我室李剑锋教授在 ACIE 上发表论文:In Situ Raman Study of CO Electrooxidation on Pt(hkl) Single Crystal Surfaces in Acidic Solution
文章链接:https://onlinelibrary.wiley.com/doi/10.1002/anie.202010431
摘要:The adsorption and electrooxidation of CO molecules at well‐defined Pt( hkl ) single crystal electrode surfaces is a key step towards addressing catalyst poisoning mechanisms in fuel cells. Herein, we employed in situ electrochemical shell‐isolated nanoparticle‐enhanced Raman spectroscopy (SHINERS) coupled with theoretical calculation to investigate CO electrooxidation on Pt( hkl ) surfaces in acidic solution. We successfully obtained the Raman signal of top and bridge site adsorbed CO* molecules on Pt(111) and Pt(100). In contrast, on Pt(110) surfaces only top site adsorbed CO* was observed during the entire electrooxidation process. Direct spectroscopic evidence for OH* and COOH* species forming on Pt(100) and Pt(111) surfaces was afforded and confirmed subsequently via isotope substitution experiments and DFT calculations. In summary, the formation and adsorption of OH* and COOH* species plays a vital role in expediting the electrooxidation process, which relates with the pre‐oxidation peak of CO electrooxidation. This work deepens knowledge of the CO electrooxidation process and provides new perspectives for the design of anti‐poisoning and highly effective catalysts.
