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Ultrathin amorphous carbon layer induced dual interactive interface for efficient C-H bond activation in heptane
Ying Feng1, Zhiquan Hou2, Peijie Ma2
1Institute of Catalysis for Energy and Environment, College of Chemistry and Chemical Engineering, Shenyang Normal University, Shenyang 110034, China; State Key Laboratory of Materials Low-Carbon Recycling, College of Materials Science and Engineering, Beijing University of Technology, Beijing 100124, China.
Abstract:
The activation of C-H bonds is a fundamental process in various chemical reactions, while faces significant challenge under mild conditions due to the high bond energy and low polarity. An ultrathin (∼3 nm) amorphous oxygen-containing carbon layer inserted into Pt/TiO2 yields C-O-M (M = Pt and Ti) dual interfaces. The photothermocatalytic consumption rate of n-heptane over Pt/C/TiO2 at 140 ℃ is 8.8 and 61.8 times higher than that over Pt/TiO2 and Pt/C, respectively. Temperature-programmed desorption (TPD) and density functional theory (DFT) calculations reveal that the constructed C-O-M interfaces significantly enhance the adsorption of hydrocarbon reactant, and decrease the C-H bond scission energy barrier. The photothermal X-ray photoelectron spectroscopy (XPS), femtosecond transient absorption (fs-TA) and electron paramagnetic resonance (EPR) experiments demonstrate that the C-O-Ti interface accelerates the electron migration and transforms the adsorbed oxygen into the superoxide species, thus efficiently oxidizing the reactant. Furthermore, introduction of an amorphous carbon layer to Pt/Al2O3, Pt/CeO2, Ce/TiO2 or Cu/TiO2 remarkably enhances the photothermal catalytic performance for propane, pentane, octane, toluene or hexanal oxidation. The unique effect of C-O-M dual interfaces induced via the ultrathin amorphous carbon layer provides a guideline for designing catalysts with efficient C-H bond activation ability.
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