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 .
Priority
Receipt is acknowledged of certified copies of papers required by 37 CFR 1.55.
Election/Restrictions
Applicant's election with traverse of Group I, claims 36-64 and 67-69 in the reply filed on 04/17/2026 is acknowledged.
The traversal is on the grounds that Fang does not disclose a method in which nanoparticles are deposited on carbon support by reduction of urea/urea derivative metal complexes adsorbed on the surface of this support. Applicant summarizes the perceived differences between the prior art product of Fang and the instant invention on Pg. 11, noting differences in the distribution of size of nanoparticles, cyclic voltammograms, and the solubility of the metal-urea complexes in water.
This is not found persuasive because these features and differences noted by Applicant do not pertain to the special technical feature identified by Examiner in the restriction requirement mailed 02/17/2026. In this action, Examiner stated the shared technical feature between Group I, claims 36-64 and 67-69, Group II, claims 65-66, and Group III, claim 70 was “complexes of platinum group metals with urea complexing agent for adsorption of platinum group metal precursors on carbon supports”. The prior art Fang teaches a method of synthesizing Pt catalysts supported on carbon-based supports, including vulcanized carbon black (VC), that includes the aid of urea to deposit the platinum on the carbon support (Abstract; Pg. 15332, 2.1 Synthesis of VC-Supported Pt Catalysts; Pg. 15337-15338, Conclusions). Fang clearly describes the deposition (i.e. adsorption) of platinum on carbon supports with the use of platinum complexes (H2PtCl6, listed in 2.1 Synthesis of VC-Supported Catalysts) and urea as a deposition assistant. Examiner encourages Applicant to review the independent claims of 04/17/2026 (i.e. claim 36, 65, and 70), where features discussed by Applicant including nanoparticles, reduction of urea derivatives, the distribution of size of nanoparticles, cyclic voltammograms, and the solubility of the metal-urea complexes in water are not shared features between the independent claims.
The requirement is still deemed proper and is therefore made FINAL.
Response to Arguments Presented in 1.132 Declaration
The 1.132 declaration filed on 04/17/2026 is acknowledged and is entered.
In the declaration, Prof. Adam Lewera discloses a series of experiments that are intended to confirm the metal-urea complexes are formed at reaction conditions specified in the application. In particular, complexes with urea complexing a platinum group metal where platinum group metals are reduced with a urea complexing agent adsorbed on the carbon support “with the formation of a product of carbon-supported metal nanoparticles” was stated to be disclosed.
Examiner acknowledges the Experimental results in Examples 1-7 on Pg. 2-11 of the Declaration however the Declaration is not convincing in regards to the restriction requirement for unity of invention set forth by Examiner on 02/17/2026. Specifically, Examiner stated the shared technical feature between Group I, claims 36-64 and 67-69, Group II, claims 65-66, and Group III, claim 70 was “complexes of platinum group metals with urea complexing agent for adsorption of platinum group metal precursors on carbon supports”. Notably, the reduction of the urea-platinum group complexes, as well as the other technical aspects discussed in Pg. 2-11 of the Declaration, are not shared technical features between the independent invention groups outlined in the restriction requirement. Accordingly, because the shared technical feature between independent claims sets forth the requirement for unity of invention, the declaration is not persuasive and the restriction is made final.
Claim Objections
Claims 36-63, 65, and 67-69 are objected to because of the following informalities:
Regarding claim 36, line 5, the phrase “agent on carbon support” is likely intended to read “agent onto a carbon support”.
Regarding claim 36, line 6, the phrase “wherein complexes with a urea…” is likely intended to read “wherein the complexes with a urea…”.
Claims 39, 50-54, 56, and 63 are objected to under 37 CFR 1.75(c) as being in improper form because a multiple dependent claim cannot depend on another multiple dependent claim. Specifically, claims 39, 50, 53, 56, and 63 depend from any of claims 36-39, where claim 38 is a multiple dependent claim, depending from claims 36 or 37. See MPEP § 608.01(n). Claims 51-54 depend on objected claim 50 and are thus also objected to. In the interest of compact prosecution, when applying art to the objected-to multiple dependent claims, the independent claim will be selected as the claim from which the multiply dependent claim depends. For example, claim 39 is examined as depending from 36.
Claim 42, line 7, it appears there may be an extra space in the phrase “agent undergo”.
Appropriate correction is required.
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 36-63, 65, and 67-69 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.
Claim 36, line 9 is indefinite for the language “selected from a group comprising urea, …” and line 12 is indefinite for the language “selected from a group comprising methylurea,…”. The use of the word “comprising” is not appropriate here as it is open ended language such that it is unclear what other things are included in the group. See MPEP 2173.05(h).
Claim 36, line 10, the term “urea derivative” is indefinite. The term “derivative” is unclear in that the meets and bounds of what constitutes a “urea derivative” is not understood from the claims. This lack of clarity is exacerbated by the known ability of urea to decompose to provide hydroxide ions such that a skilled artisan could potentially interpret a urea-derived hydroxide ion as a “urea derivatives,” being derived from urea. Additionally, the Markush listing in claim 36 including the term “comprising” further broadens the scope of what a urea derivative could be.
Claim 41, line 4-5 is indefinite for the language “selected from a group comprising urea, …”. The use of the word “comprising” is not appropriate here as it is open ended language such that it is unclear what other things are included in the group. See MPEP 2173.05(h).
Claim 62 is indefinite for the language “selected from a group comprising K2PtCl4, …”. The use of the word “comprising” is not appropriate here as it is open ended language such that it is unclear what other things are included in the group. See MPEP 2173.05(h).
