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USRE33149E Expired / Lapsed US ⏱️ 0.0 years remaining

Finely particulated colloidal platinum compound and sol for producing the same and method of preparation of fuel cell electrodes and the like employing the same

Assignee: Prototech Inc
•
Filing: 1981-12-28
•
Granted: 1990-01-16
•
Expires: 2001-12-28
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Abstract

Abstract This disclosure deals with novel very fine, particulated colloidal platinum of the 15-25 Angstrom size range of unusual catalytic activity and particularly adapted for adsorption or other deposition upon carbon for use as fuel cell catalytic electrodes and the like and produced from platinum colloids and sols including complex platinum sulfite compounds and sols derived therefrom.

Inventors

  • 👤 Henry G. Petrow
  • 👤 Robert J. Allen

Bibliographic Details

Application Number —
Jurisdiction US
Data Source google_patents
Last Synchronized 2026-10-28 01:16
CPC Classifications
H; H01; H01M; H01M4/00; H01M4/86; H01M4/90; H01M4/92; B; B01; B01J; B01J13/00; B01J13/0004; B01J13/0043; B01J23/00; B01J23/38; B01J23/40; B01J23/42; C; C01; C01G; C01G55/00; H01M4/925; H01M4/926; H01M2004/8678; H01M2004/8689; H01M2300/00; H01M2300/0002; H01M2300/0005; H01M2300/0008; Y; Y02; Y02E; Y02E60/00; Y02E60/30; Y02E60/50

