Plasmon-Enhanced Photocatalysis Coupling Electrocatalysis Steering Methanol Oxidation toward a CO-Free Dominant Pathway
Xingming Xie, Jianguang Feng, Xuejing Cui, Jing Liu, Luhua Jiang, Lifeng Dong
Abstract
Methanol electro–oxidation reaction (MOR), as the anode reaction of direct methanol fuel cells, fundamentally determines the device efficiency. Coupling electrocatalysis with photocatalysis provides a promising yet challenging strategy to accelerate the MOR kinetics. Herein, we demonstrate that the localized surface plasmon resonance (LSPR) from Ag strengthens the photo-/electrocatalysis coupling process, leading to a dramatical decrease in the apparent activation energy and thus doubling MOR currents over Pt/Ag0.333V2O5 under illumination versus in dark. Mechanism investigations reveal that the MOR enhancement can be mainly attributed to the accelerated dehydrogenation of methanol on a negatively charged Pt surface facilitated by the photogenerated OHad on Ag0.333V2O5, leading to a COad-free dominant pathway, and the LSPR of Ag promotes the charge transfer in the coupling process. This study sheds light on the mechanism of plasmonic metals involved in the photo-/electrocatalysis coupling process and provides an avenue for designing highly efficient MOR photo/electrocatalysts.