Abstract
The C-C bond cleavage remains a main challenge for alkaline EOR(ethanol oxidation reaction).In this work,we report an efficient PdSn-TaN/C electrocatalyst to split the C-C bonds in ethanol.Structurally,a series of characterization results confirm the presence of the low-coordinated Pd sites on the PdSn-TaN/C interface.The PdSn-TaN/C catalyst exhibits very high activity(almost 26.9 times of commercial Pd/C),good durability and high selectivity to CO2(20.5%)towards alkaline EOR.Specifically,in-situ ATR-SEIRAS(Attenuated total reflection-surface enhanced infrared absorption spectroscopy)results indicate that TaN facilitates the cleavage of C-C bonds,whereas Sn promotes the further oxidation of ethanol fragments.DFT(density functional theory)calculations indicate the activation barriers of the C-H bond cleavage in CH3CH2OH,CH3CHOH,CH3CHO,CH3CO,CH2CO and the C-C bond cleavage in CH3CO,CH2CO,CHCO are reduced evidently and the removal of adsorbed CH3CO and CO becomes easier on the PdSn-TaN/C catalyst surface.
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