging operation, in which lithium plates from the positive electrode (Col. 2, lines 58-66). In such a charging method, the electrode precursor is assembled with other battery elements including an electrolyte and a positive electrode (Col. 2, lines 58-61). Chu further discloses that current collectors contact both the positive and negative electrodes in a conventional manner (Col. 11, lines 24-27), and that the protective layer can be used directly as a solid electrolyte (Col. 11, lines 14-16).
Therefore, although not disclosed in a single embodiment, one of ordinary skill in the art, before the effective filing date of the claimed invention, would have found it obvious to have provided an all-solid-state battery (corresponds to a battery assembled with an electrode precursor) wherein the protective layer (18, Fig. 2) is used directly as a solid electrolyte, with a reasonable expectation that using the protective layer as a solid electrolyte would result in a successful all-solid-state battery.
The configuration of the all-solid-state battery rendered obvious by Chu can be visualized using the annotation of Chu Fig. 3, below. Notably, the configuration disclosed in Chu Fig. 3 comprises a lithium layer (314; Col. 11, lines 33-48) and an electrolyte region (316; Col. 11, lines 43-50), which are not present in the all-solid-state battery comprising the electrode precursor as rendered obvious by Chu (see above; Col. 2, line 58 – Col. 3, line 2; Col. 8, line 61 – Col. 9, line 4) wherein the protective layer is used directly as a solid electrolyte (see above; Col. 11, lines 13-21). Accordingly, the solid electrolyte layer as rendered obvious by Chu is understood to contact the coating layer and the cathode.
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Annotation of Chu Fig. 3.
Therefore, as depicted in the annotation of Chu, Fig. 3 (above), the all-solid-state battery comprises (Col. 8, line 61 – Col. 9, line 4; Col. 11, lines 14-16, 33-43):
a cathode (corresponds to the combination of positive electrode 318 and positive current collector 320);
an anode comprising an anode current collector (negative current collector 312, Fig. 3) and a coating layer (wetting layer 313, Fig. 3) on the anode current collector,
a solid electrolyte layer (protective layer 308) between the cathode and the anode, wherein the solid electrolyte layer contacts the cathode and the coating layer of the anode, wherein:
the solid electrolyte layer is a first monolayer structure, and
the coating layer is a second monolayer structure.
Chu discloses that the coating layer (wetting layer) can be formed of various materials that lower the energy of plating (Col. 6, lines 45-46), such as materials that alloy with lithium and materials that intercalate lithium (Col. 6, lines 46-49). Examples of such materials include carbon and metal sulfides such as titanium sulfide and iron sulfide (Col. 6, lines 51-52).
Although Chu does not disclose a specific example where both carbon and a metal sulfide are used together, the Examiner notes that combining equivalents known for the same purpose represents a prima facie case of obviousness (MPEP 2144.06, I). Therefore, it would have been obvious to one of ordinary skill in the art, before the effective filing date of the claimed invention, to have used a combination of carbon and a metal sulfide with a reasonable expectation that such a configuration would have resulted in a successful coating layer for use in an anode.
As laid out above, Chu renders obvious that the coating layer (wetting layer) consists of a combination of metal sulfide and carbon, and Chu discloses that the materials of the coating layer either alloy with lithium or intercalate lithium (Col. 6, lines 45-52). Chu does not teach that the coating layer comprises a magnesium-based particle.
Coowar teaches a lithium ion battery including an anode comprising an electroactive material [0056-0057]. Coowar teaches electroactive materials which are able to both incorporate and release metal ion charge carriers such as lithium [0070]. Coowar teaches specific examples of the electroactive materials include, from a list of potential candidates, MgS [0071]. The Examiner notes that this establishes MgS as a metal sulfide material which is able to intercalate lithium ions.
Therefore, it would have been obvious to one of ordinary skill in the art, before the effective filing date of the claimed invention, to have selected the metal sulfide of the coating layer of Chu to be MgS with a reasonable expectation that such a metal sulfide would result in a successful coating layer, since the selection of a known material based on its suitability for its intended use supports a prima facie case of obviousness (MPEP 2144.07).
Therefore, modified Chu renders obvious that the coating layer consists of:
a carbon material (carbon; Chu: Col. 6, line 51); and
a magnesium-based particle including a magnesium compound comprising MgS.
Although Chu does not specifically teach the content of carbon and the content of magnesium-based particles (i.e. MgS), and therefore does not explicitly teach that the coating layer consists of “10% to 70% by weight of carbon material; and 30% to 90% by weight of magnesium-based particles”, the Examiner notes that the prior art necessarily possesses a certain amount of each material. In other words, since modified Chu renders obvious that the coating layer consists of a carbon material and magnesium sulfide particles, the carbon material is understood to inherently be present in a range of greater than 0% and less than 100%. Similarly, the MgS particles are understood to be present in a range of greater than 0% and less than 100%. These ranges overlap the claimed ranges. It would have been obvious to one of ordinary skill in the art, before the effective filing date of the claimed invention, to have selected any portion of the ranges rendered obvious by the prior art, including the overlapping portion of the ranges, with a reasonable expectation that such contents of carbon material and magnesium sulfide particles would result in a successful coating layer (MPEP 2144.05, I).
Chu discloses that the coating layer does not have any lithium prior to an initial charging of the all-solid-state battery (Col. 2, line 58 – Col. 3, line 2; Col. 5, lines 4-10; Col. 8, line 61 Col. 9, line 4).
