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 .
Response to Amendments
This is a final office action in response to applicant's arguments and remarks filed on 10/21//2025.
Status of Rejections
The objections to the drawings, abstract and specification are withdrawn in view of applicant’s amendments.
The rejection(s) of claim(s) 12, 18 and 59 is/are obviated by applicant’s cancellation.
The rejection of claim(s) 20 under 35 USC 112(a) is/are withdrawn in view of applicant’s amendment.
All other previous rejections are withdrawn in view of applicant’s amendments.
New grounds of rejection are necessitated by applicant’s amendments.
Claims 1-2, 5-7, 13-15, 19-20, 24, 26, 39, 45, 51, 55, 58 and 60 are pending and under consideration for this Office Action.
Claim Objections
Claim 60 is objected to because of the following informalities:
In claim 60, line 2, “film is selected” should read “film .
Appropriate correction is required.
Claim Rejections - 35 USC § 102
The text of those sections of Title 35, U.S. Code not included in this action can be found in a prior Office action.
Claims 1-2, 6, 13-15, 19, 26, 39, 45, 51, 55 and 60 are rejected under 35 U.S.C. 102(a)(1) as being anticipated by Lim et al. (“Improvement of fuel cell catalyst performance through zirconia protective layer coating by atomic layer deposition” and Supporting Information; J. Power Sources, 2021); claim 6 evidenced by Averill et al. (“7.2 Sizes of Atoms and Ions” in Principles of General Chemistry v.1.0, 2012), and claims 26 and 60 evidenced by Sigracet (“Powering up fuel cells—Our gas diffusion layer[White Paper]”, FuelCellStore).
Regarding claim 1, Lim discloses a membrane-embedded gas diffusion electrode (ME-GDE) (see e.g. Fig. S1 and Page 2, connecting paragraph of Cols. 1-2, lines 2-4 and 8-12, gas diffusion electrode of MEA covered with porous protective layer, i.e. embedding membrane), comprising:
an electronically conductive support material, wherein the support material is a continuous porous film (see e.g. Fig. S1, porous gas diffusion layer substrate; Page 2, Col. 2, under “2.1”, lines 5-7);
a catalytic phase (see e.g. Fig. S1, Pt/C catalyst; Page 2, Col. 2, under “2.1”, lines 1-2);
a membrane phase, wherein the membrane phase is a selective barrier (see e.g. Fig. S1b and 1-2, porous ZrO2 protective layer that is at least size-selective based on the size of the pores; Page 2, connecting paragraph of Cols. 1-2, lines 2-4 and 8-12); and
an ion conducting phase (see e.g. Fig. S1, ionomer; Page 2, Col. 2, under “2.1”, lines 1-3);
wherein the catalytic phase is dispersed in the ion-conducting phase (see e.g. Fig. S1, Pt/C shown dispersed in ionomer),
wherein the ion-conducting phase is in contact with the electronically conductive support material (see e.g. Fig. S1, slurry including ionomer coated on and in contact with GDL; Page 2, Col. 2, under “2.1”, lines 6-7), and
wherein the membrane phase forms a semi-continuous layer on the electronically conductive support material (see e.g. Fig. S1b and 2, porous, i.e. semi-continuous, ZrO2 layer provided on catalyst coated GDL; Page 2, connecting paragraph of Cols. 1-2, lines 2-4 and 8-12, and Col. 2, bottom paragraph, lines 1-3).
Regarding claim 2, Lim discloses the membrane phase comprising ZrO2 (see e.g. Page 2, Col. 2, lines 5-7).
Regarding claim 6, Lim discloses the membrane phase being permeable to H+ (see e.g. Page 3, Col. 2, line 19-Page 4, Col. 1, line 2, hydrogen/hydrogen ions able to diffuse to/from the Pt catalyst surface), and the membrane phase being impermeable to at least S2-, F-, Cl-, Br-, and I- (see e.g. Page 6, Col. 2, lines 2-4, protective layer preventing dissolution of Pt ions; and would therefore block the other mentioned ionic species which are larger in size than Pt cations, as evidenced by Averill, see e.g. Averill Fig. 7.9).
Regarding claim 13, Lim discloses the membrane phase covering part of the catalytic phase (see e.g. Figs. S1 and 1-2, Pt/C covered with zirconia coating).
