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The ammonia oxidation reaction (AOR) is a key challenge limiting the performance of direct ammonia anion exchange membrane fuel cells (DA-AEMFCs) due to sluggish kinetics and catalyst poisoning. Herein, we report a metal–support interaction tuning strategy using molybdenum carbide supports to systematically regulate AOR activity of PtIr catalysts. By tuning the carburization degree from metallic Mo to Mo2C and MoC, the electronic structure and d-band center of PtIr are modulated, which is expected to regulate the adsorption/desorption behavior of reaction intermediates during AOR. The optimized PtIr/Mo2C catalyst exhibits superior activity (111.6 A gPGM−1) and high single-cell power density (278.6 mW cm−2). This work provides a controllable interfacial engineering strategy for favorable intermediate binding and advancing high-performance AOR electrocatalysis.

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