Chu discloses that the coating layer can have a thickness between 50 and 1000 angstroms (Col. 6, lines 57-59). Therefore, although modified Chu does not explicitly teach that the coating layer has a thickness of 0.1 µm to 20 µm, it would have been obvious to one of ordinary skill in the art, before the effective filing date of the claimed invention, to have selected the coating layer to have a thickness of 1000 angstroms (i.e. 0.1 µm) with a reasonable expectation that such a configuration would result in a successful coating layer for an anode (MPEP 2144.05, I).
Regarding Claim 9, modified Chu renders obvious all of the limitations as set forth above. Chu further discloses that the anode current collector be selected from the group consisting of copper, nickel, stainless steel and zinc (Chu: Claim 12). Therefore, it would have been obvious to one of ordinary skill in the art, before the effective filing date of the claimed invention, to have selected the anode current collector to comprise nickel or stainless steel with a reasonable expectation that such a configuration would have resulted in a successful anode current collector.
Regarding Claim 12, modified Chu renders obvious all of the limitations as set forth above. Although modified Chu does not explicitly teach that the all-solid-state battery further comprises “a charge product containing lithium between the coating layer and the anode current collector when the all-solid-state battery is charged”, Examiner notes that this limitation amounts to the intended use of the claimed all-solid-state battery. The recitation of intended use of a claimed invention must result in a structural difference between the claimed invention and the prior art in order to patentably distinguish the claimed invention from the prior art. If the prior art is capable of performing the intended use, then it meets the limitation of the claim. Here, the prior art renders obvious the claimed configuration of the anode necessary to perform the intended use limitation. Specifically, the prior art teaches an anode current collector, a coating layer contacting the anode current collector, wherein the coating layer consists of a carbon material and a magnesium-based particle including a magnesium compound comprising MgS. Therefore, the prior art has the structure necessary to perform the intended use limitation. Thus, the intended use limitation is met.
Additionally, since the structure rendered obvious by the prior art is substantially similar to the claimed anode structure (as laid out above), it is understood that the all-solid-state battery of the prior art necessarily and inherently undergoes the claimed transformation during charging, as evidenced by the instant specification [instant specification: 0054-0055, 0059-0060].
Claim(s) 4 and 10 is/are rejected under 35 U.S.C. 103 as being unpatentable over Chu et al. (US-6402795-B1) in view of Coowar et al. (US-20130069601-A1) as applied to Claims 1 and 8, above, and in view of Miyaki et al. (US-20020114993-A1; previously cited).
Regarding Claim 4, modified Chu renders obvious all of the limitations as set forth above, including that the coating layer comprises MgS. Modified Chu does not teach the size (D50) of MgS.
Miyaki teaches a protective layer which can be formed on a negative electrode for a lithium secondary battery [0009, 0058]. The protective layer can include alkaline earth metal salts, such as magnesium-based metal salts, which particularly preferably have a particle size of 0.05 to 10 µm [0028-0030]. The Examiner notes that MgS is a form of alkaline earth metal salt.
It would have been obvious to one of ordinary skill in the art, before the effective filing date of the claimed invention, to have selected the MgS particles of modified Chu to have a particle size of 0.05 to 10 µm (i.e. 50 nm to 10 µm) with a reasonable expectation that such a particle size would result in successful MgS particles for use in a coating layer for an anode.
The range rendered obvious by modified Chu overlaps the claimed range of 10 nm to 2000 nm. It would have been obvious to one of ordinary skill in the art, before the effective filing date of the claimed invention, to have selected the overlapping portion of the range disclosed in the prior art with a reasonable expectation that magnesium sulfide particles with a particle size (D50) of 50 nm to 2000 nm would result in a successful magnesium-based particles for use in a coating layer (MPEP 2144.05, I).
Regarding Claim 10, modified Chu renders obvious all of the limitations as set forth above, including that the coating layer comprises MgS. Modified Chu does not teach the size (D50) of MgS.
Miyaki teaches a protective layer which can be formed on a negative electrode for a lithium secondary battery [0009, 0058]. The protective layer can include alkaline earth metal salts, such as magnesium-based metal salts, which particularly preferably have a particle size of 0.05 to 10 µm [0028-0030]. The Examiner notes that MgS is a form of alkaline earth metal salt.
It would have been obvious to one of ordinary skill in the art, before the effective filing date of the claimed invention, to have selected the MgS particles of modified Chu to have a particle size of 0.05 to 10 µm (i.e. 50 nm to 10 µm) with a reasonable expectation that such a particle size would result in successful MgS particles for use in a coating layer for an anode.
The range rendered obvious by modified Chu overlaps the claimed range of 10 nm to 2000 nm. It would have been obvious to one of ordinary skill in the art, before the effective filing date of the claimed invention, to have selected the overlapping portion of the range disclosed in the prior art with a reasonable expectation that magnesium sulfide particles with a particle size (D50) of 50 nm to 2000 nm would result in a successful magnesium-based particles for use in a coating layer (MPEP 2144.05, I).
Claim(s) 7 and 12 is/are further rejected under 35 U.S.C. 103 as being unpatentable over Chu et al. (US-6402795-B1) in view of Coowar et al. (US-20130069601-A1) as applied to Claims 1 and 8, above, and in view of Ku et al. (US-20200136178-A1; previously cited).
