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 claims
The amendment to claims filed on 7/7/2026 is acknowledged. Claims 1-2, 12, 14, 16, 19-20 and 30 are amended. Currently claims 1-2, 12-22, and 27-30 are pending in the application with claims 1-2 being withdrawn from consideration.
Previous 112 rejections are withdrawn in view of the above amendment.
Previous prior art rejection is withdrawn in view of the above amendment.
Claims 12-22 and 27-30 are rejected on a new ground of disclosure.
Claim Rejections - 35 USC § 112
The following is a quotation of 35 U.S.C. 112(b):
(b) CONCLUSION.—The specification shall conclude with one or more claims particularly pointing out and distinctly claiming the subject matter which the inventor or a joint inventor regards as the invention.
The following is a quotation of 35 U.S.C. 112 (pre-AIA ), second paragraph:
The specification shall conclude with one or more claims particularly pointing out and distinctly claiming the subject matter which the applicant regards as his invention.
Claims 16, 19 and 28 are rejected under 35 U.S.C. 112(b) or 35 U.S.C. 112 (pre-AIA ), second paragraph, as being indefinite for failing to particularly point out and distinctly claim the subject matter which the inventor or a joint inventor (or for applications subject to pre-AIA 35 U.S.C. 112, the applicant), regards as the invention.
As amended, claim 16 depends on claim 12 and recites “the additive comprises at least two of: TAH, D4TBP, choline chloride (CC),gallium acetylacetonate (Ga(AcAc)3, oleylamine (OAM), or potassium thiocyanate (KSCN), while claim 12 is amended to recite “the additive comprises at least one of: tetradecyl dimethyl (3-sulfopropyl) ammonium hydroxide inner salt (TAH) or D-4-tert-butyl-Phe (D4TBP)” in lines 8-10. As such, claim 16 recites a broader range of selections that is different from the selection recited in claim 12, e.g. a selection of two additives that are not TAH and D4TBP. A broad range or limitation together with a narrow range or limitation that falls within the broad range or limitation (in the same claim) may be considered indefinite if the resulting claim does not clearly set forth the metes and bounds of the patent protection desired. See MPEP § 2173.05(c). The claim(s) are considered indefinite because there is a question or doubt as to whether the feature introduced by such narrower language is (a) merely exemplary of the remainder of the claim, and therefore not required, or (b) a required feature of the claims.
As amended, claim 19 depends on claim 12, and recites “the additive comprising at least two of: TAH, D4TBP, choline chloride (CC), gallium acetylacetonate (Ga(AcAc)3), oleylamine (OM), or potassium thiocyanate (KSCN)” in lines 5-8; while claim 12 recites “tetradecyl dimethyl (3-sulfopropyl) ammonium hydroxide inner salt (TAH) or D-4-tert-butyl-Phe (D4TBP)” in lines 8-10. As such, claim 19 recites a broader range than the range recited in claim 12, e.g. selection of two additives that are not TAH and D4TBP. A broad range or limitation together with a narrow range or limitation that falls within the broad range or limitation (in the same claim) may be considered indefinite if the resulting claim does not clearly set forth the metes and bounds of the patent protection desired. See MPEP § 2173.05(c). The claim(s) are considered indefinite because there is a question or doubt as to whether the feature introduced by such narrower language is (a) merely exemplary of the remainder of the claim, and therefore not required, or (b) a required feature of the claims.
Claim 28 depends on claim 12 and recites “the additive comprises at least two of TAH, CC, Ga(AcAc)3, Pb(SCN)2, KSCN, OAM, PbCl2, D4TBP or 4FPEAI”; while claim 12 is amended to recite “the additive comprising at least one of tetradecyl dimethyl (3-sulfopropyl) ammonium hydroxide inner salt (TAH) or D04-tert-butyl-Phe (D4TBP)” in lines 8-10. As such, claim 28 recites a broader selection than the selection recited in claim 12, e.g. selection of two additives that are not TAH and D4TBP. A broad range or limitation together with a narrow range or limitation that falls within the broad range or limitation (in the same claim) may be considered indefinite if the resulting claim does not clearly set forth the metes and bounds of the patent protection desired. See MPEP § 2173.05(c). The claim(s) are considered indefinite because there is a question or doubt as to whether the feature introduced by such narrower language is (a) merely exemplary of the remainder of the claim, and therefore not required, or (b) a required feature of the claims
The following is a quotation of 35 U.S.C. 112(d):
(d) REFERENCE IN DEPENDENT FORMS.—Subject to subsection (e), a claim in dependent form shall contain a reference to a claim previously set forth and then specify a further limitation of the subject matter claimed. A claim in dependent form shall be construed to incorporate by reference all the limitations of the claim to which it refers.
