Anchoring and Upgrading Ultrafine NiPd on Room-Temperature-Synthesized Bifunctional NH2-N-rGO toward Low-Cost and Highly Efficient Catalysts for Selective Formic Acid Dehydrogenation

Abstract

Hydrogen is widely considered to be a sustainable and clean energy alternative to the use of fossil fuels in the future. Its high hydrogen content, nontoxicity, and liquid state at room temperature make formic acid a promising hydrogen carrier. Designing highly efficient and low-cost heterogeneous catalysts is a major challenge for realizing the practical application of formic acid in the fuel-cell-based hydrogen economy. Herein, a simple but effective and rapid strategy is proposed, which demonstrates the synthesis of NiPd bimetallic ultrafine particles (UPs) supported on NH₂-functionalized and N-doped reduced graphene oxide (NH₂-N-rGO) at room temperature. The introduction of the NH₂N group to rGO is the key reason for the formation of the ultrafine and well-dispersed Ni_0.4Pd_0.6 UPs (1.8 nm) with relatively large surface area and more active sites. Surprisingly, the as-prepared low-cost NiPd/NH₂-N-rGO dsiplays excellent hydrophilicity, 100% H₂ selectivity, 100% conversion, and remarkable catalytic activity (up to 954.3 mol H₂ (mol catalyst)⁻¹ h⁻¹) for FA decomposition at room temperature even with no additive, which is much higher than that of the best catalysts so far reported.

Ultrafine NiPd nanoparticles supported on a NH₂-functionalized and N-doped reduced graphene oxide (NH₂-N-rGO) substrate are successfully prepared through a facile one-step strategy. The as-prepared NiPd/NH₂-N-rGO catalyst shows prominent catalytic performance (turnover frequency value up to 954.3 h⁻¹), 100% H₂ selectivity, and 100% conversion for formic acid dehydrogenation at 298 K without any additive.

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