Regarding Claim 7, modified Chu renders obvious all of the limitations as set forth in Claim 1, above. Although modified Chu does not explicitly teach that the anode further comprises “a charge product containing lithium between the coating layer and the anode current collector when the all-solid-state battery is charged”, modified Chu renders obvious a substantially similar coating layer structure (see rejection of Claim 1, above) and therefore it is understood that the coating layer of the prior art necessarily and inherently precipitates a charge product containing lithium between the coating layer and the anode current collector when the battery is charged (MPEP 2112.01), as evidenced by the instant specification [instant specification: 0054-0055, 0059-0060].
Assuming, arguendo, that Applicant is able to persuasively provide evidence that modified Chu lacks a critical structure that enables the prior art to possess lithium between the coating layer and the anode current collector when the all-solid-state battery is charged, this limitation would still be obvious since Ku teaches that lithium can be precipitated between a first anode active material layer and an anode current collector through charging [0055]. Specifically, Ku teaches that precipitation of a lithium layer can be achieved by performing charging in excess of the charge capacity of the first anode active material layer [0055]. Advantageously, Ku teaches that this allows for lithium to be used as an anode active material in the secondary battery, and that the precipitated metal layer serves to suppress the precipitation growth of lithium dendrite, thereby suppressing a short circuit [0055].
Therefore, in seeking to suppress a short circuit and use lithium metal as an anode active material, it would have been obvious to one of ordinary skill in the art, before the effective filing date of the claimed invention, to have overcharged the coating layer of modified Chu such that a charge product containing lithium is formed between the coating layer and the anode current collector with a reasonable expectation that such a configuration would result in a successful all-solid-state battery.
Regarding Claim 12, modified Chu renders obvious all of the limitations as set forth in Claim 8, above. Although modified Chu does not explicitly teach that the anode further comprises “a charge product containing lithium between the coating layer and the anode current collector when the all-solid-state battery is charged”, modified Chu renders obvious a substantially similar coating layer structure (see rejection of Claim 8, above) and therefore it is understood that the coating layer of the prior art necessarily and inherently precipitates a charge product containing lithium between the coating layer and the anode current collector when the battery is charged (MPEP 2112.01), as evidenced by the instant specification [instant specification: 0054-0055, 0059-0060].
Assuming, arguendo, that Applicant is able to persuasively provide evidence that modified Chu lacks a critical structure that enables the prior art to possess lithium between the coating layer and the anode current collector when the all-solid-state battery is charged, this limitation would still be obvious since Ku teaches that lithium can be precipitated between a first anode active material layer and an anode current collector through charging [0055]. Specifically, Ku teaches that precipitation of a lithium layer can be achieved by performing charging in excess of the charge capacity of the first anode active material layer [0055]. Advantageously, Ku teaches that this allows for lithium to be used as an anode active material in the secondary battery, and that the precipitated metal layer serves to suppress the precipitation growth of lithium dendrite, thereby suppressing a short circuit [0055].
Therefore, in seeking to suppress a short circuit and use lithium metal as an anode active material, it would have been obvious to one of ordinary skill in the art, before the effective filing date of the claimed invention, to have overcharged the coating layer of modified Chu such that a charge product containing lithium is formed between the coating layer and the anode current collector with a reasonable expectation that such a configuration would result in a successful all-solid-state battery.
Claim(s) 1-2 and 7-9 and 12 is/are further rejected under 35 U.S.C. 103 as being unpatentable over Chu et al. (US-6402795-B1) in view of Coowar et al. (US-20130069601-A1), and in further view of Wakita et al. (US-20090011333-A1).
Regarding Claim 1, Chu discloses an anode (electrode precursor 17’, Fig. 2). The preamble recitation of an anode “for an all-solid-state battery” amounts to a recitation of the intended use of the claimed anode. The recitation of the intended use of the claimed invention must further limit the structure of the claimed invention in order to be given patentable weight (MPEP 2111.02, II). Since the recitation of “for an all-solid-state battery” does not further limit the structure of the claimed anode, the intended use limitation “for an all solid-state battery” is not given patentable weight, since the anode of the prior art is fully capable of being used in an all-solid-state battery.
Chu thereby discloses an anode for an all-solid-state battery, the anode comprising (Col. 2, lines 19- 66; Col. 3, lines 7-18, 41-48; Col. 5, lines 1-10):
an anode current collector (14, Fig. 2); and
a coating layer (wetting layer 15, Fig. 2) contacting the anode current collector (see Fig. 2) prior to an initial charging of the all-solid-state battery (Col. 2, line 58 – Col. 3, line 2; Col. 5, lines 4-10; Col. 8, lines 61-67).
Chu discloses that the coating layer (wetting layer 15) can be formed of various materials that lower the energy of plating (Col. 6, lines 45-46), such as materials that alloy with lithium and materials that intercalate lithium (Col. 6, lines 46-49). Examples of such materials include carbon and metal sulfides such as titanium sulfide and iron sulfide (Col. 6, lines 51-52).
Although Chu does not disclose a specific example where both carbon and a metal sulfide are used together, the Examiner notes that combining equivalents known for the same purpose represents a prima facie case of obviousness (MPEP 2144.06, I). It would have been obvious to one of ordinary skill in the art, before the effective filing date of the claimed invention, to have used a combination of carbon and a metal sulfide with a reasonable expectation that such a configuration would have resulted in a successful coating layer for use in an anode.