The following is a quotation of pre-AIA 35 U.S.C. 112, fourth paragraph:
Subject to the following paragraph [i.e., the fifth paragraph of pre-AIA 35 U.S.C. 112], a claim in dependent form shall contain a reference to a claim previously set forth and then specify a further limitation of the subject matter claimed. A claim in dependent form shall be construed to incorporate by reference all the limitations of the claim to which it refers.
Claims 16, 19 and 28 are rejected under 35 U.S.C. 112(d) or pre-AIA 35 U.S.C. 112, 4th paragraph, as being of improper dependent form for failing to further limit the subject matter of the claim upon which it depends, or for failing to include all the limitations of the claim upon which it depends.
As amended, claim 16 depends on claim 12 and recites “the additive comprises at least two of: TAH, D4TBP, choline chloride (CC),gallium acetylacetonate (Ga(AcAc)3, oleylamine (OAM), or potassium thiocyanate (KSCN), while claim 12 is amended to recite “the additive comprises at least one of: tetradecyl dimethyl (3-sulfopropyl) ammonium hydroxide inner salt (TAH) or D-4-tert-butyl-Phe (D4TBP)” in lines 8-10. As such, claim 16 recites a broader selection than the selection recited in claim 12, e.g. selection of two additives that are not TAH and D4TBP; and therefore, the claim fails to further limit the subject matter of the claim upon which it depends and fails to include all the limitations of the claim upon which it depends.
As amended, claim 19 depends on claim 12, and recites “the additive comprising at least two of: TAH, D4TBP, choline chloride (CC), gallium acetylacetonate (Ga(AcAc)3), oleylamine (OM), or potassium thiocyanate (KSCN)” in lines 5-8; while claim 12 recites “tetradecyl dimethyl (3-sulfopropyl) ammonium hydroxide inner salt (TAH) or D-4-tert-butyl-Phe (D4TBP)” in lines 8-10. As such, claim 19 recites a broader range than the range recited in claim 12, therefore, the claim fails to further limit the subject matter of the claim upon which it depends and fails to include all the limitations of the claim upon which it depends.
Claim 28 depends on claim 12 and recites “the additive comprises at least two of TAH, CC, Ga(AcAc)3, Pb(SCN)2, KSCN, OAM, PbCl2, D4TBP or 4FPEAI”; while claim 12 is amended to recite “the additive comprising at least one of tetradecyl dimethyl (3-sulfopropyl) ammonium hydroxide inner salt (TAH) or D04-tert-butyl-Phe (D4TBP)” in lines 8-10. As such, claim 28 recites a broader range than the range recited in claim 12, and therefore, the claim fails to further limit the subject matter of the claim upon which it depends and fails to include all the limitations of the claim upon which it depends.
Applicant may cancel the claim(s), amend the claim(s) to place the claim(s) in proper dependent form, rewrite the claim(s) in independent form, or present a sufficient showing that the dependent claim(s) complies with the statutory requirements.
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) 12, 14 and 29 are rejected under 35 U.S.C. 103 as being unpatentable over Snaith et al. (WO 2020/109787) in view of Yang et al. (“Tailoring Passivation Molecular Structures for Extremely Small Open-Circuit Voltage Loss in Perovskite Solar Cells”).
Regarding claims 12 and 14, Snaith et al. discloses method of making a photovoltaic device (see pages 78-79, claims 32-50 and also see pages 54-77) comprising:
depositing a first charge transport layer (NiO) over a first contact layer (FTO-coated glass, see page 78);
applying a precursor solution (or perovskite precursor solution) to a surface of a first charge transport layer (NiO) resulting in a liquid layer of the precursor solution on the surface of the first charge transport layer (see page 79), wherein the precursor solution comprises a perovskite precursor comprising formamidinium iodide (FAI), cesium iodide (CsI), lead bromide (PbBr2), and lead iodide (PbI2), an additive (or ionic liquid such as BMIMBF4), and a solvent (DMF/DMSO, see paragraph bridging pages 78 and 79);
treating the liquid layer to remove at least a portion of the solvent (see annealing step on pre-heated hot plate described in page 79; also see page 63), thereby forming an absorber layer comprising a solid perovskite material (or crystalline A/M/X, see the entire document of Snaith et al., and more specifically claims 320), and crystalline perovskite material is solid.