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Claim 63, the phrase “the urea derivative is a compound containing a -HN-CO- or -HN-CO-NH- functional group” is unclear. It is unclear because the compound urea has a formula of CO(NH2)2, depicted below:
Accordingly, the compound urea contains a -HN-CO-NH- functional group and could be considered a “urea derivative” according to the claim. In the interest of compact prosecution, urea is interpreted to be a “compound containing a -HN-CO- or -HN-CO-NH- functional group,” meeting the limitation required by the claim.
Claims 37-63 and 65 depend from claim 36 and thus are also rendered indefinite.
Claim 67, line 4 is indefinite for the language “selected from a group comprising urea, …” and line 9 is indefinite for the language “selected from a group comprising methylurea,…”. The use of the word “comprising” is not appropriate here as it is open ended language such that it is unclear what other things are included in the group. See MPEP 2173.05(h).
Claims 68-69 depend from claim 67 and thus are also rendered indefinite.
Claim Rejections - 35 USC § 103
In the event the determination of the status of the application as subject to AIA 35 U.S.C.
102 and 103 (or as subject to pre-AIA 35 U.S.C. 102 and 103) is incorrect, any correction of the
statutory basis for the rejection will not be considered a new ground of rejection if the prior art
relied upon, and the rationale supporting the rejection, would be the same under either status.
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.
Claims 36-40, 53, and 56 are rejected under 35 U.S.C. 103 as being unpatentable over Yu (US20110065025; cited in IDS dated 05/01/2024).
Regarding claim 36, Yu teaches a method of preparing a platinum/support catalyst that comprises preparing a dispersion solution including urea, a support, and a water-soluble metal having catalytic activity and reacting to deposit the metal particles on the support (Abstract). Yu teaches the reaction of urea and platinum compounds produces platinum complexes that are adsorbed on the carbon support ([0066]-[0067]). Accordingly, Yu teaching urea forms complexes with platinum would reasonably suggest to a skilled artisan that “coordination complexes containing a platinum group metal as the central ion and at least one molecule of urea or urea derivative as ligand(s)” would be formed in the process of Yu, given the same materials (i.e. urea and platinum source) being used. This conclusion is further supported by Yu teaching urea interacts with the platinum species to provide platinum complex species with a smaller size than platinum particles lacking urea ([0082]), clearly teaching an interaction between urea and platinum that is understood to be a coordination (i.e. bonding) interaction.
Yu further teaches the platinum complexes are reacted at high temperature to deposit metal hydroxide species on the support that are reduced to form catalyst nanoparticles loaded on the carbon support (Abstract; [0006]; [0013]; [0019]).
It is noted Yu deposits the platinum-urea species as a platinum hydroxide following high temperature treatment prior to reduction while the instant invention claims reduction of the platinum group metal with urea complexing agent. However, because the claims include the language “comprises” in line 2, the claims broaden the scope of the claims such that the teaching of Yu fully encompass the limitations of the claims.
Regarding claim 37, Yu teaches the process of claim 36.
Yu further teaches in the adsorption step, additional metals can be included, selected from a group consisting of platinum (Pt), ruthenium (Ru), rhodium (Rh), molybdenum (Mo), osmium (Os), iridium (Ir), rhenium (Re), palladium (Pd), vanadium (V), tungsten (W), cobalt (Co), iron (Fe), selenium (Se), nickel (Ni), bismuth (Bi), tin (Sn), chromium (Cr), titanium (Ti), gold (Au), cerium (Ce) and copper (Cu) ([0097]). The instant invention describes platinum group metals as including platinum, palladium, rhodium, iridium, ruthenium, and osmium (see Pg. 2, lines 1-9 of the specification).
Regarding claim 38, Yu teaches the process of claim 36.
Yu further teaches in the adsorption step, additional metals can be included, selected from a group consisting of platinum (Pt), ruthenium (Ru), rhodium (Rh), molybdenum (Mo), osmium (Os), iridium (Ir), rhenium (Re), palladium (Pd), vanadium (V), tungsten (W), cobalt (Co), iron (Fe), selenium (Se), nickel (Ni), bismuth (Bi), tin (Sn), chromium (Cr), titanium (Ti), gold (Au), cerium (Ce) and copper (Cu) ([0097]). The instant invention describes platinum group metals as including platinum, palladium, rhodium, iridium, ruthenium, and osmium (see Pg. 2, lines 1-9 of the specification) and accordingly Yu teaching at least molybdenum qualifies as a “metal other than platinum group metals,” meeting the claim limitation.
Regarding claim 39, Yu teaches the process of claim 36.
Yu further teaches the platinum group metal precursors include chloride ligands when being mixed with urea in an aqueous solution, in addition to water and hydroxide ligands ([0076]-[0079]; [0108]).
Regarding claim 40, Yu teaches the process of claim 36.
Yu further teaches the dispersion including urea, a support, and a water-soluble metal having catalytic activity is in aqueous solution (Claim 3 and 10; [0011]).
Regarding claim 53, Yu teaches the process of claim 36.
Yu further teaches the reduction is carried out in aqueous solution using a reducing agent ([0104]).
Regarding claim 56, Yu teaches the process of claim 36.