Regarding claim 14, Lim discloses the membrane phase encapsulating the catalytic phase (see e.g. Figs. S1 and 2, Pt/C catalyst encapsulated with zirconia; Page 2, Col. 2, lines 6-8).
Regarding claim 15, Lim discloses the membrane phase being in direct contact with the ion-conducting phase (see e.g. Fig. S1b, ZrO2 coating in contact with ionomer of catalyst layer).
Regarding claim 19, Lim discloses the membrane phase partially encapsulating the electronically conductive support material (see e.g. Fig. S1b and 2, porous ZrO2 layer formed over, i.e. partially encapsulating, catalyst coated GDL; Page 2, connecting paragraph of Cols. 1-2, lines 2-4 and 8-12, and Col. 2, bottom paragraph, lines 1-3).
Regarding claim 26, Lim discloses the support material comprising nanostructured carbon (see e.g. Page 2, Col. 2, under “2.1”, lines 6-7, Sigracet 39BB GDL; which is evidenced by Sigracet to have a microporous layer including nanostructured carbon, see e.g. Sigracet Pages 3-5).
Regarding claim 39, Lim discloses the catalytic phase comprising Pt (see e.g. Fig. S1, Pt/C catalyst; Page 2, Col. 2, under “2.1”, lines 1-2).
Regarding claim 45, Lim discloses the catalytic phase being adsorbed directly to the support material (see e.g. Fig. S1, Pt/C catalyst adsorbed onto GDL; Page 2, Col. 2, under “2.1”, lines 1-7).
Regarding claim 51, Lim discloses the membrane phase comprising a thickness of about 3.5 nm (see e.g. Fig. 2e and Page 6, Col. 2, under “Conclusions”, lines 1-4, 35 cycles of ALD zirconia coating at ~0.1 nm/cycle).
Regarding claim 55, the limitation of “the thickness of the membrane phase [being] tuned to suppress one or more competing reactions selected from the group consisting of methane oxidation reaction, methanol oxidation reaction (MOR), ethanol oxidation reaction (EOR), hydrogen oxidation reaction (HOR), hydrogen evolution reaction (HER), chlorine evolution reaction (CER), oxygen evolution reaction (OER), and oxygen reduction reaction (ORR)” is a statement of intended use. MPEP § 2114 states “"[A]pparatus claims cover what a device is, not what a device does."…A claim containing a "recitation with respect to the manner in which a claimed apparatus is intended to be employed does not differentiate the claimed apparatus from a prior art apparatus" if the prior art apparatus teaches all the structural limitations of the claim.”. Lim discloses all the structural limitations of the claimed ME-GDE as stated above. Lim also discloses the membrane phase having a thickness of about 3.5 nm (see e.g. Fig. 2e and Page 6, Col. 2, under “Conclusions”, lines 1-4, 35 cycles of ALD zirconia coating at ~0.1 nm/cycle). Paragraph 0174 of the instant specification additionally teaches a membrane phase being tuned from 2 nm to 20 nm to assess the effect of membrane phase thickness on suppression of competing electrochemical reactions to CO2RR, suggesting that the 3.5 nm membrane phase of Lim within that range would have an effect on such suppression of competing electrochemical reactions.
Regarding claim 60, Lim discloses the electronically conductive support material being a continuous porous film of carbon paper and carbon fiber (see e.g. Page 2, Col. 2, under “2.1”, lines 6-7, Sigracet 39BB GDL; which is evidenced by Sigracet to have a carbon fiber paper backing layer, see e.g. Sigracet Pages 4-5).
Claim 58 is rejected under 35 U.S.C. 102(a)(1) as being anticipated by Kim et al. (“Improving the Stability of Polymer Electrolyte Membrane Fuel Cells via Atomic Layer-Deposited Cerium Oxide”, Int J Energy Research, Feb 2023).