Snaith et al. teaches using the precursor to form a perovskite material of (FA0.83MA0.17)0.95Cs0.05Pb(I0.9Br0.1)3 in the example described in the paragraph bridging pages 78 and 79, or the perovskite having 10% atomic percent of bromine in the halides.
Snaith et al. teaches the does not teach forming a perovskite material having an atomic percent of bromine in the halides in the range of 5.0% to 9.0% as claimed in claim 12, 6.0% to 9.0% as claimed in claims 12 and 14 in the example described in the paragraph bridging pages 78 and 79.
However, Snaith et al. teaches the atomic percent (y) of bromine (Br) in the halides in the perovskite material (or A/M/X material) of APb[BryI1-y]3 to be greater than 0 and less than 1, or 0.01 to 0.99 or from 1% to 99% (see page 42).
It would have been obvious to one skilled in the art before the effective filing date of the claimed invention to modify the method in the example (described in paragraph bridging pages 78-79) by forming the perovskite material having atomic percent of bromine in the halides in the perovskite material selectively to be 5.0% to 9.0% or 6.0% to 8.0% in the range of greater than 0 and less than 1, or 0.01 to 0.99 or from 1% to 99% described in page 42, because Snaith et al. explicitly suggests doing so and selection of overlapping portion of ranges has been held to be a prima facie case of obviousness. In re Malagari, 182 USPQ 549.
Snaith et al. discloses using BMIMBF4 in the example. Snaith et al. does not teaches using additives as claimed in claim 12.
Yang et al. discloses using passivation molecules such as D4TBP in the perovskite precursor for perovskite grain boundary passivation to achieve higher efficiency (see table S2 and paragraph bridging pages 5785 and 5786).
It would have been obvious to one skilled in the art before the effective filing date of the claimed invention to modify the method of Snaith et al. by using additive comprising D4TBP as taught by Yang, because Yang et al. teaches using D4TBP would provide higher efficiency.
Regarding claim 29, Snaith et al. discloses a method as in claim 12 above, and discloses the perovskite composition is (FA0.83MA0.17)0.95Cs0.05Pb(I0.9Br0.1)3 or Cs0.05MA0.1445 FA0.7885Pb(I0.9Br0.1)3 which is approximately equal (or close enough) to Cs0.05MA0.08FA0.87Pb(I0.92Br0.08)3 .
Snaith et al. does not disclose obtaining the exact composition Cs0.05MA0.08FA0.87Pb(I0.92Br0.08)3 with the atomic percent of bromine to be 0.08 and the atomic percent of and the MA to be 0.08, or (FA0.9158MA0.0842)0.95Cs0.05Pb(I0.92Br0.08)3 in the method described in pages 78-79.
However, Snaith et al. discloses the atomic percent (y) of bromine (Br) in the perovskite material (or A/M/X material) of APb[BryI1-y]3 to be 0.01 to 0.99 (see page 42) and the combining of MA (CH3NH3+) and FA (H2N-C(H)=NH2+) has a combination of formula (CH3NH3)x(H2N-C(H)-NH2)1-x with x being from 0.01 to 0.99 or from 0.05 to 0.95 or 0.1 to 0.9 (see paragraph bridging pages 41-42).
Therefore, it would have been obvious to one skilled in the art to have used the method disclosed in pages 78-29 to form the perovskite having formula (FA0.9158MA0.0842)0.95Cs0.05Pb(I0.92Br0.08)3 with the atomic percent (y) of bromine of 0.08 to be selected in the ranges 0.01 to 0.99 disclosed by Snaith et al., and the atomic percent of MA of 0.0842 to be selected in the ranges 0.01 to 0.99 or from 0.05 to 0.95 or 0.1 to 0.9 disclosed by Snaith et al., because selection of overlapping portion of ranges has been held to be a prima facie case of obviousness. In re Malagari, 182 USPQ 549.