As laid out above, Chu renders obvious that the coating layer (wetting layer) consists of a combination of metal sulfide and carbon, and Chu discloses that the materials of the coating layer either alloy with lithium or intercalate lithium (Col. 6, lines 45-52). Chu does not teach that the coating layer comprises a magnesium-based particle.
Coowar teaches a lithium ion battery including an anode comprising an electroactive material [0056-0057]. Coowar teaches electroactive materials which are able to both incorporate and release metal ion charge carriers such as lithium [0070]. Coowar teaches specific examples of the electroactive materials include, from a list of potential candidates, MgS [0071]. The Examiner notes that this establishes MgS as a metal sulfide material which is able to intercalate lithium ions.
It would have been obvious to one of ordinary skill in the art, before the effective filing date of the claimed invention, to have selected the metal sulfide of the coating layer of Chu to be MgS with a reasonable expectation that such a metal sulfide would result in a successful coating layer, since the selection of a known material based on its suitability for its intended use supports a prima facie case of obviousness (MPEP 2144.07).
Therefore, modified Chu renders obvious that the coating layer consists of:
a carbon material (carbon; Chu: Col. 6, line 51); and
a magnesium-based particle including a magnesium compound comprising MgS.
Although Chu does not specifically teach the content of carbon and the content of magnesium-based particles (i.e. MgS), modified Chu is understood to inherently possess ranges which overlap with the claimed ranges (see rejection of Claim 1 over Chu and Coowar, above; MPEP 2144.05, I).
Assuming, arguendo, that Applicant is able to show by means of persuasive argument or evidence that Chu in view of Coowar does not possess contents of carbon material and MgS which overlap the claimed ranges, the content of each would still have been obvious in view of the teachings of Wakita. Specifically, Wakita teaches that an anode material capable of improving cycle characteristics while securing input and output characteristics [0012]. The anode material is a carbon material coated with “at least one of an alkali metal salt and an alkali earth metal salt” [0031-0033, 0039-0041]. The Examiner notes that magnesium sulfide (MgS) is a form of alkaline earth metal salt, and therefore the anode material of Wakita corresponds to the coating layer of modified Chu. Wakita teaches that changes in the crystal structure of the carbon material during intercalation and deintercalation of an electrode reactant (i.e. lithium) is extremely small, and therefore a high energy density can be obtained [0032]. Wakita further teaches that the alkaline earth metal salt facilitates intercalation/de-intercalation of the electrode reactant and improves the chemical stability of the carbon material [0039].
In seeking to maximize energy density while providing sufficient alkaline earth metal salt (i.e. magnesium sulfide) such that the chemical stability of the carbon material is improved, one of ordinary skill in the art, before the effective filing date of the claimed invention, would have found it obvious to have optimized the contents of carbon material and magnesium-based particle, including selecting contents of each which fall within the claimed ranges (MPEP 2144.05, II). One of ordinary skill in the art would have had a reasonable expectations that selecting the content of carbon material to fall within the range of 10% to 70% by weight and selecting the content of magnesium-based particle to fall within the range of 30% to 90% by weight would result in a successful balance between energy density and chemical stability in the coating layer.
Chu discloses that the coating layer does not have any lithium prior to the initial charging of the all-solid-state battery (Col. 2, line 58 – Col. 3, line 2; Col. 5, lines 4-10; Col. 8, line 61 Col. 9, line 4), and that the coating layer is a monolayer structure (see Fig. 2).
Chu discloses that the coating layer can have a thickness between 50 and 1000 angstroms (Col. 6, lines 57-59). Therefore, although modified Chu does not explicitly teach that the coating layer has a thickness of 0.1 µm to 20 µm, it would have been obvious to one of ordinary skill in the art, before the effective filing date of the claimed invention, to have selected the coating layer to have a thickness of 1000 angstroms (i.e. 0.1 µm) with a reasonable expectation that such a configuration would result in a successful coating layer for an anode (MPEP 2144.05, I).
Regarding Claim 2, modified Chu renders obvious all of the limitations as set forth above. Chu further discloses that the anode current collector be selected from the group consisting of copper, nickel, stainless steel and zinc (Chu: Claim 12). Therefore, it would have been obvious to one of ordinary skill in the art, before the effective filing date of the claimed invention, to have selected the anode current collector to comprise nickel or stainless steel with a reasonable expectation that such a configuration would have resulted in a successful anode current collector.
Regarding Claim 7, modified Chu renders obvious all of the limitations as set forth above. Although modified Chu does not explicitly teach that the anode further comprises “a charge product containing lithium between the coating layer and the anode current collector when the all-solid-state battery is charged”, the Examiner notes that this limitation amounts to the intended use of the claimed anode. The recitation of intended use of a claimed invention must result in a structural difference between the claimed invention and the prior art in order to patentably distinguish the claimed invention from the prior art. If the prior art is capable of performing the intended use, then it meets the limitation of the claim. Here, modified Chu renders obvious the claimed configuration of the anode necessary to perform the intended use limitation. Specifically, modified Chu teaches an anode current collector, a coating layer contacting the anode current collector, wherein the coating layer consists of a carbon material and a magnesium-based particle including a magnesium compound comprising MgS. Therefore, the prior art has the structure necessary to perform the intended use limitation. Thus, the intended use limitation is met.
