Positronium chemistry of a Fe2+/3+ solution under electrochemical control

Philipp Brunner*, Eva-Maria Steyskal, Stefan Topolovec, Roland Würschum

*Korrespondierende/r Autor/-in für diese Arbeit

Publikation: Beitrag in einer FachzeitschriftArtikelBegutachtung


The positronium chemistry of a Fe2+/3+ solution is studied under full electrochemical control. For this novel approach to positronium
electrochemistry, a suitable cell setup is used, which allows simultaneously both electrochemical measurements and positron annihilation
spectroscopy. For the Fe2+/3+ redox couple, positronium serves as an ideally suited atomic probe owing to the rather different positronium
chemistry of Fe2+ (spin conversion) and Fe3+ (total positronium inhibition and oxidation). This enabled the precise in situ monitoring of
oxidation and reduction by means of positron lifetime upon slow cycling voltammetry or galvanostatic charging. The variation of the mean
positron lifetime with the Fe2+/3+ concentration ratio could be quantitatively described by a reaction rate model for positronium formation
and annihilation. An asymmetric behavior of the variation of the mean positron lifetime with applied potential, as compared to the simultaneously
recorded symmetric current–potential curve, could be explained by the stronger influence of Fe3+ on the characteristics of positronium
formation and annihilation. The highly reversible galvanostatic charging behavior monitored by positron lifetime underlines the attractive
application potentials of positronium electrochemistry for in situ studies of iron-based redox-flow battery electrolytes.
FachzeitschriftThe Journal of Chemical Physics
PublikationsstatusVeröffentlicht - 21 Dez. 2022

ASJC Scopus subject areas

  • Allgemeine Physik und Astronomie
  • Physikalische und Theoretische Chemie

Fields of Expertise

  • Advanced Materials Science


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