Claim(s) 13 is rejected under 35 U.S.C. 103 as being unpatentable over modified Snaith et al. (WO 2020/109787) as applied to claim 12 above, and further in view of Jung et al. (US 20180075979).
Regarding claim 13, modified Snaith et al. discloses a method as in claim 12 above.
ModifiedSnaith et al. does not disclose the step of treating the liquid layer (or the annealing step) comprises directing nitrogen gas to contact a surface of the liquid layer.
Jung et al. disclose annealing the perovskite solution including subjecting the perovskite material solution to blowing nitrogen or the like to complete drying of the solvent before the coating solution is repelled (see [0030] and [0050]). In other words, Jung et al. discloses the step of treating the liquid layer comprising directing nitrogen gas to contact a surface of the liquid layer, or subjecting the solution to blowing nitrogen.
It would have been obvious to one skilled in the art before the effective filing date of the claimed invention to modify the method of modified Snaith et al. by subjecting the liquid layer to blowing nitrogen, or directing nitrogen gas to contact a surface of the liquid layer, to complete drying of the solvent before the coating solution is repelled as taught by Jung et al.
Claim(s) 15-16, 19 and 30 are rejected under 35 U.S.C. 103 as being unpatentable over modified Snaith et al. as applied to claim 12 above, and further in view of Li et al. (“In situ induced core/shell stabilized hybrid perovskites via gallium (III) acetylacetonate intermediate towards highly efficient and stable solar cells”).
Regarding claim 15, modified Snaith et al. discloses a method as in claim 12 above, wherein Yang et al. teaches treating the perovskite absorber layer with a surface modifier (or passivation molecules – or additives) to surface passivation after the step of forming the absorber layer comprising the perovskite material and prior to providing the second contact layer (see “Device Fabrication” in paragraph bridging pages 5785 and 5786).
Modified Snaith et al. does no teaches using Ga(AcAc) as the surface modifier (or passivation molecules).
Li et al. teaches using gallium (III) acetylacetonate (GaAA3 or Ga(AcAc)) to protect the perovskite against water ingress from ambient atmosphere and passivate its defect state, and thereby enhancing the long term stability while maintaining high PCE (see abstract, “Broader context” and conclusion).
It would have been obvious to one skilled in the art before the effective filing date of the claimed invention to modify the method of modified Snaith et al. by using Ga(AcAc) taught by Li et al. as the surface modifier (or passivation molecules to surface passivation) for the perovskite absorber layer, because Li et al. teaches such surface modifier (or passivation molecules) would protect the perovskite against water ingress from ambient atmosphere and passivate its defect states to enhance the long-term stability while maintaining high PCE.
Regarding claims 16 and 30, modified Snaith et al. discloses a method as in claim 12 above, wherein the additive comprises D4TBP (see claim 12 above). Yang et al. also teaches using multiple additives would provide synergetic passivation and the efficiency would increase (see table 2 and paragraph bridging pages 5782 and 5783).
Modified Snaith et al. does not disclose the additive comprising at least two of TAH, D4TBP, choline chloride (CC), gallium acetylacetonate (Ga(AcAc)3), oleylamine (OAM), or potassium thiocyanate (CSCN) as claimed in claim 16, or further comprising at least one of choline (CC) or gallium acetylacetonate as claimed in claim 30.
Li et al. teaches Li et al. teaches using gallium (III) acetylacetonate (GaAA3 or Ga(AcAc)) to protect the perovskite against water ingress from ambient atmosphere and passivate its defect state, and thereby enhancing the long term stability while maintaining high PCE (see abstract, “Broader context” and conclusion).
It would have been obvious to one skilled in the art before the effective filing date of the claimed invention to modify the method of modified Snaith et al. by incorporating an additive Ga(AcAc)3 taught by Li et al. in addition to D4TBP; because Li et al. teaches (Ga(AcAc)3) would protect the perovskite against water ingress from ambient atmosphere and passivate its defect states to enhance the long-term stability while maintaining high PCE, and Yang teaches using multiple additives would provide synergetic passivation and increased efficiency. In such modification, the additive comprises D4TBP and Ga(AcAc)3.
