Weiye Qu, Pranav Roy, Canhui Wang, Lu Ma, Fan Bu, Xinsui Zhang, Zimin He, Michael Tsapatsis, Brandon C. Bukowski* and Chao Wang*,
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Earth-Abundant Manganese Nitride Catalysts for Mild-Condition Ammonia Synthesis
Developing advanced catalytic materials for mild-condition ammonia (NH3) synthesis is essential for improving the energy efficiency of the industrial Haber-Bosch process. Here, we report a ζ-phase manganese nitride (MnN0.43) catalyst for low-temperature NH3 synthesis. The as-synthesized MnN0.43 catalyst is protected by a carbon shell, allowing for the storage and processing of the air-sensitive metal nitride under ambient conditions. After activation in situ, the MnN0.43 catalyst exhibits high activity for NH3 synthesis at 250–350 °C, surpassing the conventional noble metal based Ru/MgO catalyst. A combination of kinetic, chemisorption, isotope labeling and computational studies indicate that a nitrogen vacancy-mediated associative mechanism accounts for the catalytic enhancements. Our work highlights the great potential of earth-abundant transition metal nitrides for catalyzing mild-condition NH3 synthesis.
期刊介绍:
ACS Catalysis is an esteemed journal that publishes original research in the fields of heterogeneous catalysis, molecular catalysis, and biocatalysis. It offers broad coverage across diverse areas such as life sciences, organometallics and synthesis, photochemistry and electrochemistry, drug discovery and synthesis, materials science, environmental protection, polymer discovery and synthesis, and energy and fuels.
The scope of the journal is to showcase innovative work in various aspects of catalysis. This includes new reactions and novel synthetic approaches utilizing known catalysts, the discovery or modification of new catalysts, elucidation of catalytic mechanisms through cutting-edge investigations, practical enhancements of existing processes, as well as conceptual advances in the field. Contributions to ACS Catalysis can encompass both experimental and theoretical research focused on catalytic molecules, macromolecules, and materials that exhibit catalytic turnover.