Tuning Pt–N₂H₄ adsorption on NiFe-LDH-Supported Pt for enhanced cycling stability in ammonia electro-oxidation

Ammonia has recently been recognized as a promising energy carrier for long-term and large-scale energy storage. Direct ammonia fuel cells (DAFCs) stand out among ammonia utilization technologies due to their high theoretical energy conversion efficiency and environmental compatibility. Although Pt has been widely regarded as the most effective electrocatalyst for ammonia oxidation in alkaline media compared to other noble metals, designing composite structures of Pt to improve the AOR performance of Pt-based catalysts through carrier modulation is still the best solution for designing fuel cell anode materials at present. This work presents an electrochemical synthesis strategy for in situ reduction of [PtCl 6 ] 2− precursors into Pt nanoparticles anchored on NiFe-layered double hydroxide/nickel foam substrates. The unique structure supplies sufficient OH ad for the gradual dehydrogenation of Pt, the two-dimensional layered structure provides a vast loading space for Pt, and more importantly, the bimetallic nature of LDH modulated the electronic state of Pt and thus further regulated the adsorption state of Pt with N 2 H 4 and was verified by in situ IR spectroscopy, which facilitated the reaction towards the G-M mechanism, reduced the toxicity of the *N atoms, and improved the CV cycling stability of the catalyst. The study of the composite structure of Pt and LDH provided a new approach for the exploration of Pt composite catalysts used in the anode catalysts of DAFC.