Yu further teaches the amount of metal in the product can be adjusted to be within a wide range of 5-95% by weight based on the total weight of the product ([0106]). Yu teaches the synthesis includes a molar ratio of urea to Pt-Ru of 20:1 ([0108]-[0111]). Since Yu arrives at a total metal concentration within the claimed range and discloses a urea to metal ratio during the synthesis, Yu sufficiently discloses adjusting the reactant ratios to a skilled artisan and meets the limitation “the amounts of complexes of platinum group metal with urea complexing agent and carbon support in step (b) are adjusted”. In the case where the claimed ranges "overlap or lie inside ranges disclosed by the prior art" a prima facie case of obviousness exists. MPEP 2144.05 (I). In the instant case, the range taught by Yu (5-95% metal by weight based on total weight of product) overlaps with the claimed range (0.001 to 60% metal by weight calculated based on the total weight of the product). Therefore, the range in Yu renders obvious the claimed range.
Regarding claim 63, Yu teaches the process of claim 36.
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Yu teaches urea (CO(NH2)2) is used to assist the metal deposition ([0071]). As stated in the 112(b) section above, urea has the structure: which includes a -NH-CO- and -NH-CO-NH linkage, meeting the limitation required by the claim for a urea derivative as a “compound containing a -HN-CO- or -HN-CO-NH- functional group.”
Claims 41-44, 55, 62 are rejected under 35 U.S.C. 103 as being unpatentable over Yu (US20110065025; cited in IDS dated 05/01/2024) in view of Kim et al. (Catalysis Today 2010, 158, 354-360).
Regarding claim 41, Yu teaches the method of claim 36 and the claim further requires “steps (b) and (c) are preceded by step (a) of complex formation by reacting in a solution a platinum group metal precursor with a urea complexing agent selected from a group comprising urea, urea derivative, a mixture of urea with at least one urea derivative, and a mixture of at least two urea derivatives,” to which Yu teaches the urea, the metal salt, and the support are mixed together.
Kim teaches the preparation of supported PtRu catalyst via urea-assisted homogenous deposition where the synthesis includes mixing hexachloroplatinate and ruthenium chloride in water, adding a urea solution, and stirring to form a metal salt-urea mixture (Title; Abstract; Pg. 354, Introduction; Pg. 356, 2.1).
Advantageously, preparing the metal salt-urea mixture prior to the addition of the carbon support provides products with better dispersion of smaller particles and thus enhanced catalytic activity (Pg. 355, right col.-Pg. 356, left col.).
Thus, prior to the effective filing date of the claimed invention, it would have been obvious to one of ordinary skill in the art to mix the metal salt and urea prior to reaction with a support in the method of Yu in order to provide better dispersion and a catalyst with enhanced activity, as taught by Kim.
Regarding claim 42, Yu teaches the method of claim 36 and Yu in view of Kim teach the method of claim 41.
Yu teaches a method of preparing a platinum/support catalyst that comprises preparing a dispersion solution including urea, a carbon support, and a water-soluble metal having catalytic activity and reacting to deposit the metal particles on the support (Abstract). Yu teaches the dispersion is heated to deposit the metal on the carbon support prior to performing reduction that produces catalyst nanoparticles loaded on the carbon support (Abstract; [0006]; ([0010]); [0013]; [0019]).
Regarding claim 43, Yu teaches the method of claim 36 and Yu in view of Kim teach the method of claim 41.
Yu teaches a method of preparing a platinum/support catalyst that comprises preparing a dispersion solution including urea, a carbon support, and a water-soluble metal having catalytic activity and reacting to deposit the metal particles on the support (Abstract). Yu teaches the dispersion is heated to deposit the metal on the carbon support prior to performing reduction that produces a catalyst nanoparticles loaded on the carbon support (Abstract; [0006]; ([0010]); [0013]; [0019]). As described above, these teachings are equivalent to step (b) and step (c) of the claimed invention.
The claim further requires “step (a) and (b) are carried out separately” to which Yu is silent.
Kim teaches the preparation of supported PtRu catalyst via urea-assisted homogenous deposition where the synthesis includes mixing hexachloroplatinate and ruthenium chloride in water, adding a urea solution, and stirring to form a metal salt-urea mixture (Title; Abstract; Pg. 354, Introduction; Pg. 356, 2.1). Kim teaches after obtaining the metal salt-urea mixture, a carbon support can be added to form an aqueous dispersion that is then heated and reduced to generate a PtRu catalyst supported on vulcanized carbon (Pg. 356, 2.1).
Advantageously, preparing the metal salt-urea mixture prior to the addition of the carbon support provides products with better dispersion of smaller particles and thus enhanced catalytic activity (Pg. 355, right col.-Pg. 356, left col.).
Thus, prior to the effective filing date of the claimed invention, it would have been obvious to one of ordinary skill in the art to mix the metal salt and urea prior to reaction with a support in the method of Yu in order to provide better dispersion and a catalyst with enhanced activity, as taught by Kim.
Regarding claim 44, Yu teaches the method of claim 36 and Yu in view of Kim teach the method of claim 41.
The claim further requires “step (a)…is carried out in an aqueous solution” to which Yu is silent.
Kim teaches the preparation of supported PtRu catalyst via urea-assisted homogenous deposition where the synthesis includes mixing hexachloroplatinate and ruthenium chloride in water, adding a water solution of urea, and stirring to form an aqueous metal salt-urea mixture (Title; Abstract; Pg. 354, Introduction; Pg. 356, 2.1).
Advantageously, preparing the metal salt-urea mixture according to the process of Kim, including as an aqueous solution, provides products with better dispersion of smaller particles and thus enhanced catalytic activity (Pg. 355, right col.-Pg. 356, left col.).
Thus, prior to the effective filing date of the claimed invention, it would have been obvious to one of ordinary skill in the art to mix the metal salt and urea in aqueous solution in the method of Yu in order to provide better dispersion and a catalyst with enhanced activity, as taught by Kim.
