期刊
ACS CATALYSIS
卷 11, 期 21, 页码 13160-13168出版社
AMER CHEMICAL SOC
DOI: 10.1021/acscatal.1c03756
关键词
photoelectrocatalysis; methanol oxidation; plasmon effect; coupling effect; mechanism
资金
- National Natural Science Foundation of China [22179067, 21805156]
- Key Research and Development Program of Shandong Province [2019JZZY020809]
- Taishan Scholar Program of Shandong Province [ts201712046]
The coupling of localized surface plasmon resonance (LSPR) from silver with photocatalysis and electrocatalysis can enhance the efficiency of methanol electro-oxidation reaction, increasing current and decreasing apparent activation energy. Mechanistic investigations shed light on the process, offering a new avenue for designing highly efficient MOR photo/electrocatalysts.
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.
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