DETAILED ACTION
This is the second Office Action regarding application number 18/722,173, filed on 06/20/2024, which is a 371 of PCT/JP2022/046454, filed on 12/16/2022, and which claims foreign priority to JP 2021-211381 and JP 2021-205821, filed on 12/24/2021 and 12/20/2021, respectively.
This action is in response to the Applicant’s Response received 12/30/2025.
Status of Claims
Claims 1 and 3-13 are currently pending.
Claim 2 is canceled.
Claims 1, 3, and 5 are amended.
Claims 1 and 3-13 are examined below.
Claims 5 and 6 allowed. All other claims are rejected.
Response to Arguments
The Applicant’s arguments received 12/30/2025 have been carefully considered but they are not found persuasive.
Arguments against the CARTER reference are not compelling because the examiner does not rely on that reference to teach and suggest the claimed ranges.
The examiner did not earlier state that the restriction requirement was withdrawn, and that claims 9-13 are rejoined continue to be examined.
Claim Rejections - 35 USC § 112
Written Description - New Matter
Claims 1 and 3, 4, 7, and 8 are rejected under 35 U.S.C. 112(a) as failing to comply with the written description requirement. The claims contain subject matter which was not described in the specification in such a way as to reasonably convey to one skilled in the relevant art that the inventor or a joint inventor had possession of the claimed invention.
Claim 1 now recites that “the percentage of O is 56.5 at% or greater from the surface to a depth of 1/3 of the film thickness of the hole transport layer when the hole transport layer has a thickness from 5 nm to 60 nm inclusive.” The applicant asserts that written support for this amended is found in paragraphs 111, 113, and 114 of the original specification. The examiner respectfully disagrees. Only for a HTL film thickness range of 60-500nm is the range of ≥56.5 at% described in para. 113. Para. 114 discloses only a range of ≥57.0 at% when the HTL thickness is 5-60nm.
Claim Rejections - 35 USC § 112
Indefiniteness
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.
Claims 1 and 3, 4, 7, and 8 are rejected under 35 U.S.C. 112 as being indefinite for failing to particularly point out and distinctly claim the subject matter which the inventor or a joint inventor, or for pre-AIA the applicant regards as the invention.
Claim 1 recites the following conflicting limitations: “when the hole transport layer has a thickness from 60 nm to 500 nm inclusive” (lines 14-15) and “when the hole transport layer has a thickness from 5 nm to 60 nm inclusive” (lines 17-18). The claim is indefinite because a reader would be unable to determine which of the two surface depths are required when the HTL thickness is 60 nm, since both conditions would seem to apply but the depth requirements are partially contradictory. The examiner understands the word “inclusive” to mean that the range endpoints are included. Claims 3, 4, 7, and 8 are also rejected because they each incorporate by reference the indefinite language of claim 1.
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 of this title, 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 set forth in Graham v. John Deere Co., 383 U.S. 1, 148 USPQ 459 (1966), that are applied for establishing a background for determining obviousness under 35 U.S.C. 103 are summarized as follows:
1. Determining the scope and contents of the prior art.
2. Ascertaining the differences between the prior art and the claims at issue.
3. Resolving the level of ordinary skill in the pertinent art.
4. Considering objective evidence present in the application indicating obviousness or nonobviousness.
Claims 1, 3, 4, 7, and 9-13 are rejected under 35 U.S.C. 103 as being unpatentable over KUBOTA (JP 2019-114691 A) in view of THIRUCHELVAN (“Combustion Processed Nickel Oxide and Zinc Doped Nickel Oxide Thin Films as a Hole Transport Layer for Perovskite Solar Cells”). DUBEY (The effect of stoichiometry on the structural, thermal and electronic properties of thermally decomposed nickel oxide) is an evidentiary reference.
Regarding claims 1 and 9, KUBOTA teaches a photoelectric conversion element comprising, in sequence:
a first conductive layer (ITO 110) having light transparency;
a hole transport layer (nickel oxide HTL 120);
a light-absorbing layer (perovskite 130);
an electron transport layer (PCBM fullerene 140); and
a second conductive layer (silver electrode layer 150),
wherein light incident through the first conductive layer is photoelectrically converted.
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KUBOTA does not disclose expressly that the hole transport layer includes zinc or possesses the recited elemental atomic percent ranges. KUBOTA describes how the authors determined that there should be a greater atomic amount of oxygen than nickel, such as a ratio of O/Ni of 1.10.
THIRUCHELVAN a 5% Zn-NiOx as the HTL in a perovskite solar cell, and that this HTL material produced improved power conversion efficiency. Figure 6 teaches that the zinc at% is about 3% and nickel is about 30%.
Skilled artisans would have found it obvious to modify KUBOTA and add zinc to the nickel oxide HTL in order to improve power conversion efficiency as taught by THIRUCHELVAN.
Both KUBOTA and THIRUCHELVAN suggest that nickel vacancies/oxygen-richness generate the p-type behavior of this material, and although neither appears to explicitly recite the oxygen range claimed, they are sufficiently instructive to skilled artisans that the relative oxygen amount will affect the material performance. Here, the prior art compositions include identical elements and are substantially similar in amount and proportion, that skilled artisans would have expected them to have the same properties. MPEP 2144.05(I).