Regarding claim 55, Yu teaches the process of claim 36 and Yu in view of Kim teach the method of claim 41.
The claim further requires “a molar ratio of urea complexing agent to metal used in step (a) is in the range of 1-20:1,” to which Yu is silent.
Kim teaches the molar ratio of urea to the metal was ~20 (i.e. ~20:1) (Pg. 356, left col.). In the case where the claimed ranges "overlap or lie inside ranges disclosed by the prior art" a prima facie case of obviousness exists. MPEP 2144.05 (I). In the instant case, the range taught by Kim (urea to metal molar ratio ~20) overlaps with the claimed range (urea to metal molar ratio 1-20:1). Therefore, the range in Kim renders obvious the claimed range.
Advantageously, providing the molar ratio of urea to metal taught by Kim ensures sufficient urea is in solution to undergo in situ hydrolysis to hydroxide ions, which stabilizes the metal hydroxides on the support as well as protecting the metal from agglomeration and precipitation (Pg. 358, right col-Pg. 359, left col.).
Thus, prior to the effective filing date of the claimed invention, it would have been obvious to one of ordinary skill in the art to provide a urea to metal molar ratio of about 20 in step (a) in the method of Yu in order to provide better dispersion and a catalyst with enhanced activity, as taught by Kim.
Claims 45-52 are rejected under 35 U.S.C. 103 as being unpatentable over Yu (US20110065025; cited in IDS dated 05/01/2024) in view of Toebes et al. (J. Phys. Chem. B 2004, 108, 11611-11619).
Regarding claim 45, Yu teaches the method of claim 36 and the claim further requires the “reduction in step (c) is carried out by using gaseous hydrogen” to which Yu is silent.
Toebes teaches a method of preparing a carbon fiber supported platinum and ruthenium catalyst where after the platinum and ruthenium are deposited on the support the metals are reduced in a hydrogen atmosphere (Pg. 11612-11613, Synthesis of CNF-Supported Ruthenium and Platinum Catalysts; Pg. 11613, Right col.).
Advantageously, the reduction treatment of Toebes provides homogenous distribution of platinum particles (Pg. 11614, right col.).
Thus, prior to the effective filing date of the claimed invention, it would have been obvious to one of ordinary skill in the art to reduce the metal/support material with hydrogen gas in the method of Yu in order to provide homogenous distribution of platinum particles as taught by Toebes.
Regarding claim 46, Yu teaches the method of claim 36 and the claim further requires the “reduction in step (c) is carried out in temperature of 50 - 200 °C by placing the carbon support with adsorbed complexes of a platinum group metal with a urea complexing agent in a stream of a gas mixture of hydrogen with an inert gas” to which Yu is silent.
Toebes teaches a method of preparing a carbon fiber supported platinum and ruthenium catalyst where after the platinum and ruthenium are deposited on the support, the metals are reduced in a hydrogen atmosphere (Pg. 11612-11613, Synthesis of CNF-Supported Ruthenium and Platinum Catalysts; Pg. 11613, Right col.). Toebes teaches the reduction is carried out at 473 K (i.e. 199.85 °C) with a 5% hydrogen and 95% argon gas mixture (Pg. 11612-11613, Synthesis of CNF-Supported Ruthenium and Platinum Catalysts; Pg. 11613, Right col.). In the case where the claimed ranges "overlap or lie inside ranges disclosed by the prior art" a prima facie case of obviousness exists. MPEP 2144.05 (I). In the instant case, the range taught by Toebes (199.85 °C) overlaps with the claimed range (50-200 °C). Therefore, the range in Toebes renders obvious the claimed range.
Advantageously, the reduction treatment of Toebes provides homogenous distribution of platinum particles (Pg. 11614, right col.).
Thus, prior to the effective filing date of the claimed invention, it would have been obvious to one of ordinary skill in the art to reduce the metal/support material at 473 K (i.e. 199.85 °C) with a 5% hydrogen and 95% argon gas mixture in the method of Yu in order to provide homogenous distribution of platinum particles as taught by Toebes.
Regarding claims 47, Yu teaches the method of claim 36 and Yu in view of Toebes teach the method of claim 46.
The claim further requires the “the gas mixture contains 1 - 10% of hydrogen” to which Yu is silent.
Toebes teaches a method of preparing a carbon fiber supported platinum and ruthenium catalyst where after the platinum and ruthenium are deposited on the support the metals are reduced in a hydrogen atmosphere (Pg. 11612-11613, Synthesis of CNF-Supported Ruthenium and Platinum Catalysts; Pg. 11613, Right col.). Toebes teaches the reduction is carried out at 473 K (i.e. 199.85 °C) with a 5% hydrogen and 95% argon gas mixture (Pg. 11612-11613, Synthesis of CNF-Supported Ruthenium and Platinum Catalysts; Pg. 11613, Right col.). In the case where the claimed ranges "overlap or lie inside ranges disclosed by the prior art" a prima facie case of obviousness exists. MPEP 2144.05 (I). In the instant case, the range taught by Toebes (5% hydrogen) overlaps with the claimed range (1-10% hydrogen). Therefore, the range in Toebes renders obvious the claimed range.
Advantageously, the reduction treatment of Toebes provides a homogenous distribution of platinum particles (Pg. 11614, right col.).
