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Item Open Access Controlling grain boundary segregation to tune the conductivity of ceramic proton conductors(2024) Kindelmann, Moritz; Povstugar, Ivan; Kuffer, Severin; Jennings, Dylan; Ebert, Julian N.; Weber, Moritz Lukas; Zahler, Pascal; Escolastico, Sonia; Almar, Laura; Serra, Jose M.; Kaghazchi, Payam; Bram, Martin; Rheinheimer, Wolfgang; Mayer, Joachim; Guillon, OlivierAcceptor‐doped barium zirconates are of major interest as proton‐conducting ceramics for electrochemical applications at intermediate operating temperatures. However, the proton transport through polycrystalline microstructures is hindered by the presence of a positive space charge potential at grain boundaries. During high‐temperature sintering, the positive charge acts as a driving force for acceptor dopant segregation to the grain boundary. Acceptor segregation to grain boundaries has been observed in sintered ceramics, but the fundamental relationship between the segregation kinetics and the protonic conductivity is poorly understood. Here, a comprehensive study of the influence of acceptor dopant segregation on the electrochemical properties of grain boundaries in barium zirconate ceramics is presented. An out‐of‐equilibrium model material that displays no detectable Y segregation at its grain boundaries is explicitly designed. This model material serves as a starting point to measure the kinetics of segregation and the induced changes in grain boundary conductivity upon varying thermal histories. Furthermore, the electrochemical results from impedance spectroscopy to atomic resolution transmission electron microscopy, atom probe tomography, and DFT simulations are correlated. It is discovered that acceptor dopant segregation drastically increases the proton conductivity in both the model system and several other application‐relevant compositions.