Holistic Assessments of New Sodium Superionic Frameworks

The discovery of tunable superionic conducting frameworks is necessary for the development of next generation solid state batteries. To this end, we present a computational-experimental materials exploration strategy leveraged to comprehensively reintroduce the sodium conducting framework, Na₄TiP₂O₉ (NTP). We utilize high-throughput computational screening to probe chemical and structural substitutions on the text-mined NTP parent structure. We validate (meta)stable NTP candidates through application of synthesis selection algorithms employed by an experimental autonomous laboratory. Our expansive data set of synthesis trials allow us to propose simple but powerful generalized synthesis methodology rules for Na_xMP₂O_9.Finally, we highlight the structural, chemical, and conductivity characterization of realized compounds. Our work is a testament to the powerful interplay of data-driven computation and experimentation, particularly when applied to research on new superionic conduction frameworks for energy storage advancement.