Thus, prior to the effective filing date of the claimed invention, it would have been obvious to one of ordinary skill in the art to reduce the metal/support material at 473 K (i.e. 199.85 °C) with a 5% hydrogen and 95% argon gas mixture in the method of Yu in order to provide a homogenous distribution of platinum particles as taught by Toebes.
Regarding claims 48, Yu teaches the method of claim 36 and Yu in view of Toebes teach the method of claim 46.
The claim further requires “the reduction is carried out for 1 to 6 hours” to which Yu is silent.
Toebes teaches a method of preparing a carbon fiber supported platinum and ruthenium catalyst where after the platinum and ruthenium are deposited on the support the metals are reduced in a hydrogen atmosphere for 1 h (Pg. 11612-11613, Synthesis of CNF-Supported Ruthenium and Platinum Catalysts; Pg. 11613, Right col.). In the case where the claimed ranges "overlap or lie inside ranges disclosed by the prior art" a prima facie case of obviousness exists. MPEP 2144.05 (I). In the instant case, the range taught by Toebes (1 hour) overlaps with the claimed range (1 to 6 hours). Therefore, the range in Toebes renders obvious the claimed range.
Advantageously, the reduction treatment of Toebes provides a homogenous distribution of platinum particles (Pg. 11614, right col.).
Thus, prior to the effective filing date of the claimed invention, it would have been obvious to one of ordinary skill in the art to reduce the metal/support material for 1 hour in the method of Yu in order to provide a homogenous distribution of platinum particles as taught by Toebes.
Regarding claims 49, Yu teaches the method of claim 36 and Yu in view of Toebes teach the method of claim 46.
The claim further requires the “the inert gas is argon or nitrogen” to which Yu is silent.
Toebes teaches a method of preparing a carbon fiber supported platinum and ruthenium catalyst where after the platinum and ruthenium are deposited on the support the metals are reduced in a hydrogen atmosphere for 1 h (Pg. 11612-11613, Synthesis of CNF-Supported Ruthenium and Platinum Catalysts; Pg. 11613, Right col.). Toebes teaches the reduction is carried out at 473 K (i.e. 199.85 °C) with a 5% hydrogen and 95% argon gas mixture (Pg. 11612-11613, Synthesis of CNF-Supported Ruthenium and Platinum Catalysts; Pg. 11613, Right col.).
Advantageously, the reduction treatment of Toebes provides homogenous distribution of platinum particles (Pg. 11614, right col.).
Thus, prior to the effective filing date of the claimed invention, it would have been obvious to one of ordinary skill in the art to reduce the metal/support material with the inert gas argon present in the method of Yu in order to provide homogenous distribution of platinum particles as taught by Toebes.
Regarding claim 50, Yu teaches the method of claim 36.
The claim further requires the “reduction in step (c) is carried out by thermal decomposition of adsorbed metal- urea complexing agent in inert atmosphere” to which Yu is silent.
Toebes teaches a method of preparing a carbon fiber supported platinum and ruthenium catalyst where after the platinum and ruthenium are deposited on the support, reduction is carried out at 473 K (i.e. 199.85 °C) with a 5% hydrogen and 95% argon gas mixture (Pg. 11612-11613, Synthesis of CNF-Supported Ruthenium and Platinum Catalysts; Pg. 11613, Right col.). It is noted Toebes includes hydrogen in the reduction, however the claims do not exclude hydrogen and Toebes including heating at 199.85 °C in the presence of an inert gas (argon), meets the limitation “carried out by thermal decomposition”. This interpretation is supported by at least claims 51-52 that further describe the thermal decomposition conditions.
Advantageously, the reduction treatment of Toebes provides a homogenous distribution of platinum particles (Pg. 11614, right col.).
Thus, prior to the effective filing date of the claimed invention, it would have been obvious to one of ordinary skill in the art to reduce the metal/support material at elevated temperatures with an inert gas of argon present in the method of Yu in order to provide homogenous distribution of platinum particles as taught by Toebes.
Regarding claim 51, Yu teaches the method of claim 36 and Yu in view of Toebes teaches the method of claim 50.
The claim further requires the “reduction in step (c) is carried out in temperature of 190 - 600 0C by placing the carbon support with adsorbed complexes of a platinum group metal with a urea complexing agent in a stream of an inert gas” to which Yu is silent.
Toebes teaches a method of preparing a carbon fiber supported platinum and ruthenium catalyst where after the platinum and ruthenium are deposited on the support, reduction is carried out at 473 K (i.e. 199.85 °C) with a 5% hydrogen and 95% argon gas mixture (Pg. 11612-11613, Synthesis of CNF-Supported Ruthenium and Platinum Catalysts; Pg. 11613, Right col.). Toebes teaches the reduction gas can be passed over the material in a flow (Pg. 11613, Right col.). In the case where the claimed ranges "overlap or lie inside ranges disclosed by the prior art" a prima facie case of obviousness exists. MPEP 2144.05 (I). In the instant case, the range taught by Toebes (199.85 °C) overlaps with the claimed range (190-600 °C). Therefore, the range in Toebes renders obvious the claimed range.
Advantageously, the reduction treatment of Toebes provides a homogenous distribution of platinum particles (Pg. 11614, right col.).
Thus, prior to the effective filing date of the claimed invention, it would have been obvious to one of ordinary skill in the art to reduce the metal/support material at elevated temperatures with an inert gas of argon present in the method of Yu in order to provide a homogenous distribution of platinum particles as taught by Toebes.
Regarding claim 52, Yu teaches the method of claim 36 and Yu in view of Toebes teaches the method of claim 50 and 51.
The claim further requires the “inert gas is argon or nitrogen” to which Yu is silent.
