Ultrathin amorphous carbon layer induced dual interactive interface for efficient C–H bond activation in heptane oxidation under mild photothermal condition

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/TiO 2 yields C–O–M (M = Pt and Ti) dual interfaces. The photothermocatalytic consumption rate of n -heptane over Pt/C/TiO 2 at 140 ℃ is 8.8 and 61.8 times higher than that over Pt/TiO 2 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/Al 2 O 3 , Pt/CeO 2 , Ce/TiO 2 or Cu/TiO 2 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.