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United States Patent to 11, 3,996,141 Updike 45 Dec United States Patent to 11, 3,996,141 Updike 45 Dec. 7, 1976 54 DALYSIS MEMBRANE 2,971,850 2/1961 Barton ............................. 195/63 X 3, 158,532 11/1964 Pall et al. ... ... 210/503 X 75 Inventor: Stuart J. Updike, Madison, Wis. 3,282,702 1 1/1966 Schreiner ........................ 195/63 X (73) Assignee: Wisconsin Alumni Research 3,327,859 6/1967 Pall .............. ........ 210/266 3,526,481 9/1970 Rubricius ........... ... 210/321 X Foundation, Madison, Wis. 3,766,013 10/1973 Forgione et al. .................... 195/63 22) Filed: Jan. 17, 1974 3,809,613 5/1974 Vieth et al. ...................... 195/68 X 3,824, 150 7/1974 Lilly et al. ... ... 195/DIG. l l X 21 ) Appl. No.: 434,231 3,846,236 1 1/1974 Updike ......................... 23/258.5 X Related U.S. Application Data Primary Examiner-Frank A. Spear, Jr. (63) Continuation-in-part of Ser. No. 191,720, Oct. 22, Attorney, Agent, or Firm-McDougall, Hersh & Scott 1971, Pat. No. 3,846,236. 57 ABSTRACT 52 U.S. Cl. ................................ 210/501; 427/245 (51) Int. Cl. ......................................... B01D 13/04 A semi-permeable membrane containing a catalyst for 58 Field of Search .............. 210/22, 23, 321,500, conversion of hydrogen peroxide introduced from one side of the semi-permeable membrane to molecular 210/501, 502; 23/258.5; 195/18, 63; oxygen which is released from the opposite side of the 106/194; 264/41, 49; 427/245 semi-permeable membrane. The catalyst is preferably 56) References Cited in the form of a ruthenium oxide or sulfide and prefer UNITED STATES PATENTS ably in assymetrical distribution in the membrane. 2008, 131 7/1935 Dieck et al. ................... 210/501 X 2,283,883 5/1942 Conconi et al. ................... 210/5O1 11 Claims, No Drawings 3,996, 141 1 2 molecular oxygen available to the blood on the oppo DALYSIS MEMBRANE site side of the membrane. Conversion of hydrogen peroxide to molecular oxy The invention described herein was made in the gen and water occurs in accordance with the following course of work under a grant or award from the De equation: partment of Health, Education, and Welfare. A con 2HO, -) + 2HO tinuation-in-part application of my copending applica tion Ser. No. 191,720, filed Oct. 22, 1971, and entitled Thus 2 millimoles of hydrogen peroxide convert to 1 “METHOD AND APPARATUS FOR DIALYSIS', millimole of molecular oxygen. Actual measurement of now U.S. Pat. No. 3,846,236. 10 the amount of oxygen released from a 0.5% solution of This application relates to the supply of oxygen to the hydrogen peroxide on the opposite side of permeable blood, or other body or chemical fluid, from hydrogen membrane containing MnO, as a conversion catalyst, peroxide via a dialysis membrane, and relates more was 260 to 450 milliliters per minute per square meter. particularly to a catalyst containing dialysis membrane This is sufficient to provide the basal oxygen require for use in same. 15 ment for a man of ordinary weight and with a mem In the aforementioned parent application, descrip brane of reasonable dimension for practical use in a tion is made of a method and apparatus for the supply respiratory device. of oxygen by conversion of hydrogen peroxide during The oxygen converted from dilute hydrogen peroxide passage through a semipermeable membrane from a solution via a catalyst containing a semipermeable dilute solution of hydrogen on one side of the mem 20 membrane, is made available uniformly over substan brane to a fluid on the opposite side of the membrane. tially the entire area of the semipermeable membrane Since the invention has primary application to the sup for release at a rate sufficient to meet basal oxygen ply of oxygen to the blood, bypassed from the human requirements, but without making oxygen available at system, at rates sufficient to maintain life, the invention such high concentrations at any one point as would will be described with reference thereto, but it will be 25 raise problems of oxygen bubble embolism toxicity. understood, as described in the aforementioned appli As the semipermeable membrane, use can be made cation, that the concepts find use in other procedures of a water insoluble, water wettable cellulose deriva wherein it is desired to make molecular oxygen avail tive, such as cellophane, cellulose acetate, cellulose able at controlled rates and in amounts suitable for use propionate, carboxyethyl cellulose, and the like; insolu in other medical applications or chemical operations, 30 bilized gelatin; partially hydrolized polyvinyl acetate; such as in various oxygenation or oxygen chlorination polyionic film forming compositions such as polysul processes. fonated anionic polymers or ionically linked polyca Attempts have previously been made to diffuse mo tionic polymers, such as marketed by Amicon Com lecular oxygen directly through a semipermeable mem pany. Use can also be made of dialysis membranes brane for passage into an extra-corporeal bypassed 