Toebes teaches a method of preparing a carbon fiber supported platinum and ruthenium catalyst where after the platinum and ruthenium are deposited on the support, reduction is carried out at 473 K (i.e. 199.85 °C) with a 5% hydrogen and 95% argon gas mixture (Pg. 11612-11613, Synthesis of CNF-Supported Ruthenium and Platinum Catalysts; Pg. 11613, Right col.). In the case where the claimed ranges "overlap or lie inside ranges disclosed by the prior art" a prima facie case of obviousness exists. MPEP 2144.05 (I). In the instant case, the range taught by Toebes (199.85 °C) overlaps with the claimed range (190-600 °C). Therefore, the range in Toebes renders obvious the claimed range.
Advantageously, the reduction treatment of Toebes provides a homogenous distribution of platinum particles (Pg. 11614, right col.).
Thus, prior to the effective filing date of the claimed invention, it would have been obvious to one of ordinary skill in the art to reduce the metal/support material at elevated temperatures with an inert gas of argon present in the method of Yu in order to provide a homogenous distribution of platinum particles as taught by Toebes.
Claim 54 is rejected under 35 U.S.C. 103 as being unpatentable over Yu (US20110065025; cited in IDS dated 05/01/2024) in view of Zeng et al. (CN106582620B English).
Regarding claim 54, Yu teaches the method of claim 36 and 53.
The claim further requires the “reducing agent is L-ascorbic acid or citric acid” to which Yu is silent.
Zeng teaches a method of preparing a highly-dispersed noble metal powder catalyst where noble metal compounds including Pt, Pd, and Ru, are loaded on a carrier, including a carbon carrier, prior to being reduced with one or more of citric acid and ascorbic acid, among others (Claims 1-3 and 8; Pg. 3, par. 5).
Advantageously, performing the method of Zeng provides a highly dispersed noble metal on the carrier that has high catalytic activity and selectivity (Pg. 3, par. 9-11).
Thus, prior to the effective filing date of the claimed invention, it would have been obvious to one of ordinary skill in the art to reduce the metal/support material with citric acid or ascorbic acid in the method of Yu in order to provide highly dispersed noble metal on the carrier that has high catalytic activity and selectivity, as taught by Zeng.
Claims 57-59, 61-62 are rejected under 35 U.S.C. 103 as being unpatentable over Yu (US20110065025; cited in IDS dated 05/01/2024) in view of Kim et al. (Catalysis Today 2010, 158, 354-360) and further in view of Anastassopoulou et al. (Inorg. Chem. Act. 1989, 159, 237-241; cited in IDS dated 05/01/2024).
Regarding claim 57, Yu teaches the method of claim 36 and Yu in view of Kim teach the method of claim 41.
The claim further requires “the concentrations of the metal precursors and urea complexing agents in the solution used in step (a) are in a range from 1 mM to 5 M,” to which Yu and Kim are silent.
Anastassopoulou teaches a method of preparing platinum-urea complexes where a water solution of potassium tetrachloroplatinate has a concentration of 0.15 M and a urea solution in water has a concentration of 0.3 M (Pg. 237, right col.). In the case where the claimed ranges "overlap or lie inside ranges disclosed by the prior art" a prima facie case of obviousness exists. MPEP 2144.05 (I). In the instant case, the values taught by Anastassopoulou (0.15 M platinum solution; 0.3 M urea solution) overlaps with the claimed range (1 mM to 5 M). Therefore, the value in Anastassopoulou renders obvious the claimed range.
Anastassopoulou is considered pertinent prior art to the instant invention because step (a) is interpreted as a platinum group metal-urea coordination step (see claim 41 and Pg. 4, lines 1-6 in the instant specification) and the disclosure of Anastassopoulou describes the coordination of urea with platinum.
Advantageously, the urea-platinum complexes prepared by the method of Anastassopoulou are stable in neutral and alkaline solutions (Pg. 237, right col.).
Thus, prior to the effective filing date of the claimed invention, it would have been obvious to one of ordinary skill in the art to provide solution concentrations with the values taught by Anastassopoulou in the method of Yu in order to provide complexes that are stable in neutral and alkaline solution, as taught by Anastassopoulou.
Regarding claim 58, Yu teaches the method of claim 36 and Yu in view of Kim teach the method of claim 41.
The claim further requires “in step (a) the solution comprising a platinum group metal precursor and urea or urea derivative is heated at 40 to 100 °C under reflux,” to which Yu and Kim are silent.
Anastassopoulou teaches a method of preparing platinum-urea complexes where a water solution of potassium tetrachloroplatinate and a urea solution in water are heated to 100 °C for 10 minutes (Pg. 237, right col.). Anastassopoulou discloses heating the solution to the 100 °C, which is within the claimed heating range, and accordingly Anastassopoulou meets the limitation “heated at 40 to 100 °C under reflux.” In the case where the claimed ranges "overlap or lie inside ranges disclosed by the prior art" a prima facie case of obviousness exists. MPEP 2144.05 (I). In the instant case, the value taught by Anastassopoulou (100 °C) overlaps with the claimed range (40 to 100 °C). Therefore, the value in Anastassopoulou renders obvious the claimed range.
Anastassopoulou is considered pertinent prior art to the instant invention because step (a) is interpreted as a platinum group metal-urea coordination step (see claim 41 and Pg. 4, lines 1-6 in the instant specification) and the disclosure of Anastassopoulou describes the coordination of urea with platinum.
Advantageously, the urea-platinum complexes prepared by the method of Anastassopoulou are stable in neutral and alkaline solutions (Pg. 237, right col.).
