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 .
Continued Examination Under 37 CFR 1.114
A request for continued examination under 37 CFR 1.114, including the fee set forth in 37 CFR 1.17(e), was filed in this application after final rejection. Since this application is eligible for continued examination under 37 CFR 1.114, and the fee set forth in 37 CFR 1.17(e) has been timely paid, the finality of the previous Office action has been withdrawn pursuant to 37 CFR 1.114. Applicant's submission filed on 17 Nov 2025 has been entered.
Response to Arguments
Applicant's arguments filed 17 Nov 2025 have been considered but are moot because the new ground of rejection now addresses the newly-amended claims, as set forth below.
Claim Interpretation
Regarding claim 1, the phrase “an amount of the substrate catalyst particles” and “an amount of the proton-conducting ionomer” are understood to refer to the quantity or number of substrate catalyst particles and proton-conducting ionomers, respectively.
Claim Rejections - 35 USC § 112
The rejection of claims 1-2 and 4-11 under 35 U.S.C. § 112(a) and 112(b) are withdrawn in view of the amended claims.
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.
Claim(s) 1, 4-7, and 11 are rejected under 35 U.S.C. 103 as being unpatentable over Sousa et al. (US 2019/0245215) in view of Kawamura et al. (JP 2018206626A, as read via machine translation) and Atanassova et al. (US 2008/0206616).
As to Claim 1, Sousa et al. discloses a method for producing a catalyst-coated membrane, comprising:
preparing and/or providing a first ink having a first ink composition (see e.g. first catalyst ink from reservoir 23a, [0027], [0079], and Fig. 2),
preparing and/or providing at least one second ink having a second ink composition (see e.g. catalyst ink from reservoir 23, [0027], [0079], and Fig. 2).
Sousa et al. does not disclose that the first ink comprises substrated catalyst particles, proton-conducting ionomer and dispersing agent, or that an amount of the substrated catalyst particles in the first ink is less than an amount
Kawamura et al., also working in the field of catalyst-coated membrane production, teaches a two-layer catalyst-coated cathode membrane in which the first and second layers comprise substrated catalyst particles, proton-conducting ionomer and dispersing agent (see e.g. second cathode layer 1 and first cathode layer 2, which comprise catalyst particles 10, ionomer 12, and a dispersant, Kawamura et al.: [0016]-[0017], [0019], and Fig. 2).
Kawamura et al. further teaches that the ratio of the amount of the proton-conducting ionomer to the amount of substrated catalyst particles in the proton-conducting ionomer in the first ink (i.e., in cathode layer 2) is preferably in the range of 0.8 to 1.9, and that the ratio of the amount of the proton-conducting ionomer to the amount of substrated catalyst particles in the proton-conducting ionomer in the second ink (i.e., in cathode layer 1) is preferably in the range of 0.6 to 1.5 (see e.g., Kawamura et al.: [0015]-[0014]). In other words, Kawamura et al. teaches a range of ionomer/catalyst values for the first and second layers that encompasses an embodiment in which an amount of the substrated catalyst particles in the first ink is less than an amount2 is from 1 to 1.9) and in which an amount of the substrated catalyst particles in the second ink is less than an amount1 is from 0.6 to 1).
It has been held that a prima facie case of obviousness exists when a prior art reference discloses a range encompassing a somewhat narrower claimed range (see MPEP § 2144.05, “Obviousness of Similar and Overlapping Ranges, Amounts, and Proportions”). Still further, Kawamura et al. additionally teaches that when the ionomer concentration in the first catalyst layer is greater than the ionomer concentration of the second catalyst layer, movement of the ionomer toward the substrate via diffusion can be suppressed (see e.g., Kawamura et al.: [0013]).
