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MELILITE COMPOSITE OXIDE

Foreign code F200010042
File No. P2019-544572
Posted date Mar 11, 2020
Country WIPO
International application number 2018JP034073
International publication number WO 2019065285
Date of international filing Sep 13, 2018
Date of international publication Apr 4, 2019
Priority data
  • P2017-190808 (Sep 29, 2017) JP
Title MELILITE COMPOSITE OXIDE
Abstract Provided is a novel compound which can be used for a positive-electrode catalyst of a metal-air battery. The melilite composite oxide according to the present invention is represented by general formula (BazSr1-z)2CoxFe2-2x(SiyGe1-y)1+xO7 (in the formula, 0 ≤ x ≤ 1, 0 ≤ y ≤ 1, and 0 ≤ z ≤ 1, excluding the case where x = 1, y = 1, and z = 0, the case where x = 1, y = 1, and z = 1, the case where x = 1, y = 0, and z = 0, the case where x = 1, y = 0, and z = 1, the case where x = 0, y = 0, and z = 0, and the case where x = 0, y = 0, and z = 1).
Outline of related art and contending technology BACKGROUND ART
Of the electric vehicle (EV) further spread, the cruising distance of the gasoline to realize parallel development of high energy density battery is indispensable. Current, the current lithium ion secondary battery exceeds the ' innovation type storage batteries' as one of, a metal-air battery is attracting attention. And a metal-air battery, metal such as zinc as the negative electrode active material, the oxygen in the air as the positive electrode active material refers to a secondary battery. Such metal-air battery, a very high theoretical energy density may be achieved. A metal-air battery, zinc-air battery using zinc as the metal in particular is, research and development in the research institute and overseas long been performed (for example, Non-Patent Document 1, 2), at present, a full-fledged into practical use has not yet been produced.
Incidentally, in the air electrode of a metal-air battery, during discharge of the oxygen reduction reaction (active material) of the hydroxide ion generated by the electronic 4, on the other hand, during charging hydroxide ions and oxygen is generated by the oxidation reaction of the electron 4. These oxygen reduction reaction with the electron transfer 4 (hereinafter, also called 'ORR'.) And the oxygen evolution reaction (hereinafter, also called 'OER'.) Is, in a very slow reaction kinetics from the overvoltage generated when the large charge and discharge, ORR/OER can promote the high activity catalyst is required.
Specifically, a metal-air battery of the charging reaction and discharging reaction at each electrode, the following (1) - (4) equation is as follows. In addition, type (1) - (4) in, for the sake of convenience, the negative electrode using zinc as an example. (Positive) charge reaction (oxygen evolution reaction): 4OH - O2+2H2O+4e -→, (1) discharge reaction (oxygen reduction reaction): O2+2H2O+4e-4OH -→, (negative electrode), (2) the charging reaction: ZnO + H2O + 2e -→Zn+2OH -, (3) the discharge reaction: Zn + 2OH -→ZnO + H2O + 2e -, (4)
Here, in a metal-air electrode, the high-concentration KOH aqueous solution as an electrolytic solution using a strong alkali aqueous solution, the (1) hydroxide ion type, (4) involved in the supply. Then, the positive electrode is immersed in an aqueous solution is strongly alkaline catalyst for, excellent chemical stability are required.
As the positive electrode catalyst, platinum, ruthenium oxide, iridium oxide or the like having the noble metal based catalyst of known ORR/OER activity. However, these noble metal contained in the rare and expensive such as a vehicle battery from a large-scale practical realization is difficult. Therefore, the transition metal or the like, is abundant in resource element as its main component with a general-purpose high-performance positive electrode active ORR/OER has been desired development of a catalyst.
On the other hand in recent years, as the positive electrode catalyst, (ABO3) type transition metal oxide perovskite has been developed. To this, the structure of the perovskite octahedral coordination of six ABO3 the energy level of the B site t2g and when dividing eg, eg the number of electrons becomes maximum in the active ORR/OER 1 have been reported (for example, Non-Patent Document 3, 4). However, such a design guideline, BO6 octahedral coordination compounds other than the perovskite structure, particularly as compared to other metal-oxygen coordination compounds having the structure described has not been considered at all. In particular, in the operating environment of the metal-air battery which is practically usable, useful materials are not yet been found.
Scope of claims (In Japanese)[請求項1]
 一般式(Ba zSr 1-z2Co xFe 2-2x(Si yGe 1-y1+xO 7(式中、0≦x≦1,0≦y≦1,0≦z≦1である。但し、x=1且つy=1且つz=0の場合、x=1且つy=1且つz=1の場合、x=1且つy=0且つz=0の場合、x=1且つy=0且つz=1の場合、x=0且つy=0且つz=0の場合及びx=0且つy=0且つz=1の場合を除く。)で表される
 メリライト型複合酸化物。

[請求項2]
 前記一般式中、0.5≦x≦0.9である
 請求項1に記載のメリライト型複合酸化物。

[請求項3]
 前記一般式中、0≦y≦0.1である
 請求項1又は2に記載のメリライト型複合酸化物。

[請求項4]
 一般式(Ba z1Sr 1-z1-z2RE z22Co x1Zn x2Fe 2-2(x1+x2)(Si yGe 1-y1+x1+x2O 7(式中、0≦x1≦1,0≦x2≦0.2,0≦y≦1,0≦z1≦1,0≦z2≦0.2であり、且つx2及びz2の少なくともいずれかが0超である)で表される
 メリライト型複合酸化物。

[請求項5]
 前記メリライト型複合酸化物は、前記一般式中、REがYである
 請求項4に記載のメリライト型複合酸化物。
  • Applicant
  • ※All designated countries except for US in the data before July 2012
  • KANAGAWA UNIVERSITY
  • Inventor
  • OGAWA SATOSHI
  • MOTOHASHI TERUKI
  • SAITO MIWA
  • SUZUKI KENTA
IPC(International Patent Classification)
Specified countries National States: AE AG AL AM AO AT AU AZ BA BB BG BH BN BR BW BY BZ CA CH CL CN CO CR CU CZ DE DJ DK DM DO DZ EC EE EG ES FI GB GD GE GH GM GT HN HR HU ID IL IN IR IS JO JP KE KG KH KN KP KR KW KZ LA LC LK LR LS LU LY MA MD ME MG MK MN MW MX MY MZ NA NG NI NO NZ OM PA PE PG PH PL PT QA RO RS RU RW SA SC SD SE SG SK SL SM ST SV SY TH TJ TM TN TR TT TZ UA UG US UZ VC VN ZA ZM ZW
ARIPO: BW GH GM KE LR LS MW MZ NA RW SD SL SZ TZ UG ZM ZW
EAPO: AM AZ BY KG KZ RU TJ TM
EPO: AL AT BE BG CH CY CZ DE DK EE ES FI FR GB GR HR HU IE IS IT LT LU LV MC MK MT NL NO PL PT RO RS SE SI SK SM TR
OAPI: BF BJ CF CG CI CM GA GN GQ GW KM ML MR NE SN ST TD TG

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