High-throughput computational screening of doped transition metal oxides as catalysts for nitrogen reduction

Developing sustainable methods for ammonia synthesis is impor-tant to combat rising global carbon emissions. An alluring possibility is the electrochemical reduction of nitrogen in an aqueous electro-lyte, driven by renewable energy, but a suitable catalyst has remained elusive. Herein, we present the results of a large-scale computational screening study of the catalytic properties of over 800 doped transition metal oxides. Using activity and selectivity descriptors, we identify MoO2-based materials that could possibly catalyze ammonia synthesis, likely along with hydrogen evolution. MoO2 doped with tungsten is the most promising candidate, with predicted limiting potentials ranging from -0.5 to -1.1 V. However, further analysis suggests that hydrogen evolution is likely to be dominant in most cases. By establishing a set of screening criteria, we further provide a framework for future screening studies of doped materials.