Claims Analysis

Total Claims: 44
Claim 1
Independent Claim 67 words
In a fuel cell.[.and the like.]., a catalytic electrode comprising an electrically conductive high surface area .Iadd.carbon .Iaddend.substrate on which has been deposited platinum particles of the order of substantially 15 to 25 Angstroms in particle size and in which said particles are formed from .[.one of.]. an oxidative decomposition of a platinum .Iadd.sulfite .Iaddend.complex comprising an oxidizable ligand.[., and hydrolysis of a non-complex platinum salt solution.]..
Claim 2
Dependent Claim 67 words
In a fuel cell.[.and the like.]., a catalytic electrode comprising an electrically conductive high surface area .Iadd.carbon .Iaddend.substrate on which has been deposited platinum particles of the order of substantially 15 to 25 Angstroms in particle size and in which said particles are formed from .[.one of.]. an oxidative decomposition of a platinum .Iadd.sulfite .Iaddend.complex comprising an oxidizable ligand.[., and hydrolysis of a non-complex platinum salt solution.]..
Claim 3
Dependent Claim 38 words
In a fuel cell .[.and the like.]., a catalytic electrode as claimed in .Iadd.claim .Iaddend.1 and in which the platinum loads the electrode surface in the range of from substantially 0.04 milligrams/cm 2 to 0.5 milligrams/cm 2 .
Claim 4
Dependent Claim 88 words
In a fuel cell .[.and the like.]., a catalytic electrode comprising an electrically-conducting high surface area carbon substrate on which has been deposited substantially uniformly platinum particles having a particle size substantially in the range of 15 to 25 Angstroms and being formed from the oxidative decomposition of a platinum .Iadd.sulfite .Iaddend.complex comprising an oxidizable ligand. .[.4. In a fuel cell and the like, a catalytic electrode as claimed as in claim 3 and in which said complex is selected from the group consisting of platinum sulfite and
Claim 5
Dependent Claim 31 words
platinum nitrite complexes..]. 5. In a fuel cell .[.and the like.]., a catalytic electrode as claimed in claim .[.4.]. .Iadd.3 .Iaddend.and in which said particles are reduced subsequent to said oxidative
Claim 6
Dependent Claim 34 words
decomposition. 6. In a fuel cell .[.and the like.]., a catalytic electrode as claimed in claim .[.4.]. .Iadd.3 .Iaddend.and in which the platinum loads the electrode surface in the range of from substantially 0.04
Claim 7
Dependent Claim 46 words
milligrams/cm 2 to 0.5 milligrams/cm 2 . 7. In a fuel cell .[.and the like.]., a catalytic electrode as claimed in claim .[.4.]. .Iadd.3 .Iaddend.and in which said platinum sulfite complex is the compound having the composition corresponding substantially to H 3 Pt(SO 3 ) 2
Claim 8
Dependent Claim 107 words
OH. 8. A fuel cell comprising a catalytic electrode having an electrically-conducting high surface area carbon substrate on which has been deposited substantially uniformly platinum particles having a particle size substantially in the range of 15 to 25 Angstroms and formed from the oxidative decomposition of a platinum .Iadd.sulfite .Iaddend.complex comprising an oxidizable ligand, .[.said complex being selected from the group consisting of platinum sulfite and platinum nitrite complexes.]. and said particles being reduced subsequent to said oxidative decomposition, said fuel cell being a phosphoric acid electrolyte fuel cell with air-hydrogen electrode supply means, and said electrode being provided with means for enabling the drawing of current
Claim 9
Dependent Claim 107 words
OH. 8. A fuel cell comprising a catalytic electrode having an electrically-conducting high surface area carbon substrate on which has been deposited substantially uniformly platinum particles having a particle size substantially in the range of 15 to 25 Angstroms and formed from the oxidative decomposition of a platinum .Iadd.sulfite .Iaddend.complex comprising an oxidizable ligand, .[.said complex being selected from the group consisting of platinum sulfite and platinum nitrite complexes.]. and said particles being reduced subsequent to said oxidative decomposition, said fuel cell being a phosphoric acid electrolyte fuel cell with air-hydrogen electrode supply means, and said electrode being provided with means for enabling the drawing of current
Claim 10
Dependent Claim 37 words
flowing through the cell. 9. A fuel cell as claimed in claim 8 and in which said electrode is a catalytic anode, and in which said air-hydrogen electrode supply means comprise a source of hydrogen containing carbon
Claim 11
Dependent Claim 25 words
monoxide impurity. 10. A fuel cell as claimed in claim 9 wherein said catalytic anode has a platinum loading in the range of from substantially
Claim 12
Dependent Claim 26 words
04 milligrams/cm 2 to 0.25 milligrams/cm 2 . 11. A fuel cell as claimed in claim 8 and in which the said carbon is composited with
Claim 13
Dependent Claim 77 words
fluorinated hydrocarbon polymer. 12. In the method of preparing electrodes for fuel cells .[.and the like.]. comprising platinum-on-carbon electro-catalyst, the steps of providing aqueous colloidal platinum-containing sol having an average platinum particle size substantially of the order of 15-25 Angstroms, depositing said platinum contained in said sol on an electrically-conducting carbon substrate, and controlling the depositing to cause the carbon to nucleate the deposit and limit the formation of platinum particles on said carbon to said size.
Claim 14
Dependent Claim 77 words
fluorinated hydrocarbon polymer. 12. In the method of preparing electrodes for fuel cells .[.and the like.]. comprising platinum-on-carbon electro-catalyst, the steps of providing aqueous colloidal platinum-containing sol having an average platinum particle size substantially of the order of 15-25 Angstroms, depositing said platinum contained in said sol on an electrically-conducting carbon substrate, and controlling the depositing to cause the carbon to nucleate the deposit and limit the formation of platinum particles on said carbon to said size.
