Transition‐Metal‐Free Barium Hydride Mediates Dinitrogen Fixation and Ammonia Synthesis

Abstract Transition‐metal‐mediated dinitrogen fixation has been intensively investigated. The employment of main group elements for this vital reaction recently sparked interest because new chemistry. We report ammonia synthesis via a chemical looping process mediated by transition‐metal‐free barium hydride (BaH 2 ). Experimental and computational studies reveal that the introduction hydrogen vacancies is essential creating multiple coordinatively unsaturated Ba sites N activation. adjacent lattice hydridic (H − ) then undergoes both reductive elimination protonation to convert NH x . production rate supports hydride‐vacancy mechanism route far exceeds catalytic process. BaH ‐mediated prospects in future technologies using materials.