Photoluminescence of stabilized ZrO2 with different dopant

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Presentation transcript:

Photoluminescence of stabilized ZrO2 with different dopant 2019/6/19 Ashida Lab. Naoki Tanimoto

Solid Oxide Fuel Cell (SOFC) Devices that convert chemical energy directly into electrical energy, noted as a highly efficient, CO2 free energy source. Malavasi, et al., Chem. Soc. Rev., 2010, 39, 4370-4387 Household fuel cell system, Panasonic ENE-FARM Cathode　 O 2 +4 e − →2 O 2− Anode　 2H 2 +2 O 2− →2 H 2 O+4 e −

Solid Electrolyte dopant vacancy Ion conductivity Ion can move freely in this solid, when it is applied an electric field.

Formation of the Vacancy in Solid Electrolyte

Motivation Kinetics of the chemical reactions and ion diffusion, and macroscopic structure have been investigated for the solid electrolyte. (Conductivity, thermogravimetry, XRD, QNS, Raman…) I investigate the photoluminescence of the doped zirconia to reveal the local structure surrounding the carrier ions.

F Center F center The F center consists of an electron trapped at an anion vacancy. The trapped electrons couple to the vibrations of the host crystal. Excited electrons change the equilibrium position of surrounding ions. : M+ : X-

F Center E Q stokes shift wide band relaxation luminescence absorption emission absorption relaxation luminescence absorption wide band relaxation JOHN.LAMBE and W. DALE COMPTON, physical review, 106, 4 (1957)

Previous Work Intrinsic defect related luminescence in ZrO2 ・abstract K.Smits, L.Grigorjeva, D.Millers, A.Sarakovskis, J.Grabis, W.Lojkowski Journal of Luminescence 131, 10, 2058–2062 (2011) ・abstract The studies of ZrO2 and YSZ nanocrystals luminescence as well as YSZ single crystal luminescence showed that the intrinsic defects are responsible for luminescence at room temperature(RT).

Previous Work 1: YSZ single crystal 3: YSZ nanocrystal by HT hνex: 4.66 eV 1: YSZ single crystal 3: YSZ nanocrystal by HT HT: hydrothermal method Intrinsic F+ center Surface defect

My Work hνex: 4.8 eV single crystal hνex: 4.8 eV sintered compact(焼結体)

My Work Group1…MgSZ,CaSZ Group2…ScSZ,YSZ,GdSZ at 78K Ion radius hνex: 4.8 eV at 78K Ion radius Mg2+<(Zr4+)<Sc3+<Y3+<Gd3+<Ca2+ Group1…MgSZ,CaSZ Group2…ScSZ,YSZ,GdSZ

My Work Zr4+ -2 Ca2+ group1 dopant vacancy 1 : 1 Zr4+ -1 Y3+ group2 1 : 1 Zr4+ Y3+ O2- Zr4+ -1 Y3+ group2 dopant vacancy 2 : 1

Summary We introduced the photoluminescence of the color center, which includes on the information on the local structure of the defects related to the ion conduction. We divided the samples into two groups according to the valence of the ions. Future Work We will perform luminescence lifetime measurement of ZrO2 with different dopant.