Regarding claim 19, modified Snaith et al. discloses a method as in claim 12 above, wherein the perovskite having a composition having formula as claimed with z is between 0.06 to 0.09 (see claim 12 above). Snaith et al. also teaches the photovoltaic device including a first charge transport layer (HTL, see NiO) or ptype (see pages 78-79 of Snaith et al.). Yang et al. also teaches the photovoltaic device including a first hole transport layer (see PTAA in fig. 1a of Yang et al.), and using multiple additives would provide synergetic passivation and the efficiency would increase (see table 2 and paragraph bridging pages 5782 and 5783 of Yang et al.).
Modified Snaith et al. does not explicitly taches the additive comprising at least two of TAH, D4TBP, choline chloride (CC), gallium acetylacetonate (Ga(AcAc)3), oleylamine (OAM), or potassium thiocyanate (KSCN).
Li et al. teaches Li et al. teaches using gallium (III) acetylacetonate (GaAA3 or Ga(AcAc)) to protect the perovskite against water ingress from ambient atmosphere and passivate its defect state, and thereby enhancing the long term stability while maintaining high PCE (see abstract, “Broader context” and conclusion).
It would have been obvious to one skilled in the art before the effective filing date of the claimed invention to modify the method of modified Snaith et al. by incorporating an additive Ga(AcAc)3 taught by Li et al. in addition to D4TBP; because Li et al. teaches (Ga(AcAc)3) would protect the perovskite against water ingress from ambient atmosphere and passivate its defect states to enhance the long-term stability while maintaining high PCE, and Yang teaches using multiple additives would provide synergetic passivation and increased efficiency. In such modification, the additive comprises two of D4TBP and Ga(AcAc)3.
Claim(s) 17-18 are rejected under 35 U.S.C. 103 as being unpatentable over modified Snaith et al. (WO 2020/109787) as applied to claim 12 above, and further in view of Du et al. (“Polymer Surface Modification of NiOx-Based Inverted Planar Perovskite Solar Cells with Enhanced Performance”).
Regarding claims 17-18, modified Snaith et al. disclose a method as in claim 12 above, wherein Snaith et al. teaches using two or more hole transport materials such as nickel oxide (NiOx) and PTAA are among others (see fig. 1a and pages 28-29).
Modified Snaith et al. does not explicitly disclose the first charge transport layer is a bilayer comprising a first sublayer and a second sublayer, wherein the second sublayer is adjacent to and in direct contact with both the absorber layer and the first sublayer as claimed in claim 17; nor do they teach the first charge transport layer is a bilayer comprising a first sublayer and a second sublayer; the first sublayer comprises nickel oxide; the second sublayer comprises PTAA; and depositing the first charge transport layer comprises: forming a layer of nickel oxide over the first contact and forming a layer of PTAA over the layer of nickel oxide as claimed in claim 18.
Du et al. disclose a transport layer comprises a first sublayer (NiOx) and a second sublayer (PTAA) such that the second sublayer (PTAA) is adjacent to and in direct contact with both the absorber layer (PVK) and the first sublayer (NiOx, see NiOx/PTAA/PVK shown in fig. 1f, and described throughout the document, also see the Experimental section in page 16807) such that the nickel oxide layer is deposited on the first contact (or FTO-coated glass substrate) and the PTAA layer is deposited over the layer of nickel oxide (NiOx, see Experimental section in page 16807)
It would have been obvious to one skilled in the art before the effective filing date of the claimed invention to modify the method of modified Snaith et al. by forming the transport layer of bilayer of NiOx and PTAA, or adding PTAA layer on top of the NiOx layer of Li et al., as taught by Du et al.; because Du et al. teaches the bilayer of NiOx/PTAA would enhance the performance of the device (see abstract, figs. 5-6, table 1 and conclusion)b and Snaith et al. teaches using two or more hole transport materials such as NiOx and PTAA.
Claim(s) 20-21 rejected under 35 U.S.C. 103 as being unpatentable over Snaith et al. (WO 2020/109787) in view of Yang et al. (“Tailoring Passivation Molecular Structures for Extremely Small Open-Circuit Voltage Loss in Perovskite Solar Cells”), and further in view of Du et al. (“Polymer Surface Modification of NiOx-Based Inverted Planar Perovskite Solar Cells with Enhanced Performance”).
