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\.\F\ US 20030008210A1 (19) United States (12) Patent Application Publication (10) Pub. No.: US 2003/0008210 A1 Licht (43) Pub. Date: Jan. 9, 2003 (54) SILVER MAGANESE SALT CATHODES FOR (30) Foreign Application Priority Data ALKALINE BATTERIES Feb. 20, 2001 (IL) ............................................... .. 141527 (75) Inventor: Stuart Licht, Haifa (IL) Publication Classi?cation Correspondence Address; (51) Int. Cl.7 .......................... .. H01M 4/54; H01M 4/50; BROWDY AND NEIMARK, P.L.L.C. H01M 4/24; H01M 10/26; 624 NINTH STREET, NW H01M 10/32 SUITE 300 (52) US. Cl. ......................... .. 429/219; 429/224; 429/207 WASHINGTON, DC 20001-5303 (US) (57) ABSTRACT (73) Assignee; CHEMERGY, Energy Technologies, An electric storage alkaline battery comprising an electri Technion City (IL) cally neutral alkaline ionic conductor, an anode and a cathode, Whereby electric storage is accomplished via elec (21) Appl, No; 10/076,268 trochemical reduction of the cathode and oxidation of the anode, Whereby said cathode includes electrochemically (22) Filed: May 13, 2002 active silver (per)manganate materials. 1 O \.\f\_\ n e r___ m r<~——~—1 LOAD "-4 G V \\_/ I l ‘:3 m 0 I a r: m I Q .4 g; Reduced | *1 o o Cathode I Anode it" '1 D m m I H :8 l \' m I , 1 4 M V" ‘é f’ T\ wa , \e. 1 2 :5 l ‘n I g Cathode ; OXldlZed f3. 1 Anode (‘D I | Zi- ]\' 22__.. 1I l \ / N O Patent Application Publication Jan. 9, 2003 Sheet 4 0f 8 US 2003/0008210 A1 cOEwoQEoo20058 3.6%Qoi;@ 52688002658 359m0%;.0mm 4IOmZEOCSRZ /®/6262.665 Q,..5%? -nuI1u Es$9236é?E35.a28CNV€=8=m.32 //Q5:552x m90%v;m;0.?0.0Q0 $8589:2?552%5:5;6 55063cmmmEnumE '0 / l l 0.0 me we 0.0 0.0 v.0 m0 0.0 voEmE Sum ‘lellualod n80 Patent Application Publication Jan. 9, 2003 Sheet 5 0f 8 US 2003/0008210 A1 I I a LI H w=wowc=mi<<<<B556:?33cm:@920 93058“5:22Q0529.‘mzocm>mE~=::Lo wicoéwoaEouBEQEUwno?mon oweomgczgwsa 30%.5229‘o23 -4 @OcEmiém5:256.moswBwE3V363.822205Em?mmho VA, m6 No SIIOA ‘lenuawd n90 mSmEm Patent Application Publication Jan. 9, 2003 Sheet 6 0f 8 US 2003/0008210 Al m; - “Emmnocm:N96i8<<<6583EQESQEOQ:mc 10!Ew25%5$552:8XE251:8E 09mdw.ov.0No 65$?<<<EGEEEOQ 55463cmmmzmsu?o -d_-. coEwo285mmE00 552gO93 191$?0“Sim/$08 0.9 NAN @N m; w.” m; wd @d v.0 NO A ‘leuualod n80 @230Ev Patent Application Publication Jan. 9, 2003 Sheet 7 0f 8 US 2003/0008210 A1 1 ' ' ' I Y v v | I I Various AgO composite cathodes discharged in Zn anode alkaline cells at high rate (2.8Q): 1 . Con?guration: AAA cell, cathode mix contains: 1 Z, 9wt% graphite & 18m KOH. 0.8 - aI We Kmno“I A 55%K2Mn04t0 45%Ag0 I ‘We KMHO“ El 55%KMnO4 to 45%AgO A 55%K2Mn04 lo 45%AgO 1 A A 67%K2MnO4 i0 33%AgO J >'_ b ‘ A 86%K2MnO4to14‘Z/oAgO E . *" 1 2 * r:m 7S\ H O a 0-8 l E U U4 * A pure KPMnOa O 50%BaMnO4 lo 50%Ag0 1' 6 ' 55%BaMnO4to 45%Ag0 _ ‘ ‘ ’ O 67%BaMnO4 lo 33%Ag0 1.2 - C34 . Dure BaMnOA C‘ l 1 - l I l 1 L 1 l n l O 0.2 0.4 0.6 0.8 1.0 1.2 Discharge Energy, Wh Figure 7 Patent Application Publication Jan. 9, 2003 Sheet 8 0f 8 US 2003/0008210 Al @N M60muocmCMnewEQESQEQQ=858<<<6583 IOxw2.5980m:wEmEoo5E$35wnoémoE -__Px>vrIrI démém<<<EBEEEOU mm0Nwe0.?m._.w;0.0#0m0 c>>055cmmmhmcuwmc 692352.30a2“2.8@5255225 mmuo?muwommmmhwocémd‘U928"65204*0ucmcozmi?m - 0.0 0.? 0.0 0.0 m0 A klellualod H9O 930K0 US 2003/0008210 A1 Jan. 9, 2003 SILVER MAGANESE SALT CATHODES FOR 1371]. In principle, this silver (per)manganate, AgMnO4, ALKALINE BATTERIES represent a substantial cathodic charge source for electrochemical storage, but [0001] The present invention relates to electric storage high rate charge transfer has been ine?icient. Independent of Whether batteries. More particularly, the invention relates to a novel AgMnO4 is described as silver permanganate, Ag(I)Mn(VII)O4, or silver alkaline electric storage battery With a cathode formed from peroximanganate, Ag(II)Mn(VI)O4, or as a mixed intermediate valence, Where O<x<1) for Ag(I+x)Mn(VII—x)O4, AgMnO4, can in principal provide a silver manganese compound. a higher cathodic charge capacity than other permanganate or manganate salts. In addition to the manganese reduction, AgMnO4 permits the alkaline BACKGROUND OF THE INVENTION reduction, as Ag(I) (or if Ag(MnO4)2 had been used as Ag(II)) in the same [0002] MnO2 is the common active cathode material in potential domain, and exempli?ed by the silver oxide reductions: primary alkaline batteries. As an alternative to MnO2, a variety of permanganate compounds have been considered for cathode materials due to their high oxidation state Which, in principle permits signi?cant storage and release of elec [0009] Hence, independent of the