Rational design of ZrO2-supported d-block single-atom electrochemical catalysts for the nitrogen reduction reaction

Abstract

The development of effective and robust electrochemical catalysts for the nitrogen reduction reaction (NRR) remains a substantial challenge for ammonia synthesis under mild conditions. In this study, we investigate the potential of single-atom d-block transition metals embedded within ZrO₂ monolayers as catalysts for the NRR. Through advanced ab initio calculations, we elucidate a straightforward yet effective principle for describing the limiting potential of the NRR. Additionally, we identify two previously unreported and highly efficient electrocatalysts, Nb@ZrO₂ and V@ZrO₂, both of which demonstrate notably low limiting potentials of −0.3 V. Furthermore, these catalysts exhibit excellent selectivity and commendable stability. These results offer valuable insights for advancing research on high-performance NRR catalysts.