Additionally, since the structure rendered obvious by the prior art is substantially similar to the claimed structure (as laid out above), it is understood that the anode of the prior art necessarily and inherently undergoes the claimed transformation during charging, as evidenced by the instant specification [instant specification: 0054-0055, 0059-0060].
Regarding Claim 8, Chu discloses an electrode precursor wherein a protective layer (18, Fig. 2) is deposited onto the surface of a current collector (14, Fig. 2) with a wetting layer (15, Fig. 2) between the protective layer and the current collector (Col. 2, lines 19- 57; Col. 3, lines 7-18; Col. 5, lines 1-10). The electrode precursor can then be converted to an alkali metal electrode by an initial charging operation, in which lithium plates from the positive electrode (Col. 2, lines 58-66). In such a charging method, the electrode precursor is assembled with other battery elements including an electrolyte and a positive electrode (Col. 2, lines 58-61). Chu further discloses that current collectors contact both the positive and negative electrodes in a conventional manner (Col. 11, lines 24-27), and that the protective layer can be used directly as a solid electrolyte (Col. 11, lines 14-16).
Therefore, although not disclosed in a single embodiment, one of ordinary skill in the art, before the effective filing date of the claimed invention, would have found it obvious to have provided an all-solid-state battery (corresponds to a battery assembled with an electrode precursor) wherein the protective layer (18, Fig. 2) is used directly as a solid electrolyte, with a reasonable expectation that using the protective layer as a solid electrolyte would result in a successful all-solid-state battery.
The configuration of the all-solid-state battery rendered obvious by Chu can be visualized using the annotation of Chu Fig. 3, below. Notably, the configuration disclosed in Chu Fig. 3 comprises a lithium layer (314; Col. 11, lines 33-48) and an electrolyte region (316; Col. 11, lines 43-50), which are not present in the all-solid-state battery comprising the electrode precursor as rendered obvious by Chu (see above; Col. 2, line 58 – Col. 3, line 2; Col. 8, line 61 – Col. 9, line 4) wherein the protective layer is used directly as a solid electrolyte (see above; Col. 11, lines 13-21). Accordingly, the solid electrolyte layer as rendered obvious by Chu is understood to contact the coating layer and the cathode.
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Annotation of Chu Fig. 3.
Therefore, as depicted in the annotation of Chu, Fig. 3 (above), the all-solid-state battery comprises (Col. 8, line 61 – Col. 9, line 4; Col. 11, lines 14-16, 33-43):
a cathode (corresponds to the combination of positive electrode 318 and positive current collector 320);
an anode comprising an anode current collector (negative current collector 312, Fig. 3) and a coating layer (wetting layer 313, Fig. 3) on the anode current collector,
a solid electrolyte layer (protective layer 308) between the cathode and the anode, wherein the solid electrolyte layer contacts the cathode and the coating layer of the anode, wherein:
the solid electrolyte layer is a first monolayer structure, and
the coating layer is a second monolayer structure.
Chu discloses that the coating layer (wetting layer) can be formed of various materials that lower the energy of plating (Col. 6, lines 45-46), such as materials that alloy with lithium and materials that intercalate lithium (Col. 6, lines 46-49). Examples of such materials include carbon and metal sulfides such as titanium sulfide and iron sulfide (Col. 6, lines 51-52).
Although Chu does not disclose a specific example where both carbon and a metal sulfide are used together, the Examiner notes that combining equivalents known for the same purpose represents a prima facie case of obviousness (MPEP 2144.06, I). Therefore, it would have been obvious to one of ordinary skill in the art, before the effective filing date of the claimed invention, to have used a combination of carbon and a metal sulfide with a reasonable expectation that such a configuration would have resulted in a successful coating layer for use in an anode.
As laid out above, Chu renders obvious that the coating layer (wetting layer) consists of a combination of metal sulfide and carbon, and Chu discloses that the materials of the coating layer either alloy with lithium or intercalate lithium (Col. 6, lines 45-52). Chu does not teach that the coating layer comprises a magnesium-based particle.
Coowar teaches a lithium ion battery including an anode comprising an electroactive material [0056-0057]. Coowar teaches electroactive materials which are able to both incorporate and release metal ion charge carriers such as lithium [0070]. Coowar teaches specific examples of the electroactive materials include, from a list of potential candidates, MgS [0071]. The Examiner notes that this establishes MgS as a metal sulfide material which is able to intercalate lithium ions.
Therefore, it would have been obvious to one of ordinary skill in the art, before the effective filing date of the claimed invention, to have selected the metal sulfide of the coating layer of Chu to be MgS with a reasonable expectation that such a metal sulfide would result in a successful coating layer, since the selection of a known material based on its suitability for its intended use supports a prima facie case of obviousness (MPEP 2144.07).
Therefore, modified Chu renders obvious that the coating layer consists of:
a carbon material (carbon; Chu: Col. 6, line 51); and
a magnesium-based particle including a magnesium compound comprising MgS.
Although Chu does not specifically teach the content of carbon and the content of magnesium-based particles (i.e. MgS), modified Chu is understood to inherently possess ranges which overlap with the claimed ranges (see rejection of Claim 8 over Chu and Coowar, above; MPEP 2144.05, I).