Ag(I)/Mn(VII) or trical charge. HoWever, as described by J. Epstein and C. C. Ag(II)/Mn(VI) starting point, the alkaline cathodic reduction Liang, US. Pat. No. 3,799,959 (Oct. 12, 1971), most per AgMnO4 is consistent With an overall 5 electron reduction to manganates salts are overly soluble in alkaline solution and Ag(0) and Mn(III) at thermodynamically potential, this solubility can be destructive to the battery performance. E§0.35V vs SHE, for example as: In addition, most permanganate salts do not discharge effec tively in the solid phase, although as described by S. Licht E;0.35v vs SHE (7) and C. Marsh, US. Pat. No. 5,549,991, (Aug. 27, 1996), in [0010] It is an object of the present invention to provide an the solution phase they can support high currents. additive to the cathode in alkaline batteries Which provides a practical storage capacity greater than the capacity knoWn [0003] Compared to the manganese dioxide alkaline cath for conventional cathode materials. A novel electrochemi ode reaction, both manganates and permanganates can have cally active solid cathode is demonstrated using silver a signi?cantly higher faradaic capacity and higher cathodic permanganate. potential. The thermodynamic potential for the le- perman ganate to manganate reduction in aqueous alkaline media is: BRIEF DESCRIPTION OF THE INVENTION [0011] The invention relates to an electrical storage cell, [0004] and manganate also can exhibit a direct discharge so-called alkaline battery, comprising tWo half-cells Which to manganese dioxide, summariZed as the 2e“ reduction: are in electrochemical contact With one another through an electrically neutral alkaline ionic conductor, Wherein one of said half-cells comprises an anode and the other half-cell [0005] and alternately permanganate also can exhibit a comprises a cathode, Whereby electrical storage is accom direct discharge to manganese dioxide, summariZed as the plished via electrochemical reduction of the cathode and 3e- reduction: oxidation of the anode. The cathode contains an electro chemically active silver manganate, or silver permanganate [0006] In addition, the MnO2 product can undergo a fur compound, or oxidiZed silver and manganate or permanga ther 1e- reduction, as utiliZed in the conventional commer nate material. cial alkaline (Zn anode/MnO2 cathode) cell: BRIEF DESCRIPTION OF THE FIGURES [0012] FIG. 1 is a diagrammatic illustration of the silver [0007] Manganate salts, being in the less oxidiZed man (per)manganate material cathode battery according to the ganese valence state of Mn(VI), Will store less charge in principle, than the permanganates. This loWer valence state invention; and Would also suggest that they Would be considered to be less [0013] FIGS. 2 to 8: illustrate graphically performance of chemically active. In principal, as described by equations 2 various battery aspects according to the invention as and 4, permanganate salts can undergo a total of a 4e described in the Examples. alkaline cathodic reduction, and by equations 3 and 4 manganate salts can undergo a total of a 3e- alkaline DETAILED DESCRIPTION OF THE cathodic reduction. Yet the manganate and permanganate INVENTION salts have not replaced the Widely used commercial alkaline MnO2 cathode due to a general perception that these salts are [0014] The novel battery according to the present inven too soluble (creating a tendency to react and decompose the tion is based on the addition of an electrochemically active anode), and that they exhibit only inef?cient, and/or loW silver manganate material or silver permanganate material to current density, charge transfer. form a cathode in an alkaline battery, as silver (permanga nate and hydroxide. In one embodiment the hydroxide is in [0008] The absorbance spectra and Xray diffraction of the form of a salt solid. In a preferred embodiment the solid AgMnO4 has been characteriZed P. Doyle, I. Kirkpatrick, hydroxide comprises at least 1% of the Weight of the cathode Spectrochimica Acta, 24A (1968) 1495]. AgMnO4 is not a mass. In other embodiments, the solid hydroxide comprises traditional Mn(VII) permanganate salt and the manganese at least 5% or 25% of the Weight of the cathode mass. In a evidently exists in a valence state betWeen VI and VII, While preferred embodiment the silver (per)manganate is in the the silver exists in a valence state betWeen I and II [L. F. form of AgMnO4, or in an alternate embodiment is in the Mehne, B. B. Wayland, J. Inorg. Nucl. Chem., 37 (1975) form of Ag(MnO 4)2, or in an alternate preferred embodiment US 2003/0008210 A1 Jan.
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