It would therefore have been obvious to one of ordinary skill in the art prior to the filing date of the claimed invention to modify Sousa et al.’s process in the manner taught by Kawamura et al. such that the first ink of Sousa et al. contains substrated catalyst particles, proton-conducting ionomer and a dispersing agent, in which the volume fraction of the substrated catalyst particles remains behind the volume fraction of the proton-conducting ionomer; and in which the second ink of Sousa et al. comprises substrated catalyst particles, the proton-conducting ionomer and the dispersing agent, in which the volume fraction of the proton-conducting ionomer remains behind the volume fraction of the substrated catalyst particles, as taught by Kawamura et al.. Said artisan would have been motivated to modify Sousa et al.’s process in this manner in order to realize the benefits taught by Kawamura et al.: specifically, the suppression of ionomer diffusion toward the substrate.
Further regarding claim 1, Sousa et al. discloses unwinding a weblike proton-conducting membrane material provided on a roll (see e.g. membrane, which may be referred to as a web, and is provided on feed spool roll 7, [0045] and Fig. 1);
applying at least one layer of the first ink with a first application tool onto at least one section of the weblike proton-conducting membrane material (ink from reservoir 23a is applied to the membrane via sprayer 21a, which reads on the claimed first application tool, [0056], [0079], and Fig. 2);
taking of the weblike proton-conducting membrane material, which is at least partially coated with the first ink, to an intermediate drying unit (see e.g. heating zone 27a, which dries the catalyst ink from reservoir 23a, [0058], [0079] and Fig. 2).
Sousa et al. in view of Kawamura et al. as applied above does not disclose the step of only partially drying the first ink via the intermediate drying unit to form a dry marginal film of the first ink at an outer marginal portion of the first ink facing away from the weblike proton-conducting membrane material before the second ink is applied while the remaining portion of the first ink remains wet.
Atanassova et al., also working on the problem of catalyst-coated membrane manufacture, teaches that, when multiple catalyst inks are sprayed on top of one another (which is analogous to the process disclosed by Sousa et al.), only partially drying the first ink of a catalyst ink between consecutive ink deposition steps such that the first ink is at least partially wet results in a gradient in composition rather than a sharp concentration change at the interface between the two ink layers (see e.g. Atanassova et al., [0179]-[0180] and Fig. 12). Atanassova et al. further teaches that the formation of a concentration gradient improves the methanol diffusivity of the membrane without sacrificing the electrical conductivity of the catalyst membrane (see e.g. Atanassova et al., [0162]).
It would therefore have been obvious to one of ordinary skill in the art prior to the filing date of the claimed invention to modify the process of Sousa et al. by only partially drying the first ink via the intermediate drying unit to form a dry marginal film of the first ink at an outer marginal portion of the first ink facing away from the weblike proton-conducting membrane material before the second ink is applied while the remaining portion of the first ink remains wet, in the manner taught by Atanassova et al.. Said artisan would have been motivated to modify Atanassova et al.’s process in this manner in order to produce a membrane with a concentration gradient that improves the methanol diffusivity of the membrane without sacrificing electrical conductivity, as taught by Atanassova et al..
Further regarding claim 1, Sousa et al. in view of Kawamura et al. and Atanassova et al. as applied above discloses applying at least one layer of the second ink with a second application tool onto an outermost side of the dry marginal film of the first ink21, which reads on the second application tool and deposits a second ink from reservoir 23 onto the top surface of the membrane, such that the second ink is applied to an outermost side of the dry marginal film of the first ink
and taking of the weblike proton-conducting membrane material, which is at least partially coated with the first ink and the second ink to another drying unit (see e.g. heating zone 27, Sousa et al. [0079] and Fig. 2), and fully drying the first ink along with fully drying the second ink such that no portion of the first ink and no portion of the second ink remains wet (i.e., after heating in heating zone 27 the membrane is cured to yield a dimensionally stable catalyst coated membrane, implying that the inks are fully dry, Sousa et al. [0036]-[0037]).
As to Claim 4, Sousa et al. discloses the method according to claim 1, wherein a layer thickness measurement is performed for the layer of the first ink after the depositing of the first ink (see e.g. gauges 31a and 31, which measure the thickness of the membrane before and after coating, [0065] and Fig. 2).
