Yokohama National University H.Nakatsugawa, H.M.Jeong and K.Nagasawa

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Yokohama National University H.Nakatsugawa, H.M.Jeong and K.Nagasawa Thermoelectric properties and crystal structures in Y doped Ca3Co4O9 Yokohama National University H.Nakatsugawa, H.M.Jeong and K.Nagasawa

Outline Introduction Experimental Results and Discussion Summary Resistivity & Seebeck coefficient Thermoelectric property & crystal structure Magnetic susceptibility & valence state of Co Powder neutron diffraction data Modulation of Co-O bond distances Summary

Introduction 15mΩcm 130μV/K 0.98W/mK J.Sugiyama et al. : Phys.Rev.B 68 (2003) 134423 Y.Miyazaki et al : Solid State Ionics 172 (2004) 463-467

Experimental Solid-State reaction method ～ 85% Theoretical density Calcination in air at 920℃ Cold Isostatic Press (CIP) at 200MPa Sintered in O2 at 920℃ ～ 85% Theoretical density Magnetic properties Magnetic susceptibility at 10Oe : 2K ～ 350K Powder Neutron Diffraction Thermoelectric properties Rietveld refinement using PREMOS91 Crystal structures using PRJMS Interatomic distance plots using MODPLR Electrical resistivity : 80K ～ 800K Seebeck coefficient : 80K ～ 800K

Resistivity & Seebeck coefficient

Thermoelectric property & crystal structure

Magnetic susceptibility & valence state of Co [(Ca0.99Y0.01)2CoO3.20]0.62CoO2 [(Ca0.98Y0.02)2CoO3.21]0.62CoO2 [(Ca0.97Y0.03)2CoO3.18]0.62CoO2 [(Ca0.96Y0.04)2CoO3.21]0.62CoO2

Powder neutron diffraction data：pre-modulation Rwp = 12.39% x=0.02 0050 0010 0030 0020

Powder neutron diffraction data：after-modulation Rwp = 5.91% x=0.02 0050 0010 0030 0020

Modulation of Co-O bond distances (1) x=0 x=0.01 x=0.02 x=0.03 x=0.04

Modulation of Co-O bond distances (2) x=0 x=0.01 x=0.02 x=0.03 x=0.04

Modulation of Co-O bond distances (3) x=0 x=0.01 x=0.02 x=0.03 x=0.04

Y-doping is an effective method to improve TE performance of Ca3Co4O9 Summary The valence state of Co ions in Y doped Ca3Co4O9 Co3.2+ in CoO2 sheet Co3.6+ in RS-type BL A broad minimum at 100K and a broad maximum at 350K ～ 600K in ρ(T) curve Incommensurate SDW transition below TSDWon = 100K Spin-state transition below TSSon = 600K Y-doping is an effective method to improve TE performance of Ca3Co4O9