ACS Sustainable Chemistry & Engineering | 2019
Pd-Supported N/S-Codoped Graphene-Like Carbons Boost Quinoline Hydrogenation Activity
Abstract
Pd nanoparticles (∼2.1 nm) supported on biomolecule-derived graphene-like carbons have been studied as highly active and stable catalysts for the selective hydrogenation of quinolines. A novel strategy is developed by pyrolysis of guanine with H2SO4, yielding heteroatom-doped (N/O, N/O/S) and minimally layered carbon nanosheets with large accessible areas, which can facilitate mass transfer and stabilize Pd nanoparticles. XPS results indicate that the intensity ratio of Pd0/Pd2+ increases with N/S codoping in graphene-like carbons, suggesting a significant correlation between support properties and electronic structure of Pd species. N/O/S-codoped Pd@GS1000 shows substantially enhanced activity for quinoline hydrogenation reactions, with almost >99% conversion and >99% selectivity to 1,2,3,4-tetrahydroquinoline under mild catalytic conditions, superior to Pd@G1000 (without sulfur doping) and the reference Pd/OCNT catalyst. Further investigation indicates that sulfur-containing carbon nanosheets strongly i...