Assuming, arguendo, that Applicant is able to show by means of persuasive argument or evidence that Chu in view of Coowar does not possess contents of carbon material and MgS which overlap the claimed ranges, the content of each would still have been obvious in view of the teachings of Wakita. Specifically, Wakita teaches that an anode material capable of improving cycle characteristics while securing input and output characteristics [0012]. The anode material is a carbon material coated with “at least one of an alkali metal salt and an alkali earth metal salt” [0031-0033, 0039-0041]. The Examiner notes that magnesium sulfide (MgS) is a form of alkaline earth metal salt, and therefore the anode material of Wakita corresponds to the coating layer of modified Chu. Wakita teaches that changes in the crystal structure of the carbon material during intercalation and deintercalation of an electrode reactant (i.e. lithium) is extremely small, and therefore a high energy density can be obtained [0032]. Wakita further teaches that the alkaline earth metal salt facilitates intercalation/de-intercalation of the electrode reactant and improves the chemical stability of the carbon material [0039].
In seeking to maximize energy density while providing sufficient alkaline earth metal salt (i.e. magnesium sulfide) such that the chemical stability of the carbon material is improved, one of ordinary skill in the art, before the effective filing date of the claimed invention, would have found it obvious to have optimized the contents of carbon material and magnesium-based particle, including selecting contents of each which fall within the claimed ranges (MPEP 2144.05, II). One of ordinary skill in the art would have had a reasonable expectations that selecting the content of carbon material to fall within the range of 10% to 70% by weight and selecting the content of magnesium-based particle to fall within the range of 30% to 90% by weight would result in a successful balance between energy density and chemical stability in the coating layer.
Chu discloses that the coating layer does not have any lithium prior to an initial charging of the all-solid-state battery (Col. 2, line 58 – Col. 3, line 2; Col. 5, lines 4-10; Col. 8, line 61 Col. 9, line 4).
Chu discloses that the coating layer can have a thickness between 50 and 1000 angstroms (Col. 6, lines 57-59). Therefore, although modified Chu does not explicitly teach that the coating layer has a thickness of 0.1 µm to 20 µm, it would have been obvious to one of ordinary skill in the art, before the effective filing date of the claimed invention, to have selected the coating layer to have a thickness of 1000 angstroms (i.e. 0.1 µm) with a reasonable expectation that such a configuration would result in a successful coating layer for an anode (MPEP 2144.05, I).
Regarding Claim 9, modified Chu renders obvious all of the limitations as set forth above. Chu further discloses that the anode current collector be selected from the group consisting of copper, nickel, stainless steel and zinc (Chu: Claim 12). Therefore, it would have been obvious to one of ordinary skill in the art, before the effective filing date of the claimed invention, to have selected the anode current collector to comprise nickel or stainless steel with a reasonable expectation that such a configuration would have resulted in a successful anode current collector.
Regarding Claim 12, modified Chu renders obvious all of the limitations as set forth above. Although modified Chu does not explicitly teach that the all-solid-state battery further comprises “a charge product containing lithium between the coating layer and the anode current collector when the all-solid-state battery is charged”, Examiner notes that this limitation amounts to the intended use of the claimed all-solid-state battery. The recitation of intended use of a claimed invention must result in a structural difference between the claimed invention and the prior art in order to patentably distinguish the claimed invention from the prior art. If the prior art is capable of performing the intended use, then it meets the limitation of the claim. Here, the prior art renders obvious the claimed configuration of the anode necessary to perform the intended use limitation. Specifically, the prior art teaches an anode current collector, a coating layer contacting the anode current collector, wherein the coating layer consists of a carbon material and a magnesium-based particle including a magnesium compound comprising MgS. Therefore, the prior art has the structure necessary to perform the intended use limitation. Thus, the intended use limitation is met.
Additionally, since the structure rendered obvious by the prior art is substantially similar to the claimed anode structure (as laid out above), it is understood that the all-solid-state battery of the prior art necessarily and inherently undergoes the claimed transformation during charging, as evidenced by the instant specification [instant specification: 0054-0055, 0059-0060].
Claim(s) 4 and 10 is/are further rejected under 35 U.S.C. 103 as being unpatentable over Chu et al. (US-6402795-B1) in view of Coowar et al. (US-20130069601-A1) and if view of Wakita et al. (US-20090011333-A1) as applied to Claims 1 and 8, above, and in view of Miyaki et al. (US-20020114993-A1; previously cited).
Regarding Claim 4, modified Chu renders obvious all of the limitations as set forth above, including that the coating layer comprises MgS. Modified Chu does not teach the size (D50) of MgS.
Miyaki teaches a protective layer which can be formed on a negative electrode for a lithium secondary battery [0009, 0058]. The protective layer can include alkaline earth metal salts, such as magnesium-based metal salts, which particularly preferably have a particle size of 0.05 to 10 µm [0028-0030]. The Examiner notes that MgS is a form of alkaline earth metal salt.
It would have been obvious to one of ordinary skill in the art, before the effective filing date of the claimed invention, to have selected the MgS particles of modified Chu to have a particle size of 0.05 to 10 µm (i.e. 50 nm to 10 µm) with a reasonable expectation that such a particle size would result in successful MgS particles for use in a coating layer for an anode.
The range rendered obvious by modified Chu overlaps the claimed range of 10 nm to 2000 nm. It would have been obvious to one of ordinary skill in the art, before the effective filing date of the claimed invention, to have selected the overlapping portion of the range disclosed in the prior art with a reasonable expectation that magnesium sulfide particles with a particle size (D50) of 50 nm to 2000 nm would result in a successful magnesium-based particles for use in a coating layer (MPEP 2144.05, I).
