Publication date: 10th April 2024
Lanthanide doped cerias show fast oxide ion conduction and have been applied as electrolytes in solid oxide fuel cells, operating at intermediate temperature range (ca. 500-700 °C) [1]. Among all the lanthanides, ceria doped with gadolinium (GDC, Ce1-xGdxO2-x/2) offers the best conductivity systems and has already been adopted commercially [2]. Although the conductivity of Nd-doped ceria (NDC, Ce1-xNdxO2-x/2) is slightly lower than that of GDC, it shows a lower minimum activation energy [3]. However, a lack of homogeneity or disruptions in local atomic arrangements in these systems can impede O2- ion transport, potentially suppressing ionic conductivity.
Using reverse Monte Carlo (RMC) analysis of total neutron scattering data on NDC compositions we have identified three distinct local structural features which cannot be determined by conventional average structure methods [4]. These features are the clustering of Nd3+ cations, preferred Nd3+-oxide ion vacancy association and oxide ion vacancy clustering with preferential alignment in the <100> direction. Dopant cation-oxide ion vacancy association is thought to play an important role at lower temperatures leading to higher activation energies. Interestingly, we also find evidence for a persistence of this association up to 600 °C, although diminished compared to the level at room temperature, which suggests a continued contribution of defect association enthalpy to activation energy at elevated temperatures.
The authors gratefully acknowledge Queen Mary University of London and the China Scholarship Council (Grant No. 202009150002) for a PhD scholarship to JM. The Science and Technology Facilities Council (STFC) is thanked for a neutron beam time award at ISIS (RB1810151). Dr Ron Smith at the ISIS Facility, Rutherford Appleton Laboratory UK is thanked for his help in neutron data collection. The authors gratefully acknowledge support from the National Science Centre, Poland under grant numbers UMO-2018/30/M/ST3/00743 and UMO-2016/23/D/ST5/03293.
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