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Linking origin of the electric field-assisted β-PbF2 crystallization in lead oxyfluoroborate glasses below T g to simultaneous cathode/anode-compensated electrochemical reactions

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Abstract

Full validation of the electrochemical mechanisms so far postulated as driving force of electric field-assisted non-spontaneous crystallization development in given glasses has suffered experimental restrictions. In this work, we looked into origin of this phenomenon in lead oxyfluoroborate glasses, resulting in β-PbF2 growth even below the corresponding glass transition temperatures, through achieving a systematic study of not only Pt,Ag/Glass/Ag,Pt- but also Pt,Ag/Glass/YSZ:PbF2/Ag,Pt-type cells, where YSZ:PbF2 represents a two-phase system (formed by Y2O3-doped ZrO2 and PbF2). It is demonstrated that crystallization induction in these glasses involves Pb2+ ions reduction at the cathode, the phenomenon being, however, confirmed only when the F− ions were simultaneously also able to reach the anode for oxidation, after assuring either a direct glass–anode contact or percolation pathways for free fluoride migration across the YSZ:PbF2 mixtures. A further support of this account is that the electrochemically induced β-PbF2 phase crystallizes showing ramified-like microstructure morphology that arises, accordingly, from development of electroconvective diffusion processes under electric field action.

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Acknowledgments

The authors gratefully acknowledge financial support from the Fundação de Apoio à Pesquisa do Estado de São Paulo (FAPESP) and the Conselho Nacional de Desenvolvimento Científico e Tecnológico (CNPq), two Brazilian research funding agencies.

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  1. Grupo Crescimento de Cristais e Materiais Cerâmicos (GCCMC), Instituto de Física de São Carlos (IFSC), Universidade de São Paulo (USP), C. Postal: 369, CEP: 13560-970, São Carlos, São Paulo, Brazil

    José Ezequiel De Souza & Jean-Claude M’Peko

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  1. José Ezequiel De Souza
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  2. Jean-Claude M’Peko
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Correspondence to Jean-Claude M’Peko.

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De Souza, J.E., M’Peko, JC. Linking origin of the electric field-assisted β-PbF2 crystallization in lead oxyfluoroborate glasses below T g to simultaneous cathode/anode-compensated electrochemical reactions. J Solid State Electrochem 16, 191–196 (2012). https://doi.org/10.1007/s10008-011-1310-2

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  • DOI: https://doi.org/10.1007/s10008-011-1310-2

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