Cooperative active sites on Ag2Pt3TiS6 for enhanced low‐temperature ammonia fuel cell electrocatalysis

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 Ag2Pt3TiS6 electrocatalyst that facilitates both reactions at activities exceeding that of commercial Pt/C. Through comprehensive density functional theory simulations, 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 *NOx formation and hence an increased resistance toward catalyst poisoning for AOR. Employing Ag2Pt3TiS6 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.