Claim 15
Dependent Claim 96 words
In a fuel cell .[.and the like.]., an electrode comprising a platinum-on-carbon electrocatalyst, said electrode being produced by a process including the steps of oxidizing the ligand of a complex platinum .Iadd.sulfite .Iaddend.compound comprising an oxidizable ligand to substantially non-complexing products by means of a non-complexing oxidant, producing therefrom an aqueous dispersion comprising the products of said oxidation, depositing the platinum compound contained in said dispersion on an electrically conducting carbon substrate, and decomposing said platinum compound thereon, thereby forming platinum particles on said carbon having an average particle size of the order of substantially 15-25
Claim 16
Dependent Claim 96 words
In a fuel cell .[.and the like.]., an electrode comprising a platinum-on-carbon electrocatalyst, said electrode being produced by a process including the steps of oxidizing the ligand of a complex platinum .Iadd.sulfite .Iaddend.compound comprising an oxidizable ligand to substantially non-complexing products by means of a non-complexing oxidant, producing therefrom an aqueous dispersion comprising the products of said oxidation, depositing the platinum compound contained in said dispersion on an electrically conducting carbon substrate, and decomposing said platinum compound thereon, thereby forming platinum particles on said carbon having an average particle size of the order of substantially 15-25
Claim 17
Dependent Claim 34 words
Angstroms. 14. In a fuel cell .[.and the like.]., an electrode .[.produced by the process of.]. .Iadd.as claimed in .Iaddend.claim 13 wherein said complex platinum compound is .[.platinum sulfite and it is.]. subjected to
Claim 18
Dependent Claim 29 words
air oxidation. 15. In a fuel cell .[.and the like.]., an electrode .[.produced by the process of.]. .Iadd.as claimed in .Iaddend.claim 14 wherein said complex platinum sulfite .Iadd.compounds .Iaddend.contains
Claim 19
Dependent Claim 39 words
groups of (OH) and H 3 Pt(SO 3 ) 2 . 16. In a fuel cell .[.and the like.]., an electrode .[.produced by the process of.]. .Iadd.as claimed in .Iaddend.claim 14 wherein said air oxidation is carried out at
Claim 20
Dependent Claim 44 words
about 135° C. 17. In a fuel cell .[.and the like.]., an electrode .[.produced by the process of.]. .Iadd.as claimed in .Iaddend.claim 13 wherein said dispersion contains the product of said complex platinum sulfite and a non-complexing oxidant, said oxidation being carried out in
Claim 21
Dependent Claim 33 words
said dispersion. 18. In a fuel cell .[.and the like.]., an electrode .[.produced by the process of.]. .Iadd.as claimed in .Iaddend.claim 17 wherein said oxidant is selected from the group consisting of hydrogen
Claim 22
Dependent Claim 58 words
peroxide, potassium permanganate and persulfuric acid. 19. In a fuel cell .[.and the like.]., an electrode .[.produced by the process of.]. .Iadd.as claimed in .Iaddend.claim 17 wherein said complex platinum sulfite is selected from the group of compounds having substantially the composition of Na 6 Pt(SO 3 ) 4 and H 3 Pt(SO 3 ) 2 OH and
Claim 23
Dependent Claim 46 words
mixtures thereof. 20. In a fuel cell .[.and the like.]., an electrode .[.produced by the process of.]. .Iadd.as claimed in .Iaddend.claim 17 wherein said complex platinum sulfite is the compound having the composition of Na 6 Pt(SO 3 ) 4 and wherein said compound is in
Claim 24
Dependent Claim 36 words
an aqueous sulfuric acid solution. 21. In a fuel cell .[.and the like.]., an electrode .[.produced by the process of.]. .Iadd.as claimed in .Iaddend.claim 19 wherein said oxidation is effected with H 2 H 2 .
Claim 25
Dependent Claim 35 words
In a fuel cell .[.and the like.]., an electrode .[.produced by the process of.]. .Iadd.as claimed in .Iaddend.claim 13 wherein said oxidation is carried out in the presence of said carbon substrate in finely divided
Claim 26
Dependent Claim 45 words
form. 23. In a fuel cell .[.and the like.]., an electrode .[.produced by the process of.]. .Iadd.as claimed in .Iaddend.claim 13 wherein said complex platinum compound is formed in said dispersion by reacting a solution of chloroplatinic acid .[.and the like.]. with a sulfiting agent.
Claim 27
Dependent Claim 33 words
In a fuel cell .[.and the like.]., an electrode .[.produced by the process of.]. .Iadd.as claimed in .Iaddend.claim 23 wherein aid oxidation is effected thermally in air, and said decomposing following depositing on
Claim 28
Dependent Claim 70 words
the carbon is effected by reducing the same. 25. In a fuel cell .[.and the like.]., a catalytic electrode comprising an electrically conductive high surface area carbon substrate on which has been deposited platinum particles of the order of substantially 15 to 25 Angstroms in particle size and in which said platinum loads the electrode surface in the range of from substantially 0.04 milligrams/cm 2 to 0.5 milligrams/cm 2 .
Claim 29
Dependent Claim 70 words
the carbon is effected by reducing the same. 25. In a fuel cell .[.and the like.]., a catalytic electrode comprising an electrically conductive high surface area carbon substrate on which has been deposited platinum particles of the order of substantially 15 to 25 Angstroms in particle size and in which said platinum loads the electrode surface in the range of from substantially 0.04 milligrams/cm 2 to 0.5 milligrams/cm 2 .
Claim 30
Dependent Claim 87 words
A fuel cell comprising a catalytic cathode electrode having an electrically conductive high surface area carbon substrate on which has been deposited platinum particles substantially of the order of 15 to 25 Angstroms in particle size, said electrode having an electrode surface platinum loading within the range of from substantially 0.04 milligrams/cm 2 to 0.5 milligrams/cm 2 , said fuel cell being an air-hydrogen high temperature fuel cell with a phosphoric acid electrolyte and being capable of producing in excess of 100 Amperes per square foot of
Claim 31
Dependent Claim 87 words
