Abstract: Ammonia serves as a crucial chemical raw material and hydrogen energy carrier. Aqueous electrocatalytic nitrogen reduction reaction (NRR), powered by renewable energy, has attracted tremendous interest during the past few years. Although some achievements have been revealed in aqueous NRR, significant challenges have also been identified. The activity and selectivity are fundamentally limited by nitrogen activation and competitive hydrogen evolution. This review focuses on the hurdles of nitrogen activation and delves into complementary strategies, including materials design and system optimization (reactor, electrolyte, and mediator). Then, it introduces advanced interdisciplinary technologies that have recently emerged for nitrogen activation using high-energy physics such as plasma and triboelectrification. With a better understanding of the corresponding reaction mechanisms in the coming years, these technologies have the potential to be extended in further applications. This review provides further insight into the reaction mechanisms of selectivity and stability of different reaction systems. We then recommend a rigorous and detailed protocol for investigating NRR performance and also highlight several potential research directions in this exciting field, coupling with advanced interdisciplinary applications, in situ/operando characterizations, and theoretical calculations. ; This work was supported by the Natural Sciences and Engineering Research Council of Canada (NSERC), the Fonds de Recherche du Québec-Nature et Technologies (FRQNT), Centre Québécois sur les Materiaux Fonctionnels (CQMF), Institut National de la Recherche Scientifique (INRS), École de Technologie Supérieure (ÉTS), and the King Abdullah University of Science and Technology (KAUST). Dr. Gaixia Zhang thanks for the support from the Marcelle-Gauvreau Engineering Research Chair program.
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