Regarding Claim 10, modified Chu renders obvious all of the limitations as set forth above, including that the coating layer comprises MgS. Modified Chu does not teach the size (D50) of MgS.
Miyaki teaches a protective layer which can be formed on a negative electrode for a lithium secondary battery [0009, 0058]. The protective layer can include alkaline earth metal salts, such as magnesium-based metal salts, which particularly preferably have a particle size of 0.05 to 10 µm [0028-0030]. The Examiner notes that MgS is a form of alkaline earth metal salt.
It would have been obvious to one of ordinary skill in the art, before the effective filing date of the claimed invention, to have selected the MgS particles of modified Chu to have a particle size of 0.05 to 10 µm (i.e. 50 nm to 10 µm) with a reasonable expectation that such a particle size would result in successful MgS particles for use in a coating layer for an anode.
The range rendered obvious by modified Chu overlaps the claimed range of 10 nm to 2000 nm. It would have been obvious to one of ordinary skill in the art, before the effective filing date of the claimed invention, to have selected the overlapping portion of the range disclosed in the prior art with a reasonable expectation that magnesium sulfide particles with a particle size (D50) of 50 nm to 2000 nm would result in a successful magnesium-based particles for use in a coating layer (MPEP 2144.05, I).
Claim(s) 7 and 12 is/are further rejected under 35 U.S.C. 103 as being unpatentable over Chu et al. (US-6402795-B1) in view of Coowar et al. (US-20130069601-A1) and in view of Wakita et al. (US-20090011333-A1) as applied to Claims 1 and 8, above, and in view of Ku et al. (US-20200136178-A1; previously cited).
Regarding Claim 7, modified Chu renders obvious all of the limitations as set forth in Claim 1, above. Although modified Chu does not explicitly teach that the anode further comprises “a charge product containing lithium between the coating layer and the anode current collector when the all-solid-state battery is charged”, modified Chu renders obvious a substantially similar coating layer structure (see rejection of Claim 1, above) and therefore it is understood that the coating layer of the prior art necessarily and inherently precipitates a charge product containing lithium between the coating layer and the anode current collector when the battery is charged (MPEP 2112.01), as evidenced by the instant specification [instant specification: 0054-0055, 0059-0060].
Assuming, arguendo, that Applicant is able to persuasively provide evidence that modified Chu lacks a critical structure that enables the prior art to possess lithium between the coating layer and the anode current collector when the all-solid-state battery is charged, this limitation would still be obvious since Ku teaches that lithium can be precipitated between a first anode active material layer and an anode current collector through charging [0055]. Specifically, Ku teaches that precipitation of a lithium layer can be achieved by performing charging in excess of the charge capacity of the first anode active material layer [0055]. Advantageously, Ku teaches that this allows for lithium to be used as an anode active material in the secondary battery, and that the precipitated metal layer serves to suppress the precipitation growth of lithium dendrite, thereby suppressing a short circuit [0055].
Therefore, in seeking to suppress a short circuit and use lithium metal as an anode active material, it would have been obvious to one of ordinary skill in the art, before the effective filing date of the claimed invention, to have overcharged the coating layer of modified Chu such that a charge product containing lithium is formed between the coating layer and the anode current collector with a reasonable expectation that such a configuration would result in a successful all-solid-state battery.
Regarding Claim 12, modified Chu renders obvious all of the limitations as set forth in Claim 8, above. Although modified Chu does not explicitly teach that the anode further comprises “a charge product containing lithium between the coating layer and the anode current collector when the all-solid-state battery is charged”, modified Chu renders obvious a substantially similar coating layer structure (see rejection of Claim 8, above) and therefore it is understood that the coating layer of the prior art necessarily and inherently precipitates a charge product containing lithium between the coating layer and the anode current collector when the battery is charged (MPEP 2112.01), as evidenced by the instant specification [instant specification: 0054-0055, 0059-0060].
Assuming, arguendo, that Applicant is able to persuasively provide evidence that modified Chu lacks a critical structure that enables the prior art to possess lithium between the coating layer and the anode current collector when the all-solid-state battery is charged, this limitation would still be obvious since Ku teaches that lithium can be precipitated between a first anode active material layer and an anode current collector through charging [0055]. Specifically, Ku teaches that precipitation of a lithium layer can be achieved by performing charging in excess of the charge capacity of the first anode active material layer [0055]. Advantageously, Ku teaches that this allows for lithium to be used as an anode active material in the secondary battery, and that the precipitated metal layer serves to suppress the precipitation growth of lithium dendrite, thereby suppressing a short circuit [0055].
Therefore, in seeking to suppress a short circuit and use lithium metal as an anode active material, it would have been obvious to one of ordinary skill in the art, before the effective filing date of the claimed invention, to have overcharged the coating layer of modified Chu such that a charge product containing lithium is formed between the coating layer and the anode current collector with a reasonable expectation that such a configuration would result in a successful all-solid-state battery.
Response to Arguments
Applicant's arguments filed 06/01/2026 have been fully considered but they are not persuasive. Specifically, Applicant has argued that it is unreasonable to reject a claim feature specifying the coating thickness based solely on the fact that a single numerical value (0.1 µm) overlaps (Remarks, Pg. 7 of 9).