A fuel cell comprising a catalytic cathode electrode having an electrically conductive high surface area carbon substrate on which has been deposited platinum particles substantially of the order of 15 to 25 Angstroms in particle size, said electrode having an electrode surface platinum loading within the range of from substantially 0.04 milligrams/cm 2 to 0.5 milligrams/cm 2 , said fuel cell being an air-hydrogen high temperature fuel cell with a phosphoric acid electrolyte and being capable of producing in excess of 100 Amperes per square foot of
Claim 32
Dependent Claim 30 words
electrode area at a cell voltage of at least 0.5 volts. 27. A fuel cell as claimed in claim 26 and in which the platinized carbon is admixed with a
Claim 33
Dependent Claim 98 words
fluorinated hydrocarbon polymer. 28. A fuel cell comprising a catalytic anode electrode having an electrically conductive high surface area carbon substrate on which has ben deposited platinum particles substantially of the order of 15 to 25 Angstroms in particle size, said electrode having an electrode surface platinum loading within the range of from substantially 0.04 milligrams/cm 2 to 0.5 milligrams/cm 2 , said fuel cell being an air-hydrogen high temperature fuel cell with a phosphoric acid electrolyte, said hydrogen comprising carbon monoxide impurity, and said fuel cell being capable of producing in excess of 100 Amperes per square
Claim 34
Dependent Claim 98 words
fluorinated hydrocarbon polymer. 28. A fuel cell comprising a catalytic anode electrode having an electrically conductive high surface area carbon substrate on which has ben deposited platinum particles substantially of the order of 15 to 25 Angstroms in particle size, said electrode having an electrode surface platinum loading within the range of from substantially 0.04 milligrams/cm 2 to 0.5 milligrams/cm 2 , said fuel cell being an air-hydrogen high temperature fuel cell with a phosphoric acid electrolyte, said hydrogen comprising carbon monoxide impurity, and said fuel cell being capable of producing in excess of 100 Amperes per square
Claim 35
Dependent Claim 30 words
foot of electrode area at a cell voltage of at least 0.5 volts. 29. A fuel cell as claimed in claim 28 and in which the platinized carbon is admixed
Claim 36
Dependent Claim 90 words
with a fluorinated hydrocarbon polymer. 30. A fuel cell as claimed in claim 28, and in which said fuel cell comprises a catalytic cathode having an electrically conductive high surface area carbon substrate on which substrate has been deposited platinum particles substantially of the order of 15 to 25 Angstroms in particle size, the platinum loading of the cathode surface being within the range of from substantially 0.04 milligrams/cm 2 to 0.5 milligrams/cm 2 , said fuel cell having connected thereto fuel and oxidant supply means and means for enabling
Claim 37
Dependent Claim 35 words
drawing current through the cell. 31. A fuel cell as claimed in claim 26 and in which means is provided for operating said cathode electrode at a temperature of from substantially 135° to substantially 190°
Claim 38
Dependent Claim 27 words
C. 32. A fuel cell as claimed in claim 28 and in which means is provided for operating said anode electrode at a temperature of from substantially
Claim 39
Dependent Claim 65 words
170° to substantially 190° C. 33. A fuel cell comprising a catalytic electrode having an electrically conductive high surface area carbon substrate on which has been deposited platinum particles of the order of substantially 15 to 25 Angstroms in particle size and formed from a complex platinum sulfite .[.selected from the group of compounds.]. having substantially the composition of Na 6 (Pt(SO 3 ) 4
Claim 40
Dependent Claim 65 words
170° to substantially 190° C. 33. A fuel cell comprising a catalytic electrode having an electrically conductive high surface area carbon substrate on which has been deposited platinum particles of the order of substantially 15 to 25 Angstroms in particle size and formed from a complex platinum sulfite .[.selected from the group of compounds.]. having substantially the composition of Na 6 (Pt(SO 3 ) 4
Claim 41
Dependent Claim 49 words
.[.and H 3 Pt(SO 3 ) 2 OH and mixtures thereof,.]..Iadd.. 34. A fuel cell as claimed in claim 33 and in which said fuel cell comprises an additional electrode, an electrolyte, fuel and oxidant supply means, and means for enabling the drawing of current flowing through the cell.
Claim 42
Dependent Claim 104 words
.Iadd. 5. A fuel cell comprising a catalytic electrode having an electrically conductive high surface area carbon substrate on which has been deposited platinum particles of the order of substantially 15 to 25 Angstroms in particle size, with the average particle size being in that range, and formed from a complex platinum sulfite having substantially the composition of H 3 Pt(SO 3 ) 2 OH. .Iaddend. .Iadd.36. A fuel cell as claimed in claim 35 and in which said fuel cell comprises an additional electrode, an electrolyte, fuel and oxidant supply means, and means for enabling the drawing of current flowing through the cell.
Claim 43
Dependent Claim 39 words
.Iaddend. .Iadd.37. A catalyst electrode in accordance with claim 25, wherein the platinum particles are adsorbed on the inherently porous carbon substrate. .Iaddend. .Iadd.38. A catalytic electrode in accordance with claim 25, wherein the substrate comprises carbon black. .Iaddend.
Claim 44
Dependent Claim 20 words
.Iadd.39. A catalytic electrode in accordance with claim 38, wherein the platinum particles are adsorbed on the carbon black. .Iaddend.

USPTO Annuity & Maintenance Windows

Annuity Stage Window Opens Payment Deadline Surcharge Period Until Estimated Fee Status
3.5 Years (Year 4) 1993-01-15 1993-07-17 1994-01-16 $2000.00 Window Closed / Lapsed
7.5 Years (Year 8) 1997-01-15 1997-07-17 1998-01-16 $3760.00 Window Closed / Lapsed
11.5 Years (Year 12) 2001-01-15 2001-07-17 2002-01-16 $7700.00 Window Closed / Lapsed

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