Detailed Action
This is a Non-Final Office action based on application 18/577,608 filed on 8 January 2024. The application is a 371 of PCT/ EP2022/ 068957 with priority to FR2107350 filed 7 July 2021
Claims 1-8 are pending and have been fully considered.
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 § 102
The following is a quotation of the appropriate paragraphs of 35 U.S.C. 102 that form the basis for the rejections under this section made in this Office action:
A person shall be entitled to a patent unless –
(a)(1) the claimed invention was patented, described in a printed publication, or in public use, on sale, or otherwise available to the public before the effective filing date of the claimed invention.
(a)(2) the claimed invention was described in a patent issued under section 151, or in an application for patent published or deemed published under section 122(b), in which the patent or application, as the case may be, names another inventor and was effectively filed before the effective filing date of the claimed invention.
Claims 1-3 and 5-7 are rejected under 35 U.S.C. 102(a)(1) as being anticipated by Huang (US 2008/0190781 A1).
Regarding claim 1, Huang teaches a method for generating hydrogen by water electrolysis (abstract, “electrochemical method for producing and storing hydrogen”), wherein same uses an electrochemical device comprising only two electrodes (per para [0005]-[0006] the electrochemical device comprises a gas-generating electrode and a zinc electrode; in example 2 at para [0044] there are exactly two electrodes), namely
a positive electrode containing a bifunctional catalyst successively forming an oxygen evolution reaction electrode and a hydrogen evolution reaction (HER) electrode, according to whether the device is subjected to an electric charge or produces an electric charge (para [0005]-[0006], the “gas-generating electrode” alternatively generates hydrogen gas when discharged in closed circuit with the zinc electrode, or generates oxygen gas when charged at a positive potential against the zinc electrode; para [0044], “foamed nickel sheet is as the hydrogen-generating that is concurrently as the oxygen-generating electrode”), and
a negative electrode using a redox pair Mm+/M, wherein M represents a metal element in reduced form and M+ represents said metal element in oxidized form (the Zn(0) / Zn(II) electrode as disclosed at para [0005]-[0006], [0019], [0044]), the electrodes being immersed in an aqueous electrolyte (para [0020] the electrolyte is an aqueous solution; para [0044], in a particular example the electrode is aqueous 5 M NaOH), the method comprising:
- a step of electrolysis under biasing inducing, at the negative electrode, a reduction of the metal element in oxidized form Mm+ to a reduced metal element M in solid form, the metal exhibiting an H2 overvoltage, and inducing, at the positive electrode, the generation of oxygen O2 forming the OER electrode (para [0013]-[0017], [0045], [0050]);
- a step of conversion by spontaneous reaction, between the positive electrode generating hydrogen H2, forming the HER electrode, and the negative electrode, seat of the oxidation of the metal element in reduced form M into a metal element in oxidized form Mm+ (para [0008]-[0012], [0046], [0051]).
Regarding claim 2, Huang teaches the method according to claim 1, wherein the reduced metal element M in solid form forms a deposit on the negative electrode (para [0014]; para [0025], “When the hydrogen gas is to be stored, ... connect the negative pole to the external circuit of the zinc electrode, switch on the direct current, the zinc electrode begins to be reduced into zinc”).
Regarding claim 3, Huang teaches the method according to claim 1, wherein the step of conversion by spontaneous reaction generates an electrical voltage, giving rise to an effective electrical energy (para [0011], “ΔE0 = 0.421 V”).
Regarding claim 5, Huang teaches the method according to claim 1, wherein M represents Zn and Mm+ represents Zn2+ (para [0008]-[0017]) and the electrolyte is basic (para [0044], “5 Mol/L NaOH aqueous solution is as the electrolyte”).
Regarding claim 6, Huang teaches the method of claim 1 and also teaches a device for implementing such a method (para [0026], “The device ...”), comprising:
- at least one closed chamber intended to contain at least one aqueous electrolyte (para [0026], “a plurality of electrode chambers ... the electrolyte in the storage tank flowing into every electrode chamber”);
- at least one positive electrode capable of forming an OER electrode and an HER electrode intended to be immersed in the electrolyte (50) (para [0026], “the hydrogen-generating electrode that is concurrently as the oxygen-generating electrode”);
- at least one negative electrode forming a redox electrode intended to be immersed in the electrolyte (para [0026], “zinc electrode”);
- a power supply connected to the positive electrode and to the negative electrode (para [0026], “power source to the external circuit”);
- an electrical connection for managing the charge and discharge of the device, apt to successively produce the functioning the positive electrode as OER electrode and as HER electrode (para [0026], “the external circuit”; per para [0026], the external circuit is switched between a discharging state, in which the zinc is oxidized and the positive electrode evolves hydrogen, and a charging state, in which power is supplied to the cell, zinc oxides are reduced to metallic zinc, and the positive electrode evolves oxygen)
- at least one discharge pipe for the gaseous oxygen generated by the method, and independently, at least one discharge pipe for the gaseous hydrogen generated by the method (para [0026], “hydrogen gas is collected in the hydrogen collecting chamber and flows out through the hydrogen outlet ... oxygen discharges directly from the oxygen outlet”).
