Tuning Interfacial Electronic Properties of Palladium Oxide on Vacancy-Abundant Carbon Nitride for Low-Temperature Dehydrogenation
journal contributionposted on 07.05.2021, 12:36 authored by Hao Chen, Huili Shuang, Wenwen Lin, Xiaoxuan Li, Zihao Zhang, Jing Li, Jie Fu
Hydrogen energy has the merits of high energy value and zero carbon emissions, but its practical application is hindered by the intensive energy input required for dehydrogenation of liquid hydrocarbons (170–300 °C). Herein, toward highly efficient dehydrogenation of saturated N-heterocycles, assembly of PdO on carbon vacancy-abundant carbon nitride skeleton derived from in situ Zr-doping was demonstrated to improve catalyst with superior performance under mild conditions. Electron paramagnetic resonance (EPR), electrochemical impedance spectroscopy (EIS), and X-ray photoelectron spectroscopy (XPS) confirmed that the Zr-doped carbon nitride (Zr–C3N4) support showed a higher number of lone pair electrons and faster electron transfer rate compared with the parent. Strong interaction between PdO and the C3N4 skeleton was proved by the hydrogenation temperature-programmed reduction (H2-TPR) and XPS. By efficiently turning the electronic properties of PdO by Zr–C3N4, in which the affinity influences the strength of the metal–support interactions and therefore PdO dispersion, the as-prepared prototype catalyst PdO/Zr–C3N4 was capable of achieving complete dehydrogenation of a series of saturated N-heterocycles at only 140 °C within 8 h, supassing the performance rendered by most of the catalytic systems reported so far. This work offers a promising pathway for energy-efficient and cost-effective hydrogen energy utilization under practical conditions.
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pair electronsEPRZr-doped carbon nitrideTPRXPScarbon emissionsVacancy-Abundant Carbon NitrideStrong interactionH 2hydrogenation temperature-programme...Low-Temperature Dehydrogenation Hyd...N-heterocycleTuning Interfacial Electronic Prope...catalystC 3 N 4 skeletonaffinity influencesPdO dispersionenergy inputEISPalladium Oxidedehydrogenationperformancehydrogen energy utilizationcarbon vacancy-abundant carbon nitr...X-ray photoelectron spectroscopy8 henergy valueelectron transfer rate