Results
Title

In Situ Raman Study of CO Electrooxidation on Pt(hkl) Single‐Crystal Surfaces in Acidic Solution.

Authors

Su, Min; Dong, Jin‐Chao; Le, Jia‐Bo; Zhao, Yu; Yang, Wei‐Min; Yang, Zhi‐Lin; Attard, Gary; Liu, Guo‐Kun; Cheng, Jun; Wei, Yi‐Min; Tian, Zhong‐Qun; Li, Jian‐Feng

Abstract

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 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 detected 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.

Subjects

CATALYST poisoning; RAMAN spectroscopy; FUEL cells; ADSORPTION (Chemistry); ELECTROCATALYSTS; PLATINUM catalysts; SINGLE crystals; SURFACE enhanced Raman effect

Publication

Angewandte Chemie, 2020, Vol 132, Issue 52, p23760

ISSN

0044-8249

Publication type

Academic Journal

DOI

10.1002/ange.202010431