Regarding claim 7, Huang teaches the device according to claim 6, comprising only two electrodes (para [0026], the device comprises any number of electrochemical cells and each cell comprises exactly two electrodes; in Examples 2 and 3, para [0044]-[0052], the device comprises only one cell having only two electrodes).
Claims 1 and 2 are rejected under 35 U.S.C. 102(a)(1) as being anticipated by Klein (US 5,540,831 A).
Regarding claim 1, Klein teaches a method for generating hydrogen by water electrolysis (col 1 ln 10-12), wherein same uses an electrochemical device comprising only two electrodes (figure 1, a device comprising first electrode 3, second electrode 4, and no other electrodes), namely:
a positive electrode containing a bifunctional catalyst successively forming an oxygen evolution reaction electrode and a hydrogen evolution reaction (HER) electrode, according to whether the device is subjected to an electric charge or produces an electric charge (figure 1, gas electrode 2; col 2 ln 35-37, “the gas electrode comprises materials and or catalysts that exhibit stable low gas evolution voltages”; col 2 ln 50-60, “When the electrodes 2 and 3 are subjected to a charging potential at a preselected voltage, the water in the electrolyte 5 is dissociated to evolve oxygen at the cathode or gas electrode 2 ... When the electrodes are then subjected to a discharging potential (a potential in the opposite direction to the charging potential) hydrogen is evolved from the gas or cathode electrode 2”), and
a negative electrode (figure 1, battery electrode 3) using a redox pair Mm+/M, wherein M represents a metal element in reduced form and M+ represents said metal element in oxidized form, the electrodes being immersed in an aqueous electrolyte (col 3 table 1 lists several metal electrode materials which are deemed suitable, including zinc, iron, cadmium, and lead-acid; col 4 ln 25-35, when the battery electrode material is cadmium, the metal is cycled between Cd(0) and Cd2+ oxidation states; col 5 ln 6-13, when the battery electrode material is iron, the metal is cycled between Fe(0) and Fe2+), the method comprising:
- a step of electrolysis under biasing inducing, at the negative electrode, a reduction of the metal element in oxidized form Mm+ to a reduced metal element M in solid form, the metal exhibiting an H2 overvoltage, and inducing, at the positive electrode, the generation of oxygen O2 forming the OER electrode (col 2 ln 50-56, “When the electrodes 2 and 3 are subjected to a charging potential at a preselected voltage, the water in the electrolyte 5 is dissociated to evolve oxygen at the cathode or gas electrode 2. The evolved oxygen is then vented from the housing 4 via the port 6. The anode or battery electrode, in turn, is reduced”; in the example of col 4 ln 28-31, Cd(OH)2 is reduced to metallic Cd);
- a step of conversion by spontaneous reaction, between the positive electrode generating hydrogen H2, forming the HER electrode, and the negative electrode, seat of the oxidation of the metal element in reduced form M into a metal element in oxidized form Mm+ (col 2 ln 56-60, “When the electrodes are then subjected to a discharging potential (a potential in the opposite direction to the charging potential) hydrogen is evolved from the gas or cathode electrode 2 and the anode or battery electrode 3 is stripped of hydrogen or oxidized”; in the example of col 4 ln 32-35, Cd metal is oxidized to Cd(OH)2).
Regarding claim 2, Klein teaches the method according to claim 1, wherein the reduced metal element M in solid form forms a deposit on the negative electrode (col 4 ln 12-15, in Example 1, the cadmium hydroxide is reduced to cadmium metal at the negative electrode during charging; col 4 ln 61-64, in Example 2, iron hydroxide is reduced to metallic iron at the negative electrode during charging).
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 4 is rejected under 35 U.S.C. 103 as being unpatentable over Klein as applied to claim 1 above, and further in view of Griffin (US 2006/0180464 A1).
Regarding claim 4, Klein teaches the method of claim 1. Klein further teaches that one of several suitable materials for the negative electrode is a lead-acid electrode (pg 3 table 1), such that M would represent Pb and Mm+ would represent a compound of Pb. However, Klein does not teach wherein the electrolyte comprises H2SO4 such that the lead compound represented by Mm+ would be PbSO4.
Griffin is similarly directed to a method of hydrogen production (para [0015]-[0016], [0036]) using an electrochemical device comprises a catalytic gas evolving cathode (figure 1, electrode 104) and a redox active metal anode (figure 1 electrode 106) via a cycle comprising a first phase of electrochemically reducing a metal ion Mm+ to form the corresponding metal M with concomitant evolution of oxygen from the cathode, and a second phase of electrochemically oxidizing the metal M to the metal ion Mm+ with concomitant evolution of hydrogen gas at the cathode (para [0116], [0219]).
Griffin further teaches that several metals are suitable for use as the M / Mm+ redox couple, including zinc (in Examples 15-18, para [0214]-[0217]) and lead (in examples 19-21, para [0218]-[0220]), with lead being particularly suitable (para [0055], “When lead, for example, is employed as the colloidal metal ion in equations 30 and 31, the pair of reactions is found to take place quite readily”).