As to Claim 5, Sousa et al. discloses the method according to claim 4, wherein the first ink is applied to subsequent sections of the membrane material in dependence on the measured layer thickness of preceding sections of the membrane material (see e.g. the closed-loop control using a PLC, in which thickness data determined from sensors, is used to adjust the ink flow rate to the spray nozzles. [0039], [0065]-[0066], [0079], and Fig. 2).
As to Claim 6, Sousa et al. discloses the method according to claim 4, wherein the second ink is deposited in dependence on the measured layer thickness of the first ink in order to limit an electrode thickness (see e.g. the closed-loop control using a PLC, in which thickness data determined from sensors, is used to adjust the ink flow rate to the spray nozzles. [0039], [0065]-[0066], [0079], and Fig. 2).
As to Claim 7, Sousa et al. discloses the method according to claim 1, wherein a layer thickness measurement of the electrode thickness is performed after applying the second ink (see e.g. sensors 31 and 81a, which are placed before and after the second sprayer 21, to perform a thickness measurement after the second sprayer 21 applies the second ink [0065]-[0066] and Fig. 2), and the second ink is deposited on subsequent sections of the membrane material in dependence on a measured electrode thickness (see e.g. the measured coat thickness, which is determined from sensors, is used to adjust the ink flow rate to the spray nozzles via a programmable logic controller ([0039], [0065]-[0066]).
As to Claim 11, Sousa et al. discloses the method according to claim 1, wherein a catalyst content is determined by a layer thickness measurement and/or by a charge measurement (see e.g. beta sensors, which measure the layer thickness of the catalyst coating and thereby determine the catalyst content).
Claim 2 is rejected under 35 U.S.C. 103 as being unpatentable over Sousa et al. (US 2019/0245215) in view of Kawamura et al. (JP 2018206626A, as read via machine translation) and Atanassova et al. (US 2008/0206616) as applied to claim 1 above, and further in view of Lee et al. (KR 20200002144A, as read via machine translation).
As to Claim 2, Sousa et al. discloses the method according to claim 1, wherein the first ink is applied with the first application tool on a first side of the weblike proton-conducting membrane material (see e.g. sprayer 21a, which applies a first ink from reservoir 23a, [0079] and Fig. 2), and subsequently in time the second ink is applied with the second application tool on the first ink deposited on the first side of the weblike proton-conducting membrane material (see e.g. sprayer 21, which applies a first ink from reservoir 23, [0079] and Fig. 2).
Sousa et al. does not disclose a method in which the first ink is applied with the first application tool on both of first and second sides of the weblike proton- conducting membrane material, or in which the second ink is applied with the second application tool on the first ink deposited on the second side of the weblike proton-conducting membrane material.
Lee et al., also working in the field of catalyst-coated membrane production, teaches a process in which a slot die is used to apply a catalyst layer to both sides of a membrane simultaneously (see e.g. Lee et al.: [0130]). Lee et al. teaches that slot die coating is an alternative to spray coating, and that one or both sides of the membrane may be coated (see e.g. Lee et al.: [0054]).
It would therefore have been obvious to one of ordinary skill in the art prior to the filing date of the claimed invention to replace the spray applicators of Sousa et al. with the slot die coating applicators taught by Lee et al., such that both sides of the membrane are simultaneously coated by the coating applicators such that the slot die application tool applies the first catalyst ink to both the first ink deposited on the first side of the weblike proton-conducting membrane and on the first ink deposited on the second side of the weblike proton-conducting membrane material.
Said artisan would have been motivated to make such a modification in order to increase the amount of catalyst per square area of membrane, and thereby improve the performance of the catalyst-coated membrane.
Claims 9 is rejected under 35 U.S.C. 103 as being unpatentable over Sousa et al. (US 2019/0245215) in view of Kawamura et al. (JP 2018206626A, as read via machine translation) and Atanassova et al. (US 2008/0206616) as applied to claim 1 above, and further in view of Vlajnic et al. (US 2004/0086632).
