MgO-Decorated Amino-Functionalized N-Doped Mesoporous Carbon: A Robust Support for PdAu-Catalyzed Hydrogen Evolution from Formic Acid.

Formic acid (FA) is a promising liquid hydrogen carrier for sustainable energy storage, but its efficient dehydrogenation under mild conditions requires advanced catalyst designs. Here, we design a multifunctional supported PdAu catalyst tailored to the mechanistic demands of formic acid dehydrogenation (FAD), constructed by anchoring PdAu nanoparticles (NPs) onto MgO-decorated, nitrogen-doped, and amino-functionalized mesoporous carbon microspheres (MgO-NMC-NH2). Systematic characterization reveals MgO decoration introduces abundant surface basic sites, improves PdAu NP dispersion, and induces the formation of electron-enriched Pd species. The optimized PdAu/0.6MgO-NMC-NH2 catalyst exhibits exceptional FAD performance at 298 K, achieving complete conversion with an initial turnover frequency of 1866 h-1, 2.37 times as high as that of the MgO-free PdAu/NMC-NH2. This work highlights the potential of multicomponent support engineering for boosting the performance of noble metal catalysts, offering a scalable strategy to advance FA as a viable hydrogen storage material for clean energy applications.