Abstract
This review adopts a fundamental perspective of effective N2/NOx conversion catalysts. In particular, we delve into how the intrinsic catalyst-reactant binding and microenvironment effects dictate the reaction mechanism, pathway, and ultimately, efficiency. We apply this framework to critically examine not only molecular catalysts but also enzymatic and heterogeneous systems from this unique lens. In doing so, we identify fundamental parallels and critical contrasts among all classes of catalytic systems. In a forward-thinking manner, we use this unifying framework to identify remaining knowledge gaps to be closed and pinpoint key areas for future pursuits. This includes the identification of concrete, translatable insights to boost practically geared systems and directions for future synthetic development toward model molecular catalysts that are poised to answer long-standing fundamental questions.