Regarding claim 58, Kim discloses a membrane-embedded gas diffusion electrode (ME-GDE) (see e.g. Fig. 1, gas diffusion cathode encapsulated with CeOx, i.e. membrane-embedded; Page 3, Col. 1, lines 3-6), comprising:
an electrically conductive support material, wherein the support material is a continuous porous film (see e.g. Fig. 1, carbon gas diffusion layer; Page 3, Col. 1, bottom paragraph, lines 1-2);
a catalytic phase (see e.g. Fig. 1, Pt catalyst; Page 3, Col. 1, lines 3-4); and
a membrane phase, wherein the membrane phase is a selective barrier (see e.g. Figs. 1 and 3, CeOx film coated on Pt, the CeOx preventing attack by H2O2 and Pt dissolution but allowing access of the H+ and O2 reactants to the catalyst for the cathode reaction; Page 2, Col. 2, line 6-Page 3, Col. 1, line 3, Page 4, Col. 2, bottom paragraph, lines 1-10, and Page 7, Col. 1, lines 5-6);
wherein the catalytic phase is in contact with the electronically conductive support material (see e.g. Fig. 1, Pt sputtered on GDL), and
wherein the membrane phase forms a semi-continuous layer on the electronically conductive support material (see e.g. Fig. 1, CeOx layer deposited over porous catalyst coated GDL; Page 3, Col. 1, lines 3-5, and Col. 2, lines 12-13).
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 5 is rejected under 35 U.S.C. 103 as being unpatentable over Lim in view of Choun et al. (“Polydimethylsiloxane treated cathode catalyst layer to prolong hydrogen fuel cell lifetime”, Catalysis Today, 2016).
Regarding claim 5, Lim teaches all the elements of the ME-GDE of claim 1 as stated above. Lim further teaches the membrane phase comprising a first layer comprising ZrO2 (see e.g. Page 2, Col. 2, lines 5-7).
Lim does not teach the membrane phase comprising a second layer comprising one or more functionalized organic polymers selected from the group consisting of poly-dimethyl-siloxane (PDMS), organo-siloxane composites, sodium dodecyl sulfate (SDS), poly-tetrafluoroethylene, tetra-ethoxy silane (TEOS), cellulose acetates, polyamides, polyimides, and polysulfones. Lim does however teach the electrode comprising a gas diffusion layer and being used as a cathode in a fuel cell (see e.g. Fig. S1, Abstract and Page 2, Col. 2, lines 3-5)
Choun teaches a cathode for fuel cells (see e.g. Abstracts), wherein a layer of PDMS is coated on and in the cathode catalyst layer and GDL (see e.g. Scheme 1, Page 157, Col. 2, lines 5-7, and Page 158, Col. 1, lines 8-12), the hydrophobic PDMS layer suppressing carbon corrosion of the carbon catalyst support and GDL of the cathode by providing effective water removal from the catalyst layer (see e.g. Page 160, Col. 1, lines 5-8, and Page 155, Col. 2, lines 1-7).
It would have been obvious to one of ordinary skill in the art before the effective filing date of the claimed invention to have modified the electrode of Lim to further comprise a layer of hydrophobic PDMS on and in the catalyst layer and GDL as taught by Choun to suppress carbon corrosion of the carbon catalyst support and GDL by providing effective water removal from the catalyst layer.
Claim 7 is rejected under 35 U.S.C. 103 as being unpatentable over Lim in view of Takenaka et al. (“Catalytic Activity of Highly Durable Pt/CNT Catalysts Covered with Hydrophobic Silica Layers for the Oxygen Reduction Reaction in PEFCs”, J. Phys. Chem. C, 2014).
Regarding claim 7, Lim teaches all the elements of the ME-GDE of claim 1 as stated above. Lim further teaches the membrane phase being permeable to at least H2O (see e.g. Fig. S1, diffusion of H2O produced at cathode catalyst of PEMFC). Lim does not explicitly teach the membrane phase being impermeable to one or more molecules selected from the group consisting of NO, O2, C2-C6 alkanes, C1-C6 alkenes, and C1-C6 alkynes. Lim does however teach the membrane phase being a porous oxide protective layer for the cathode catalyst of a polymer electrolyte membrane fuel cell (see e.g. Abstract and Page 2, connecting paragraph of Cols. 1-2, lines 2-4 and 8-12).
Takenaka teaches a catalyst for the cathode in a polymer electrolyte fuel cell covered with silica (SiO2) layers to improve catalyst durability (see e.g. Abstract), wherein the silica layers have a porous structure that acts as a barrier to C1-C3 alcohols (see e.g. Page 777, Col. 1, lines 9-11, and Col. 2, lines 15-17), and would therefore similarly block larger hydrocarbons such as C4-C6 alkanes, alkenes and alkynes, this porous structure with large pore diameters however not inhibiting the diffusion of molecular oxygen to the Pt catalyst surface and thus enabling high ORR activity (see e.g. Page 781, Col. 2, lines 3-5 and 10-16).