Thus, prior to the effective filing date of the claimed invention, it would have been obvious to one of ordinary skill in the art to heat the urea and metal solution at 100 °C in the method of Yu in order to provide complexes that are stable in neutral and alkaline solution, as taught by Anastassopoulou.
Regarding claim 59, Yu teaches the method of claim 36, Yu in view of Kim teach the method of claim 41, and Yu in view of Kim and Anastassopoulou teach the method of claim 58.
The claim further requires “in step (a) the solution comprising a platinum group metal precursor and urea complexing agents is heated for 10 minutes - 10 hours,” to which Yu and Kim are silent.
Anastassopoulou teaches a method of preparing platinum-urea complexes where a water solution of potassium tetrachloroplatinate and a urea solution in water are heated to 100 °C for 10 minutes (Pg. 237, right col.). In the case where the claimed ranges "overlap or lie inside ranges disclosed by the prior art" a prima facie case of obviousness exists. MPEP 2144.05 (I). In the instant case, the value taught by Anastassopoulou (10 minutes) overlaps with the claimed range (10 minutes to 10 hours). Therefore, the value in Anastassopoulou renders obvious the claimed range.
Anastassopoulou is considered pertinent prior art to the instant invention because step (a) is interpreted as a platinum group metal-urea coordination step (see claim 41 and Pg. 4, lines 1-6 in the instant specification) and the disclosure of Anastassopoulou describes the coordination of urea with platinum.
Advantageously, the urea-platinum complexes prepared by the method of Anastassopoulou are stable in neutral and alkaline solutions (Pg. 237, right col.).
Thus, prior to the effective filing date of the claimed invention, it would have been obvious to one of ordinary skill in the art to heat the urea and platinum solution for 10 minutes in the method of Yu in order to provide complexes that are stable in neutral and alkaline solution, as taught by Anastassopoulou.
Regarding claim 61, Yu teaches the method of claim 36 and Yu in view of Kim teach the method of claim 41.
The claim further requires “in step (a) an organic solvent is added to the solution in a volumetric ratio of 0.05 - 30:1 calculated based on water volume in the solution,” to which Yu and Kim are silent.
Anastassopoulou teaches a method of preparing platinum-urea complexes where a water solution of potassium tetrachloroplatinate and a urea solution are mixed prior to adding 20 vol. of ethanol relative to the aqueous solution (Pg. 237, right col.). Ethanol is an organic solvent and is described as such in the instant specification in at least Pg. 13, lines 14-20 of the instant specification. In the case where the claimed ranges "overlap or lie inside ranges disclosed by the prior art" a prima facie case of obviousness exists. MPEP 2144.05 (I). In the instant case, the value taught by Anastassopoulou (20 vol. of ethanol relative to the water volume) overlaps with the claimed range (volumetric ratio of 0.05-30:1 of organic solvent to water). Therefore, the value in Anastassopoulou renders obvious the claimed range.
Anastassopoulou is considered pertinent prior art to the instant invention because step (a) is interpreted as a platinum group metal-urea coordination step (see claim 41 and Pg. 4, lines 1-6 in the instant specification) and the disclosure of Anastassopoulou describes the coordination of urea with platinum.
Advantageously, the urea-platinum complexes prepared by the method of Anastassopoulou are stable in neutral and alkaline solutions (Pg. 237, right col.).
Thus, prior to the effective filing date of the claimed invention, it would have been obvious to one of ordinary skill in the art to add 20 vol. of ethanol relative to the aqueous solution in the method of Yu in order to provide urea-platinum complexes that are stable in neutral and alkaline solution, as taught by Anastassopoulou.
Regarding claim 62, Yu teaches the process of claim 36 and Yu in view of Kim teach the method of claim 41.
The claims further requires “the metal precursor is selected from the group comprising K2PtCl4, K2PdCl4, and IrCl4” to which Yu and Kim are silent.
Anastassopoulou teaches a method of preparing platinum-urea complexes where a water solution of potassium tetrachloroplatinate (i.e. K2PtCl4) is used (Pg. 237, right col.).
Anastassopoulou is considered pertinent prior art to the instant invention because step (a) is interpreted as a platinum group metal-urea coordination step (see claim 41 and Pg. 4, lines 1-6 in the instant specification) and the disclosure of Anastassopoulou describes the coordination of urea with platinum.
Advantageously, urea-platinum complexes prepared with K2PtCl4 (potassium tetrachloroplatinate) are stable and well-defined (Pg. 237, left col.).
Thus, prior to the effective filing date of the claimed invention, it would have been obvious to one of ordinary skill in the art to use K2PtCl4 (potassium tetrachloroplatinate) as the metal precursor in the method of Yu in order to produce a stable and well-defined urea-platinum complex, as taught by Anastassopoulou.
Claim 60 is rejected under 35 U.S.C. 103 as being unpatentable over Yu (US20110065025; cited in IDS dated 05/01/2024) in view of Kim et al. (Catalysis Today 2010, 158, 354-360) and further in view of Song et al. (Applied Energy 2012, 100, 132-137).
Regarding claim 60, Yu teaches the method of claim 36 and Yu in view of Kim teach the method of claim 41.
The claim further requires “in step (a) the solution comprising a platinum group metal precursor and urea complexing agent is heated at 40 to 100 °C until all the liquid evaporates,” to which Yu and Kim are silent.