Further, DUBEY establishes that the Ni:O stoichiometry is a result effective variable. DUBEY asserts that nickel oxide is the most exhaustively investigated transition metal oxide, and that nickel oxide’s electrical, optical, and thermal properties “depend strongly” on its stoichiometry. Skilled artisans would, without doubt, instantly comprehend the criticality of the Ni:O elemental ratio and its influence on layer function and performance as a hole transport layer in a solar cell.
Further, a prima facie case of obviousness exists where the claimed ranges or amounts do not overlap with the prior art but are merely close. Titanium Metals; MPEP 2144.05. Here, the oxygen range taught by the prior art is substantially near the claimed range, and thus is prima facie obvious, with the burden shifting to the applicant to demonstrate compelling rationale of non-obviousness.
Regarding claim 3, modified KUBOTA teaches the photoelectric conversion element according to claim 2, wherein
the hole transport layer has a thickness from 5 nm to 500 nm inclusive (KUBOTA, para. 33, 20nm of less for HTL thickness), and
the percentage of O is 57.0 at% or greater from the surface of the hole transport layer to a depth of 20 nm in a depth direction.
Regarding claim 4, modified KUBOTA teaches the photoelectric conversion element according to claim 1, wherein
the electron transport layer contains fullerene or phenyl-C61-butyric acid methyl ester (PCBM, KUBOTA, para. 22).
Regarding claim 7, modified KUBOTA teaches the photoelectric conversion element according to claim 1, further comprising a substrate having flexibility (KUBOTA, para. 34 teaches a stainless-steel substrate, and stainless steel is made flexible by the routine adjustment of thickness size dimension, and is a prima facie obvious change, MPEP 2144.04(IV)(A)).
Regarding claim 10, modified KUBOTA teaches the photoelectric conversion element comprising a light-absorbing layer, an electron transport layer, and a second conductive layer, in this order on the surface of the hole transport layer of the laminated film according to claim 9 (see rejection of claim 9 above with claim 1).
Regarding claim 11, modified KUBOTA teaches the manufacturing method of a laminated film, comprising: forming a first conductive layer on a substrate; forming a hole transport layer including Zn-doped nickel oxide on the first conductive layer; and
UV ozone treating the hole transport layer (KUBOTA does these steps including the UV ozone treatment, para. 27; entirety of claim 1 rejection above is applied here).
Regarding claim 12, modified KUBOTA teaches the manufacturing method according to claim 11, wherein in the hole transport layer, the percentage of Ni is from 30 at% to 40 at% inclusive, the percentage of O is from 55 at% to 60 at% inclusive, and the percentage of Zn is from 3 at% to 15 at% inclusive.
Both KUBOTA and THIRUCHELVAN suggest that nickel vacancies/oxygen-richness generate the p-type behavior of this material, and although neither appears to explicitly recite the ranges claimed, they are sufficiently instructive to skilled artisans that the relative zinc and oxygen amount will affect the material performance. Here, the prior art compositions include identical elements and are substantially similar in amount and proportion, that skilled artisans would have expected them to have the same properties. MPEP 2144.05(I).
Regarding claim 13, modified KUBOTA teaches the laminated film according to claim 9, wherein
the percentage of O is 56.5 at% or greater from a surface of the hole transport layer remote from the first conductive layer to a depth of 20 nm or from the surface to a depth of 1/3 of the film thickness of the hole transport layer (the information within the cited references suggests that the element compositions would be uniform since there is no indication of variation in the thickness direction).
Claim 8 is rejected under 35 U.S.C. 103 as being unpatentable over KUBOTA (JP 2019-114691 A) in view of THIRUCHELVAN (“Combustion Processed Nickel Oxide and Zinc Doped Nickel Oxide Thin Films as a Hole Transport Layer for Perovskite Solar Cells”) as applied to claim 1 above, and further in view of GHOSH (Superior Performance of Silver Bismuth Iodide Photovoltaics Fabricated via Dynamic Hot-Casting Method under Ambient Conditions).
Regarding claim 8, modified KUBOTA teaches the photoelectric conversion element according to claim 1, but does not disclose expressly that the light-absorbing layer expressed by a composition formula AgaBibIc, and in the composition formula, the composition ratio a, b, and c satisfies c=a+3b and 2≤b/a≤2.5.
GHOSH teaches light-absorbing layer materials of AgBiI having the claimed composition formula (Table 1), and explains to readers that these materials have recently gained a lot of attention as lead-free perovskite materials and represent the highest efficiency for solution processed air-stable lead-free perovskite solar cells (abstract).
Skilled artisans would have found it obvious to modify KUBOTA and replace its perovskite with the AgBiI perovskite because this material is free of the “highly toxic Pb2+” element and provides high efficiency in a solar cell as taught by GHOSH.
Conclusion
No claim is allowed.
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 extension fee 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.
Contact Information
Any inquiry concerning this communication or earlier communications from the examiner should be directed to ANGELO TRIVISONNO whose telephone number is (571) 272-5201 or by email at <angelo.trivisonno@uspto.gov>. The examiner can normally be reached on MONDAY-FRIDAY, 9:00a-5:00pm EST. The examiner's supervisor, NIKI BAKHTIARI, can be reached at (571) 272-3433.
/ANGELO TRIVISONNO/
Primary Examiner