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Bulk response and grain boundary microelectrical activity of high TC BaTiO3–(Bi1/2K1/2)TiO3-based positive temperature coefficient of resistance ceramics

Published online by Cambridge University Press:  23 October 2013

Mohammad A. Zubair ,
Hiroaki Takeda ,
Colin Leach ,
Robert Freer ,
Takuya Hoshina  and
Takaaki Tsurumi
Mohammad A. Zubair
Affiliation:
Department of Metallurgy and Ceramic Science, Graduate School of Science and Engineering, Tokyo Institute of Technology, Meguro, Tokyo 152-8552, Japan; and Materials Science Center, School of Materials, University of Manchester, Manchester M1 7HS, United Kingdom
Hiroaki Takeda*
Affiliation:
Department of Metallurgy and Ceramic Science, Graduate School of Science and Engineering, Tokyo Institute of Technology, Meguro, Tokyo 152-8552, Japan
Colin Leach
Affiliation:
Materials Science Center, School of Materials, University of Manchester, Manchester M1 7HS, United Kingdom
Robert Freer
Affiliation:
Materials Science Center, School of Materials, University of Manchester, Manchester M1 7HS, United Kingdom
Takuya Hoshina
Affiliation:
Department of Metallurgy and Ceramic Science, Graduate School of Science and Engineering, Tokyo Institute of Technology, Meguro, Tokyo 152-8552, Japan
Takaaki Tsurumi
Affiliation:
Department of Metallurgy and Ceramic Science, Graduate School of Science and Engineering, Tokyo Institute of Technology, Meguro, Tokyo 152-8552, Japan
*
a)Address all correspondence to this author. e-mail: htakeda@ceram.titech.ac.jp
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Abstract

Lead-free positive temperature coefficient of resistance (PTC) thermistors were synthesized from (1 − x/100)BaTiO3–(x/100)(Bi1/2K1/2)TiO3-based solid solutions, using a conventional mixed-oxide fabrication route, and sintered in N2 followed by air annealing. A maximum TC of 205 °C was achieved for x = 20. An increase in x from 0 to 20 decreased the grain size by more than 92% and increased room temperature resistivity (ρRT) by 7 orders of magnitude. For x ≤ 10, PTC ratio (ρmax/ρmin) ≈ 104.5 and temperature coefficient of resistivity (α) > 10.3%/°C were achieved using Mn and Al2O3:SiO2:TiO2 (AST) additions. For x > 10, ρmax/ρmin > 103 and α > 8%/°C were only obtained in samples sintered in N2 without subsequent air annealing. Complex impedance analysis revealed three relaxation processes, attributed to a semiconducting grain core, a PTC active grain boundary interface, and a grain boundary insulating layer. Local electrical activity was investigated by hot-stage conductive mode microscopy. The existence of symmetrical grain boundary electron beam-induced current and β-conductivity contrast at the grain boundaries, consistent with the presence of an electron trapping two-dimensional grain boundary plane, compensated by positive space charge layers and a low conductivity vacancy-rich layer, was revealed for the first time within this system.

Keywords

lead freethermistorCurie temperatureconductive modeelectron microscopyBaTiO3grain boundary
Type
Articles
Information
Journal of Materials Research , Volume 28 , Issue 21 , 14 November 2013 , pp. 2946 - 2959
Copyright
Copyright © Materials Research Society 2013 

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