Song teaches a method of preparing a Pt electrode material by the homogenous deposition of solutions containing urea and platinum that are prepared by dissolving H2PtCl6 in ethanol, adding an aqueous urea solution to the Pt solution, and heating the mixture to 80 °C to dry the droplets of urea-Pt solution on a glass substrate (Abstract; Title; Pg. 133, 2.1). In the case where the claimed ranges "overlap or lie inside ranges disclosed by the prior art" a prima facie case of obviousness exists. MPEP 2144.05 (I). In the instant case, the value taught by Song (80 °C) overlaps with the claimed range (40 to 100 °C). Therefore, the value in Song renders obvious the claimed range.
Advantageously, the deposition of the urea-platinum solution by heating and drying of solvent (i.e. evaporation) provides better control over the size and dispersion of Pt nanoparticles (Pg. 133, left col.).
Thus, prior to the effective filing date of the claimed invention, it would have been obvious to one of ordinary skill in the art to heat the urea and platinum solution to remove the solvent in the method of Yu in order to provide better control over the size and dispersion of the deposited Pt nanoparticles, as taught by Song.
Claims 67-69 are rejected under 35 U.S.C. 103 as being unpatentable over Yu (US20110065025; cited in IDS dated 05/01/2024).
Regarding claim 67, Yu teaches a method of preparing a platinum/support catalyst that comprises preparing a dispersion solution including urea, a support, and a water-soluble metal having catalytic activity and reacting to deposit the metal particles on the support (Abstract). Yu teaches the reaction of urea and platinum compounds produces platinum complexes that are adsorbed on the carbon support ([0066]-[0067]). Yu teaches in the adsorption step, additional metals can be included, selected from a group consisting of platinum (Pt), ruthenium (Ru), rhodium (Rh), molybdenum (Mo), osmium (Os), iridium (Ir), rhenium (Re), palladium (Pd), vanadium (V), tungsten (W), cobalt (Co), iron (Fe), selenium (Se), nickel (Ni), bismuth (Bi), tin (Sn), chromium (Cr), titanium (Ti), gold (Au), cerium (Ce) and copper (Cu) ([0097]). The instant invention describes platinum group metals as including platinum, palladium, rhodium, iridium, ruthenium, and osmium (see Pg. 2, lines 1-9 of the specification).
Accordingly, Yu teaching urea forms complexes with platinum would reasonably suggest to a skilled artisan that “coordination complexes containing a platinum group metal as the central ion and at least one molecule of urea or urea derivative as ligand(s)” would be formed in the process of Yu. This conclusion is further supported by Yu teaching urea interacts with the platinum species to provide platinum complex species with a smaller size than platinum particles lacking urea ([0082]), clearly teaching an interaction between urea and platinum that is understood to be a coordination (i.e. bonding) interaction.
Yu further teaches the platinum complexes are reacted at high temperature to deposit metal hydroxide species on the support (Abstract; [0006]; [0013]; [0019]).
Regarding claim 68, Yu teaches the process of claim 67.
Yu teaches a method of preparing a platinum/support catalyst that comprises preparing a dispersion solution including urea, a support, and a water-soluble metal having catalytic activity (Abstract). Yu teaches the reaction of urea and platinum compounds produces platinum complexes that are adsorbed on the carbon support ([0066]-[0067]). Yu teaches in the adsorption step, additional metals can be included in the reaction with urea, selected from a group consisting of platinum (Pt), ruthenium (Ru), rhodium (Rh), molybdenum (Mo), osmium (Os), iridium (Ir), rhenium (Re), palladium (Pd), vanadium (V), tungsten (W), cobalt (Co), iron (Fe), selenium (Se), nickel (Ni), bismuth (Bi), tin (Sn), chromium (Cr), titanium (Ti), gold (Au), cerium (Ce) and copper (Cu) ([0097]). The instant invention describes platinum group metals as including platinum, palladium, rhodium, iridium, ruthenium, and osmium (see Pg. 2, lines 1-9 of the specification).
Regarding claim 69, Yu teaches the process of claim 68.
Yu teaches a method of preparing a platinum/support catalyst that comprises preparing a dispersion solution including urea, a carbon support, and a water-soluble metal having catalytic activity (Abstract; [0067]). Yu teaches the reaction of urea and platinum compounds produces platinum complexes that are adsorbed on the carbon support ([0066]-[0067]). Yu teaches in the adsorption step, additional metals can be included in the reaction with urea, selected from a group consisting of platinum (Pt), ruthenium (Ru), rhodium (Rh), molybdenum (Mo), osmium (Os), iridium (Ir), rhenium (Re), palladium (Pd), vanadium (V), tungsten (W), cobalt (Co), iron (Fe), selenium (Se), nickel (Ni), bismuth (Bi), tin (Sn), chromium (Cr), titanium (Ti), gold (Au), cerium (Ce) and copper (Cu) ([0097]). The instant invention describes platinum group metals as including platinum, palladium, rhodium, iridium, ruthenium, and osmium (see Pg. 2, lines 1-9 of the specification).
Accordingly, Yu teaching urea forms complexes with platinum and/or platinum group metals, would reasonably suggest to a skilled artisan that coordination complexes containing a platinum group metal as the central ion and at least one molecule of urea or urea derivative as ligand would be formed in the process of Yu. This conclusion is further supported by Yu teaching urea interacts with the platinum species to provide platinum complex species with a smaller size than platinum particles lacking urea ([0082]), clearly teaching an interaction between urea and platinum that is understood to be a coordination (i.e. bonding) interaction.
Conclusion
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/JORDAN W TAYLOR/Examiner, Art Unit 1738
/SALLY A MERKLING/SPE, Art Unit 1738
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