As to Claim 9, Sousa et al. discloses the method according to claim 1, wherein an amount of catalyst of the weblike proton-conducting membrane material coated with the first and second inks is determined (see e.g. PLC, which determined the amount of catalyst via beta sensors, [0039]), and the flow rate of the catalyst particles in the first and second inks is adjusted as a function of a measured catalyst amount (see e.g. PLC, which measures the amount of catalyst and regulates the flow rate of the sprayer, [0039]).
Sousa et al.’s method differs from the instantly-claimed invention in that in Sousa et al., the sensors are beta gauges, and Sousa et al. does not disclose the use of X-ray fluorescence (XRF) analysis. Further, Sousa et al.’s method works by altering the flow rate of the sprayers rather than by adjusting of the fraction of substrated catalyst particles.
Vlajnic et al., also working in the field of catalyst-coated membrane production, teaches the use of XRF analysis as a tool to measure the amount of catalyst in a catalyst coating (see e.g. the catalyst loading, Vlajnic et al.: [0029]-[0030]). Further, Vlajnic et al. teaches that XRF is a highly-precise, non-destructive tool for measuring the amount of catalyst (Vlajnic et al.: [0029]).
It would therefore have been obvious to one of ordinary skill in the art prior to the filing date of the claimed invention to replace the beta gauges of Sousa et al. with the XRF analysis taught by Vlajnic et al., and said artisan would have been motivated to replace the beta gauges with XRF because Vlajnic et al. teaches that XRF measurements are a highly-precise and non-destructive way of performing the same function of measuring catalyst content.
Further regarding claim 9, Vlajnic et al. also teaches that the fraction of substrated particles can be modified by adjusting the composition of the catalyst ink (see e.g., the catalyst loading is modified by adjusting the catalyst concentration in bed reactor 34, Vlajnic et al.: [0029]-[0030])
It would therefore have been obvious to one of ordinary skill in the art to adjust the fraction of substrated particles in Sousa et al.’s method according to Vlajnic et al.’s teachings, rather than adjusting the flow rate of the sprayer. Said artisan would have recognized such a modification to be an art-recognized process that accomplishes the same function of adjusting the amount of catalyst applied to the membrane material.
Claim 10 is rejected under 35 U.S.C. 103 as being unpatentable over Sousa et al. (US 2019/0245215) in view of Kawamura et al. (JP 2018206626A, as read via machine translation) and Atanassova et al. (US 2008/0206616) as applied to claim 1 above, and further in view of Yoon et al. (KR 20080008855, as read via machine translation).
Regarding claim 10, Sousa et al. discloses the method according to claim 1, wherein the weblike proton-conducting membrane material is coated with the first and second inks (see e.g. first and second inks from reservoirs 23 and 23a, [0027], [0079] and Fig. 2).
Sousa et al. does not disclose a method in which the membrane, coated with catalyst first and second inks, is cut up into individual catalyst-coated membranes.
Yoon et al., also working in the field of catalyst-coated membrane manufacturing, teaches a cutter (see e.g. cutter 600) that cuts the processed catalyst-coated membrane on a roll into individual coated membranes corresponding to the predetermined size of stack of a fuel cell system (see e.g. pg. 6, Yoon et al.: lines 278-282 and Fig. 1).
It would have been obvious to one of ordinary skill in the art prior to the filing date of the claimed invention to similarly provide the method of Sousa et al. with the cutter taught by Yoon et al. at the end of the processing line such that the membrane, coated with first and second catalyst inks, is cut up into individual catalyst membranes. Said artisan would have been motivated to install Yoon et al.’s cutter in order to automatically cut the membranes into a size that is compatible with a fuel cell system, as is taught by Yoon et al..
Conclusion
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/A.M.H./Examiner, Art Unit 1723
/TONG GUO/Supervisory Patent Examiner, Art Unit 1723