Nitrogen-doped carbon supported PtPd alloy nanoparticles exhibiting high catalytic activity for cyclohexane dehydrogenation under low temperatures

Abstract

While Pt-based heterogeneous catalysts have been extensively studied for cyclohexane dehydrogenation, the reaction efficiency under low temperatures remains to be resolved. In this paper, ultrafine PtPd alloy nanoparticles homogeneously anchored on nitrogen-doped carbon were synthesized and applied for cyclohexane dehydrogenation. The experimental results indicate that the synergistic effect of Pt-Pd in PtPd/CN catalyst enhances the activity and durability of the catalyst in cyclohexane dehydrogenation compared with Pt/CN and Pd/CN catalysts. The as-prepared catalyst (labeled as Pt0.75Pd0.25/CN) exhibits an excellent catalytic performance with an initial TOF value of 90.07 mmol·g−1metal·min−1 and a 100% H2 purity for cyclohexane dehydrogenation at 180 °C, exceeding reported values under comparable reaction conditions. Catalyst characterizations and DFT calculations reveal that the electronic coupling effect of Pd and Pt in PtPd/CN catalyst makes the d-band center of Pt active sites closer to the Fermi level, which promotes the specific adsorption/activation of cyclohexane on Pt active sites, thus improving the catalytic performance of cyclohexane dehydrogenation. Under this guidance, the synthesized PtRu/CN and PtIr/CN alloy catalysts exhibited similar enhanced activity in cyclohexane dehydrogenation. This work provides insights into the rational design of efficient and stable Pt-based bimetallic catalysts for cyclohexane dehydrogenation.