Griffin further teaches that electrolyte compositions suitable for use in the method include sodium hydroxide and sulfuric acid (para [0139], “reaction medium preferably comprises water and, most preferably, further comprises either a base or an acid, ... In basic media, the base is preferably sodium hydroxide ... In acidic media, the acid is preferably sulfuric acid or hydrochloric acid”), with sulfuric acid in being suitable for use in combination with a lead anode (see Examples 19-21, para [0218]-[0220]).
It would have been obvious to a person having ordinary skill in the art before the effective filing date of the claimed invention to modify the method of Klein by selecting the lead-acid electrode from among the five negative electrode materials disclosed in Klein (col 3 table 1). The court has held that if an anticipated success is attained by a person pursuing one of a finite number of known options within their technical grasp, the outcome likely reflects ordinary skill and common sense, rather than inventiveness (see KSR Int'l Co. v. Teleflex Inc., 550 U.S. at 421, 82 USPQ2d at 1397 (2007); also see MPEP 2143(E) and case law discussed therein).
Furthermore it would have been obvious to a person having ordinary skill in the art before the effective filing date of the claimed invention, when using a lead acid battery electrode in the method of Klein, to use it in combination with an electrolyte composition comprising sulfuric acid such that the lead metal electrode oxidizes to PbSO4, based on Griffin’s teaching, in the context of a similar hydrogen production method, that sulfuric acid is a suitable electrolyte to use when the negative electrode material is lead (para [0139], [0218]-[0220]). The simple substitution of one known element for another (i.e., one electrolyte material for another) is likely to be obvious when predictable results are achieved (i.e., effective production of hydrogen gas via oxidation and reduction of lead electrode in the recited electrolyte) [MPEP § 2143(B)]. The selection of a known material, which is based upon its suitability for the intended use, is within the ambit of one of ordinary skill in the art [MPEP § 2144.07].
Claim 8 is rejected under 35 U.S.C. 103 as being unpatentable over Huang as applied to claim 6 above, and further in view of Rothschild et al (US 2017/0306510 A1).
Regarding claim 8, Huang teaches the device according to claim 6, further comprising a device for storing the gaseous hydrogen generated by the method (para [0026], “hydrogen gas is collected in the hydrogen collecting chamber”). However, Huang does not disclose a second gas storage device for storing the oxygen generated by the method.
Rothschild is similarly directed to a system and method of generating hydrogen by water splitting (abstract) using an electrochemical device that comprises two electrodes (figure 5a-5b; figure 2), namely
a positive electrode containing a bifunctional catalyst successively forming an oxygen evolution reaction electrode and a hydrogen evolution reaction (HER) electrode, according to whether the device is subjected to an electric charge or produces an electric charge (figure 2, working electrode 118; in figure 5a-b this corresponds to the Pt electrode at the left of the cell, which is a HER cathode during charging (figure 5a) and a OER anode during discharging (figure 5b); para [0265]-[0266]), and
a negative electrode using a metal redox pair (figure 2, redox electrode 116; figure 5a-5b, the nickel hydroxide electrode at the right of the cell, which is an anode during charging and a cathode during discharging; para [0259]), the electrodes being immersed in an aqueous electrolyte (figure 2, aqueous solution 140; para [0255], [0259]-[0260]), the method comprising:
- a step of electrolysis under biasing inducing, at the negative electrode, a reduction of the oxidized metal element inducing, at the positive electrode, the generation of oxygen O2 forming at the OER electrode (the “Discharge” reaction as illustrated in figure 5b, in which nickel at the negative electrode is reduced from Ni3+ to Ni2+, and the Pt anode operates as an OER electrode; para [0266]);
- a step of conversion by reaction, between the positive electrode generating hydrogen H2, forming the HER electrode, accompanied by oxidation of the reduced metal species at the negative electrode (the “Charge” reaction as illustrated in figure 5a, in which nickel at the negative electrode is oxidized from Ni2+ to Ni3+, and the Pt anode operates as an HER electrode; para [0265]).
Rothschild further teaches that their device for performing the water splitting method additionally comprises a device for storing the gaseous hydrogen generated by the method; and a device for storing the gaseous oxygen generated by the method (para [0272]; claims 32, 33, and 34).
It would have been obvious to a person having ordinary skill in the art before the effective filing date of the claimed invention to incorporate, into Huang’s hydrogen-and-oxygen production system, a second gas storage device for storing the oxygen produced by the system, based on Rothschild’s disclosure of a similar hydrogen-and-oxygen production system, which comprises a first gas storage device for storing the hydrogen produced, and a second gas storage device for storing the oxygen produced. One possible motivation to store the produced oxygen, rather than discharging it to exhaust as Huang does (Huang at para [0026]), could be to reserve the oxygen for productive use, such as an oxygen-consuming fuel cell as contemplated by Huang (para [0002]).
Conclusion
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/ANDREW KOLTONOW/Examiner, Art Unit 1795
/ALEXANDER W KEELING/Primary Examiner, Art Unit 1795
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