| Summary: | Formic acid (FA) is one of the most prospective hydrogen carriers for renewable energy transformation. In this context, the addition of extra-amine is always required for promoting the reactivity of FA, which is still a key challenge. Herein, we report a simple but effective strategy to synthesize Pd nanoparticles, supported on NH<sub>2</sub>-functionalized, phosphorous-doped glucose-based porous carbon (NH<sub>2</sub>-P-GC). The introduction of NH<sub>2</sub>- groups on the support acts as an immobilized amine-additive for FA dehydrogenation, while phosphorus not only serves as an electronic promoter to keep Pd in the electronic deficient state for FA dehydrogenation, but also as an enlarger of the aperture size of the carbon. As a result, the Pd/NH<sub>2</sub>-P-GC has exceptional catalytic activity, 100% H<sub>2</sub> selectivity, CO generation that is undetectable, and good reusability for hydrogen production from FA. In the additive-free dehydrogenation of aqueous FA solution, the initial turnover frequency (TOF) can reach 5126 h<sup>−1</sup> at room temperature, which is substantially higher than the best heterogeneous catalyst so far recorded. Overall, the system’s high activity, selectivity, stability, and simplicity in producing CO-free H<sub>2</sub>/CO<sub>2</sub> gas from FA, without the need for any additive, makes it attractive for practical deployment.
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