Regarding claim 20, Snaith et al. discloses method of making a photovoltaic device (see pages 78-79, claims 32-50 and also see pages 54-77) comprising:
depositing a first charge transport layer (NiO) over a first contact layer (FTO-coated glass, see page 78);
applying a precursor solution (or perovskite precursor solution) to a surface of a first charge transport layer (NiO) resulting in a liquid layer of the precursor solution on the surface of the first charge transport layer (see page 79), wherein the precursor solution comprises a perovskite precursor comprising formamidinium iodide (FAI), cesium iodide (CsI), lead bromide (PbBr2), and lead iodide (PbI2), an additive (or ionic liquid such as BMIMBF4), and a solvent (DMF/DMSO, see paragraph bridging pages 78 and 79);
treating the liquid layer to remove at least a portion of the solvent (see annealing step on pre-heated hot plate described in page 79; also see page 63), thereby forming an absorber layer comprising a solid perovskite material (or crystalline A/M/X, see the entire document of Snaith et al., and more specifically claims 320), and crystalline perovskite material is solid.
Snaith et al. teaches using the precursor to form a perovskite material of (FA0.83MA0.17)0.95Cs0.05Pb(I0.9Br0.1)3 in the example described in the paragraph bridging pages 78 and 79). Snaith et al. also teaches using perovskite having formula (ID, see page 42) and more specifically [(CH3NH3)x(H2N-C(H)=NH2)1-x]Pb[BryI1-y]3 – or MAxFA1-xPb(BryI1-y)3 with x and y are both greater than 0 and less than 1 or 0.01-0.99 or 0.05-0.95 (see page 43).
Snaith et al. does not explicitly discloses the perovskite having a composition Cs(1-x-y)MAxFAyPb(I(1-z)Brz)3 with 0.02≤ x ≤0.08, 0.82≤ y ≤0.92, and 0.07≤ z ≤0.09.
However, it would have been obvious to one of ordinary skill in the art at the time of invention to used perovskite having formula MAxFA1-xPb(BryI1-y)3 with x and y are both greater than 0 and less than 1 or 0.01-0.99 or 0.05-0.95 for the method in the example, because Snaith et al. explicitly suggests doing so. In addition, it would have been obvious to one skilled in the art to have selected the overlapping portion of 0.08 in the ranges of greater than 0 and less than 1, 0.01-0.99 or 0.05-0.95 for x (or amount of MA) and 0.07-0.09 in the ranges greater than 0 and less than 1, 0.01-0.99 or 0.05-0.95 for y (or amount of Br) in the perovskite MAxFA1-xPb(BryI1-y)3 disclosed by Snaith et al., because selection of overlapping portion of ranges has been held to be a prima facie case of obviousness. In re Malagari, 182 USPQ 549. In such modification, the perovskite MAxFA1-xPb(BryI1-y)3 of Snaith et al. is MA0.08FA0.92Pb(BrzI1-z)3 with 0.07≤ z (or y of Snaith et al.) ≤0.09 that is read on the claimed perovskite having formula Cs(1-x-y)MAxFAyPb(I(1-z)Brz)3 with x =0.08, y=0.92, and 0.07≤ z ≤0.09.
Snaith et al. discloses using BMIMBF4 in the example. Snaith et al. does not teaches using additives comprising at least one of TAH or D4TBP.
Yang et al. discloses using passivation molecules such as D4TBP in the perovskite precursor for perovskite grain boundary passivation to achieve higher efficiency (see table S2 and paragraph bridging pages 5785 and 5786).
It would have been obvious to one skilled in the art before the effective filing date of the claimed invention to modify the method of Snaith et al. by using an additive comprising D4TBP as taught by Yang, because Yang et al. teaches using D4TBP would provide higher efficiency.
Snaith et al. teaches including one or more additional of charge transport layer between the electrode and charge transport layer (see page 33).
Snaith et al. does not explicitly disclose the first charge transport layer is a bilayer comprising a first sublayer and a second sublayer, wherein the first sublayer comprises an inorganic hole transport material, the second sublayer comprises an organic hole transport material, the second sublayer is position between the absorber layer and the first layer and the second sublayer is adjacent to and in direct contact with both the absorber layer and the first sublayer.
