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We demonstrate that in\u2010situ N\u2010doping of Ru nanoparticles and graphitized carbon nanofiber supports during reaction produces a sharp increase in hydrogen production during the first 40\u00a0h, followed by stable activity. Spectroscopic and microscopic analyses, together with density functional theory simulations, reveal that Ru nitridation is rapid and support\u2010independent, resulting in a mechanistic shift from the traditional Langmuir\u2013Hinshelwood to a Mars\u2013van Krevelen pathway, further confirmed by isotopic labelling experiments. In contrast, the progressive nitridation of the carbon support, observed via X\u2010ray photoelectron spectroscopy, modulates the electronic environment of Ru and functions as a dynamic nitrogen reservoir that enables reversible N atoms exchange with the Ru particles, facilitating N desorption from the Ru surface and thereby governing the catalytic activity enhancement. These new findings provide new mechanistic insight into ammonia decomposition and establish progressive nitrogen doping of carbon supports as a strategy for designing efficient metal\u2010based catalysts for hydrogen production.<\/jats:p>","DOI":"10.1002\/anie.202522937","type":"journal-article","created":{"date-parts":[[2025,12,22]],"date-time":"2025-12-22T05:50:27Z","timestamp":1766382627000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":6,"title":["Metal\u2010Mediated Nitrogen Doping of Carbon Supports Boosts Hydrogen Production from Ammonia"],"prefix":"10.1002","volume":"65","author":[{"given":"Thomas J.","family":"Liddy","sequence":"first","affiliation":[{"name":"School of Chemistry University of Nottingham  Nottingham NG7 2RD UK"},{"name":"Diamond Light Source Ltd.  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