The Examiner has carefully considered this argument, but respectfully does not find it persuasive. The Examiner notes that the current evidence of record does not support any criticality to the claimed range, and that a single numerical overlap is sufficient to establish a prima facie case of obviousness. See also In re Bergen, 120 F.2d 329, 332, 49 USPQ 749, 751-52 (CCPA 1941) (The court found that the overlapping endpoint of the prior art and claimed range was sufficient to support an obviousness rejection, particularly when there was no showing of criticality of the claimed range). See also MPEP 2144.05, I.
Applicant has argued that Coowar merely mentions MgS as an anode active material and does not teach MgS for the purpose of inducing uniform lithium deposition as a coating layer for an anode-free all solid state battery (Remarks, Pgs. 7-8 of 9). Accordingly, Applicant submits that the substitution of metal sulfides of Chu for MgS as taught by Coowar is a hindsight reconstruction predicated on prior knowledge of the claimed invention (Remarks, Pg. 8 of 9).
The Examiner has carefully considered this argument, but respectfully does not find it persuasive. The Examiner notes that the primary reference (Chu) discloses that the wetting layer (reads on coating layer) either (i) intercalates alkali metal ions or (ii) alloys with the alkali metal (Col. 2: lines 46-57). When the wetting layer intercalates ions of the alkali metal, “it may be carbon, titanium sulfide, or iron sulfide, for example” (Col. 3: lines 20-25). The teaching reference (Coowar) teaches that an electroactive material is preferably able to incorporate and release lithium, and indicates MgS as a suitable metal sulfide electroactive material [0070-0071]. The Examiner notes that this establishes MgS as an alternative metal sulfide material capable of intercalating alkali metal (i.e. lithium) ions. The selection of a known material based on its suitability for its intended use supported a prima facie obviousness. See MPEP 2144.07.
In response to applicant's argument that the examiner's conclusion of obviousness is based upon improper hindsight reasoning, it must be recognized that any judgment on obviousness is in a sense necessarily a reconstruction based upon hindsight reasoning. But so long as it takes into account only knowledge which was within the level of ordinary skill at the time the claimed invention was made, and does not include knowledge gleaned only from the applicant's disclosure, such a reconstruction is proper. See In re McLaughlin, 443 F.2d 1392, 170 USPQ 209 (CCPA 1971). Here, as discussed above, Chu discloses that the wetting layer contains a material capable of intercalating alkali metal ions, and Coowar teaches that MgS can intercalate lithium ions. As such, only knowledge within the level of one of ordinary skill in the art is relied upon in the rejections of record.
Applicant has argued that Claim 1 now specifies particular contents of the carbon material and the magnesium-based particles (Remarks Pg. 8 of 9). Applicant has argued that the anode active material of Wakita is in a form where an alkaline earth metal salt is coated on the surface of a carbon material, which differs in configuration from the mixture carbon material and metal sulfides disclosed in Chu (Remarks, Pg. 8 of 9). Accordingly, Applicant submits that the optimization of the contents of carbon material and magnesium-based particles according to the teachings of Wakita would not be expected to apply to Chu (Remarks, Pg. 8 of 9).
The Examiner has carefully considered this argument, but respectfully does not find it persuasive. The Examiner notes that Wakita discloses that carbon materials have a high energy density [0032]. Such a teaching is broadly applicable to any carbon material used in battery application. Wakita additionally teaches that providing an alkaline earth metal salt on the surface of the carbon material facilitates intercalation/de-intercalation of the electrode reactant and improves the chemical stability of the carbon material [0039]. Wakita notes that such an effect is achieved when “at least part” of the surface of the anode active material is covered with alkaline earth metal salt [0044]. Also, Wakita notes that the shape, particle diameter, number and the like of the anode active material and the covering particles may be voluntarily set, and are not limited to the aspect shown in Fig. 1 [0047]. The Examiner notes that a mixture of carbon material and MgS (as rendered obvious by modified Chu) results in a configuration wherein a part of the surface of the carbon material (i.e. the anode active material) is necessarily placed in contact with the MgS (i.e. alkaline earth metal salt) material. Since there is no criticality to the size or shape of the materials, the Examiner maintains that one or ordinary skill in the art would have looked optimized the contents of carbon material and magnesium-based particles based on the teachings of Wakita. For the sake of compact prosecution, an alternative rejection is included using the teachings of the primary reference alone to render obvious the claimed contents of carbon material and magnesium-based particles.
Conclusion
Applicant's amendment necessitated the new ground(s) of rejection presented in this Office action. Accordingly, THIS ACTION IS MADE FINAL. See MPEP § 706.07(a). Applicant is reminded of the extension of time policy as set forth in 37 CFR 1.136(a).
A shortened statutory period for reply to this final action is set to expire THREE MONTHS from the mailing date of this action. In the event a first reply is filed within TWO MONTHS of the mailing date of this final action and the advisory action is not mailed until after the end of the THREE-MONTH shortened statutory period, then the shortened statutory period will expire on the date the advisory action is mailed, and any nonprovisional extension fee (37 CFR 1.17(a)) pursuant to 37 CFR 1.136(a) will be calculated from the mailing date of the advisory action. In no event, however, will the statutory period for reply expire later than SIX MONTHS from the mailing date of this final action.
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/D.C.N./Examiner, Art Unit 1751
/Haroon S. Sheikh/Primary Examiner, Art Unit 1751