It would have been obvious to one of ordinary skill in the art before the effective filing date of the claimed invention to have modified the membrane phase of Lim to have large pore diameters that do not inhibit diffusion of molecular oxygen even while blocking larger alcohols hydrocarbons such as C4-C6 alkanes, alkenes and alkynes as taught by Takenaka as a suitable porous structure for an oxide protective layer on the cathode catalyst of a polymer electrolyte membrane fuel cell. MPEP § 2143(I)(A) states that “combining prior art elements according to known methods to yield predictable results” may be obvious. The claimed elements were known in the prior art and one skilled in the art could have combined the elements as claimed by known methods with no change in their respective functions, and the combination would yield nothing more than predictable results.
Claims 20 and 24 are rejected under 35 U.S.C. 103 as being unpatentable over Lim in view of Poojary et al. (“Transport and Electrochemical Interface Properties of Ionomers in Low-Pt Loading Catalyst Layers: Effect of Ionomer Equivalent Weight and Relative Humidity”, Molecules, 2020).
Regarding claim 20, Lim teaches all the elements of the ME-GDE of claim 1 as stated above. Lim does not explicitly teach the ion-conducting phase being selective for the transport of one or more cations or one or more anions. Lim does however teach the electrode being a cathode of a polymer electrolyte membrane fuel cell (see e.g. Abstract).
Poojary teaches catalyst layer ionomers for polymer electrolyte fuel cells (see e.g. Abstract and Page 1, line 1) which must ensure proton transport, i.e. be proton selective, to achieve high in-operando electrochemical surface area utilization (see e.g. Page 1, lines 8-10, and Page 2, lines 1-2).
It would have been obvious to one of ordinary skill in the art before the effective filing date of the claimed invention to have modified the ion-conducting phase of Lim to be selective for the transport of protons, i.e. cations, as taught by Poojary to achieve high in-operando electrochemical surface area utilization.
Regarding claim 24, Lim teaches all the elements of the ME-GDE of claim 1 as stated above. Lim further teaches the ion-conducting phase comprising an ionomer (see e.g. Fig. S1, ionomer; Page 2, Col. 2, under “2.1”, lines 1-3). Lim does not explicitly teach the ionomer being selected from the group consisting of sulfonated fluorocarbon polymers, sulfonated poly(ether ether ketone), sulfonated polystyrene, imidazolium-functionalized styrene, imidazolium-functionalized vinyl-benzene chloride, and phosphoric acid-doped polybenzimidazole.
Poojary teaches catalyst layer ionomers for polymer electrolyte fuel cells (see e.g. Abstract), which comprise the sulfonated fluorocarbon polymers Nafion or Aquivion (see e.g. Scheme 1).
It would have been obvious to one of ordinary skill in the art before the effective filing date of the claimed invention to have modified the ionomer of Lim to comprise the sulfonated fluorocarbon polymers Nafion or Aquivion as taught by Poojary as a suitable particular catalyst layer ionomer for use in a polymer electrolyte fuel cell. MPEP § 2143(I)(A) states that “combining prior art elements according to known methods to yield predictable results” may be obvious. The claimed elements were known in the prior art and one skilled in the art could have combined the elements as claimed by known methods with no change in their respective functions, and the combination would yield nothing more than predictable results. Further, MPEP § 2144.07 states “The selection of a known material based on its suitability for its intended use supported a prima facie obviousness determination in Sinclair & Carroll Co. v. Interchemical Corp., 325 U.S. 327, 65 USPQ 297 (1945)”.
Response to Arguments
Applicant’s arguments, see pages 11-15, filed 10/21/2025, with respect to the rejection(s) of claim(s) 1 under 35 USC 102 over Takenaka or Yoshimura, particularly regarding the support being a continuous porous film and the membrane phase being a selective barrier, have been fully considered and are persuasive. Therefore, the rejection has been withdrawn. However, upon further consideration, a new ground(s) of rejection is made in view of Lim.
Applicant’s arguments, see pages 11-14, filed 10/21/2025, with respect to the rejection(s) of claim(s) 58 under 35 USC 102 over Takenaka, particularly regarding the support being a continuous porous film, have been fully considered and are persuasive. Therefore, the rejection has been withdrawn. However, upon further consideration, a new ground(s) of rejection is made in view of Kim.
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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/M.S.J./Examiner, Art Unit 1795
/LUAN V VAN/Supervisory Patent Examiner, Art Unit 1795
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