Du et al. disclose a transport layer comprises a first sublayer of inorganic hole transport layer (NiOx) and a second sublayer of organic hole transport layer (PTAA) such that the second sublayer (PTAA) is adjacent to and in direct contact with both the absorber layer (PVK) and the first sublayer (NiOx, see NiOx/PTAA/PVK shown in fig. 1f, and described throughout the document, also see the Experimental section in page 16807).
It would have been obvious to one skilled in the art before the effective filing date of the claimed invention to modify the method of Snaith et al. by forming the transport layer comprising a first sublayer of inorganic hole transport material of NiOx and the second sublayer of organic hole transport material of PTAA as taught by Du et al., because Snaith et al. explicitly suggest adding additional charge transport layer, and Du et al. teaches the bilayer of NiOx/PTAA would enhance the performance of the device (see abstract, figs. 5-6, table 1 and conclusion).
Regarding claim 21, modified Snaith et al. discloses a method as in claim 20 above, wherein the first sublayer is of nickel oxide (or NiOx) and the second sublayer is of PTAA (see claim 20 above). Snaith et al. discloses a charge transport layer having a thickness from 1 to 500nm, for instant from 5 to 250nm or from 10 to 75nm (see 4th paragraph of page 26 of Snaith et al.), wherein the range 10-75nm is right within the claimed range of 1.5nm to 100.0nm for the charge transport layer of NiO. Du et al. teaches the PTAA is very thin (see Experimental section of Du et al.).
Modified Snaith et al. does not explicitly disclose the second sublayer of charge transport layer of PTAA having a thickness in a range from 0.2 nm to 15.0 nm.
However, it would have been obvious to one of ordinary skill in the art at the time of invention to have selected the overlapping portions of 1-15nm in the range 1-500nm disclosed by Snaith et al., or 5-15nm in the range 5-250nm disclosed by Snaith et al., or 10-15nm in the range 10-75nm disclosed by Snaith et al., because Du et al. explicitly teaches the PTAA is very thin and selection of overlapping portion of ranges has been held to be a prima facie case of obviousness. In re Malagari, 182 USPQ 549.
Claim(s) 22, 27 and 28 are rejected under 35 U.S.C. 103 as being unpatentable over modified Snaith et al. as applied to claim 12 above, in view of Degani et al. (“23.7% Efficient inverted perovskite solar cells by dual interfacial modification).
Regarding claims 22 and 27-28, modified Snaith et al. discloses a method as in claim 12 above, wherein the additive comprising D4TBP (see claim 12 above). Yang et al. teaches using PEA and combining additives to achieve synergetic passivation to improve efficiency (see table S2 and paragraph bridging pages 5782-5783).
Modified Snaith et al. does not disclose the additive comprises PEAI as claimed in claim 27, nor do they teach the additive comprises at least two of TAH, CC, Ga(AcAc)3, Pb(SCN)2, OAM, PbCl2, D4TBP, PEAI, or 4F-PEAI as claimed in claim 28 such that the additive is present in the absorber layer with a concentration gradient as claimed in claim 22.
Degani et al. discloses adding PEAI such as PEAI or 4F-PEAI in addition to an ionic liquid ([BMP]+[BF4]-) (see fig. 1B and “perovskite film preparation and device fabrication”) to improve both open-circuit voltage and fill factor thereby improving the device efficiency (see abstract, table 1).
It would have been obvious to one skilled in the art before the effective filing date of the claimed invention to modify the method of modified Snaith et al. by further incorporating PEAI or 4F-PEAI as taught by Degani et al. in addition to D4TBP so that the additive comprises two of D4TBP and 4F-PEAI; because Degani et al. teaches such adding additive such as PEAI or 4F-PEAI would improve the efficiency and Yang et al. teaches combining additives to achieve synergetic passivation to improve the efficiency.
Response to Arguments
Applicant’s arguments with respect to claim(s) 12-22 and 27-30 have been considered but are moot because the new ground of rejection does not rely on any reference applied in the prior rejection of record for any teaching or matter specifically challenged in the argument.
Applicant argues previous cited references do not teach the claimed method. However, Applicant’s arguments are moot in view of the new ground of rejection. See the rejection above.
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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THANH-TRUC TRINH
Primary Examiner
Art Unit 1726
/THANH TRUC TRINH/Primary Examiner, Art Unit 1726
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