Cooperative Active Sites on Ag₂Pt₃TiS₆ for Enhanced Low‐Temperature Ammonia Fuel Cell Electrocatalysis

Abstract Ammonia has attracted considerable interest as a hydrogen carrier that can help decarbonize global energy networks. Key to realizing this is the development of low temperature ammonia fuel cells for the on‐demand generation of electricity. However, the efficiency of such systems is significantly impaired by the sluggish ammonia oxidation reaction (AOR) and oxygen reduction reaction (ORR). Here, we report the design of a bifunctional Ag 2 Pt 3 TiS 6 electrocatalyst that facilitates both reactions at mass activities exceeding that of commercial Pt/C. Through comprehensive density functional theory calculations, we identify that active site motifs composed of Pt and Ti atoms work cooperatively to catalyze ORR and AOR. Notably, in situ shell‐isolated nanoparticle‐enhanced Raman spectroscopy (SHINERS) experiments indicate a decreased propensity for *NO x formation and hence an increased resistance toward catalyst poisoning for AOR. Employing Ag 2 Pt 3 TiS 6 as both the cathode and anode, we constructed a low temperature ammonia fuel cell with a high peak power density of 8.71 mW cm −2 and low Pt loading of 0.45 mg cm −2 . Our findings demonstrate a pathway towards the rational design of effective electrocatalysts with multi‐element active sites that work cooperatively.