35 formed of multiple hollow fibers, such as marketed by stream of human blood in contact with the opposite the Dow Chemical Company, or hydrophobic mem side of the dialysis membrane. This technique has not branes, such as formed of organosilicon rubbers. found acceptance because the rate of diffusion of mo In the practice of the invention, it is important to lecular oxygen through a wettable semipermeable make use of a conversion catalyst that does not wash membrane is so slow as to require a diffusion area so 40 out of the membrane under acid, neutral, or alkaline large as to make it impractical for use in a respiratory conditions so that the semipermeable membrane will device. remain effective over long periods of continuous use Considerable effort has been expended in another under the widely varying conditions to which it is ex direction of approach, addressed to the supply of oxy posed in dialysis. Another characteristic of the catalyst, gen by direct introduction of hydrogen peroxide into 45 in order to achieve the desired utility, over long periods the blood-stream, preferably in controlled amounts, as of use, is the freedom of the catalyst from poisoning by by diffusion through a semipermeable or dialysis mem components present in the fluids to which it is exposed, brane, as described in the Rubricius U.S. Pat. No. or which in turn does not contribute any undesirable 3,526,481. In this approach, reliance is had upon the components into the bloodstream. enzyme catalase in the blood to convert the hydrogen 50 Another factor, which should be taken into consider peroxide into molecular oxygen and water. This proce ation, in defining a catalyst containing permeable mem dure utilizes the catalase activity normally in the blood, brane, suitable for use in the practice of this invention, and which can be supplemented by injection of highly is the ability to effect substantially complete conversion purified exogenous catalase to break down hydrogen of the hydrogen peroxide before passage through the peroxide. However, this technique has been rejected 55 semipermeable membrane so that practically no hydro because the conversion rate in the blood plasma is so gen peroxide will break through the membrane and be rapid as to generate oxygen gas bubbles which embol introduced into the bloodstream. ize and can fatally plug the micro-circulation of the These characteristics are generally derived from the lung. use of an inorganic catalyst. Manganese dioxide has It has been found, in accordance with the invention 50 been described in the aforementioned parent applica described in the aforementioned application, that hy tion as a preferred catalyst which can be incorporated drogen peroxide, in dilute solution, can be used to into the dialysis membrane in accordance with the make molecular oxygen available at a rate sufficient to following example: supply venous blood with its requirement to sustain life, when use is made of a dialysis membrane which con 65 EXAMPLE I tains a catalyst for conversion of the hydrogen peroxide An untreated cellophane membrane, of the type pre to molecular oxygen during diffusion from dilute solu viously described as being used in artificial kidney dial tion on one side of the wettable membrane to make ysis, is first hydrated in water and then simultaneously 3,996,141 3 4. exposed on one side to a 0.3 molar potassium perman ganate solution, and on the opposite side, to a 0.1 EXAMPLE II molar sodium iodide solution for one minute. Diffusion An untreated cellophane membrane of the type de of the two solutions from opposite sides into the mem scribed in Example I is first hydrated in water and then brane brings about the precipitation of manganese simultaneously exposed on one side to a 0.25 M. solu dioxide in the interior of the dialysis membrane. This tion of ruthenium chloride (103) and on the opposite gives the membrane a homogeneous translucent amber side to a 0.1 M. sodium hydroxide solution. Diffusion of pigmentation. Instead of making use of sodium iodide the two solutions from opposite sides to the membrane for precipitation of MnO, from the permanganate, brings about precipitation within the membrane of O ruthenium oxide or its hydrated form. The solutions are other alkali metal iodides or similar reducing agents then rinsed from the membrane, leaving the membrane can be employed. Similarly, other water soluble per with its insoluble precipitate of ruthenium oxide sub manganates, such as sodium permanganate, ammo stantially uniformly distributed therethrough. nium permanganate, and the like can be used instead of potassium permanganate. For good diffusion at a uni 15 EXAMPLE III form rate, it is desirable to make use of a dialysis mem The procedure of Example II is followed but instead brane, in the form of a semipermeable membrane of sodium hydroxide solution, the membrane is ex formed of materials that are wet by the fluids disposed posed to a solution of sodium sulfide whereby the pre on both sides of the membrane.
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