Method of producing thin palladium-copper and the like,...

Gas separation: apparatus – Apparatus for selective diffusion of gases – Plural layers

Reexamination Certificate

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C095S056000, C427S437000, C428S607000, C428S670000

Reexamination Certificate

active

06238465

ABSTRACT:

BACKGROUND
The present invention relates to thin hydrogen-selective palladium-alloy membranes and the like and to novel methods of preparing the same; being more particularly directed to such alloys produced by novel solid-solid interdiffusion of pressure-contacting films or layers of palladium metal with palladium-enhancing metals, such as copper and silver and the like.
This application is based in part upon the discovery disclosed in our U.S. patent application Ser. No. 880,990, now U.S. Pat. No. 5,904,754 in which an assembly of a palladium/copper (60%:40% by weight) alloy foil is edge-area diffusion-bonded to a copper-surfaced metallic frame. The advantages of such hydrogen-selective Pd/Cu alloy membranes have been cited in this application which is incorporated herein by reference.
Commonly, thin 60% Pd/40% Cu foil membranes are made from billets which are solidified melts of the two metals in uniform admixture. Starting with the billet, thinning involves an elaborate and expensive sequence of steps of rolling and annealing, with the cost increasing disproportionately as the practical low thickness limit of about 0.001 inch of a pinhole-free foil is reached. Similarly, other hydrogen-selective palladium alloy foils are generally made from alloy billets. These include in particular the well known silver/palladium alloy containing 23-25% silver (herein Pd/23-25% Ag). In general, to form a suitable palladium bearing membrane, palladium is alloyed with one (and sometimes more than one) stability- and/or permeability-enhancing metal, as shown, for example, in the publication entitled “Hyperpure Hydrogen From Palladium Alloy Membrane Permeation”, by R. Goto,
Chemical Economy and Engineering Review
(Japan), 2(10), pp 44-50 (1970), also included herein by reference.
We have now found that the edge-area intermetallic diffusion-bonding technique of said copending application can be extended to the generation of, preferably, thin palladium/copper and the like selected alloy foils, including the above-referred silver/palladium alloy. The method is especially advantageous in producing less than about 25 micrometer (ca. 0.001″) thick membranes. Here the thinner the better for intermetallic diffusion, in contrast to the limitation of excessive costs of thin sheet rolling from billets.
The prior art in this field has been oriented toward determining intermetallic diffusion constants for Pd/Cu and Pd/Ag binary, thin film systems. Intermetallic diffusion of Pd/Ag layers has been discussed in “Interdiffusion studies in silver/palladium couples by means of Auger depth profiling”, by Bukaluk and Rozwadowski in Vacuum 46(5/6), pp 579-582 (1995) and in “Interdiffusivities in silver-palladium composition-modulated foils”, by Henein and Hilliard in
Journal of Applied Physics
55(8), pp 2895-2900 (1984). The Pd/Cu system has been likewise investigated in “Diffusion and Size Effect in Thin Films of the Systems Cu-Pd and Cu-Ag”, by Grebennik and Zyman in
Fiz. metal metalloved.
(Russian), 32(4), pp 891-893 (1971), and in “Study of interdiffusion in Pd/Cu multilayered films by Auger depth profiling”, by Jeon, et. al.,
Journal of Applied Physics,
75(12), pp 7825-7828 (1994). While these studies attempt to understand the fundamentals of the intermetallic diffusion process they do not disclose methods for fabricating thin foils for use as hydrogen separation membranes.
In accordance with the present invention, an improved technique and method of fabricating hydrogen-selective alloy membranes by a novel intermetallic solid-metal interdiffusion process is now provided, producing also improved stability and/or enhanced hydrogen permeability in the resulting alloy membranes.
OBJECTS OF INVENTION
An object of the invention, accordingly, is to provide a new and improved method of producing thin hydrogen-selective palladium-alloy membranes and the like that shall not be subject to the above discussed and other limitations of the prior art; but, to the contrary, through a novel interdiffusion of physically contacting thin palladium and copper or other palladium-enhancing metal films or layers at elevated temperatures in the presence of a reducing agent, provides significant improvements in fabrication facility, cost and performance, particularly for very thin films or layers.
A further object of this invention to produce, by interdiffusion of solid metals, a novel thin hydrogen-selective alloy membrane of palladium with, preferably, copper, or another interdiffusing metal that contributes stability and/or enhanced hydrogen-permeability to the membrane (referred to above as a “Palladium-enhancing metal”).
Other and further objects will be explained hereafter and are more particularly delineated in the appended claims.
SUMMARY
In summary, from one of its broader aspects, the invention embraces a method of producing a hydrogen-selective palladium-alloy membrane comprising the steps of physically contacting, as with pressure, a thin solid specimen of palladium metal with a thin solid specimen of a Pd-enhancing metal, preferably copper, and subjecting the same in the presence of a reducing agent, preferably hydrogen gas, to an elevated temperature below the melting point of both metals for a sufficient period of time to effect substantially complete solid-solid interdiffusion of said metals.
Preferred and best mode techniques and membrane compositions are later detailed.


REFERENCES:
patent: 3428476 (1969-02-01), Langley et al.
patent: 3439474 (1969-04-01), McKinley
patent: 3447288 (1969-06-01), Juda et al.
patent: 4589891 (1986-05-01), Iniotakis et al.
patent: 4655797 (1987-04-01), Iniotakis et al.
patent: 5139541 (1992-08-01), Edlund
patent: 5217506 (1993-06-01), Edlund et al.
patent: 5259870 (1993-11-01), Edlund
patent: 5393325 (1995-02-01), Edlund
patent: 5498278 (1996-03-01), Edlund
patent: 5738708 (1998-04-01), Peachey et al.
patent: 5904754 (1999-05-01), Juda et al.

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