Mechanistic Understanding of Oxygen Activation on Bulk Au(111) Surface Using Tip‐Enhanced Raman Spectroscopy

Author:

Cai Zhen‐Feng12ORCID,Tang Zi‐Xi3,Zhang Yao3,Kumar Naresh2ORCID

Affiliation:

1. Key Laboratory of Green Chemistry and Technology of Ministry of Education, College of Chemistry Sichuan University 29 Wangjiang Road Chengdu 610064 P. R. China

2. Department of Chemistry and Applied Biosciences ETH Zurich Vladimir-Prelog-Weg 3 Zurich CH-8093 Switzerland

3. Hefei National Laboratory for Physical Sciences at the Microscale and Synergetic Innovation Center of Quantum Information and Quantum Physics University of Science and Technology of China 230026 Hefei, Anhui P. R. China

Abstract

AbstractGaining mechanistic understanding of oxygen activation on metal surfaces is a topical area of research in surface science. However, direct investigation of on‐surface oxidation processes at the nanoscale and the empirical validation of oxygen activation pathways remain challenging for the conventional analytical tools. In this study, we applied tip‐enhanced Raman spectroscopy (TERS) to gain mechanistic insights into oxygen activation on bulk Au(111) surface. Specifically, oxidation of 4‐aminothiophenol (4‐ATP) to 4‐nitrothiophenol (4‐NTP) on Au(111) surface was investigated using hyperspectral TERS imaging. Nanoscale TERS images revealed a markedly higher oxidation efficiency in disordered 4‐ATP adlayers compared to the ordered adlayers signifying that the oxidation of 4‐ATP molecules proceeds via interaction with the on‐surface oxidative species. These results were further validated via direct oxidation of the 4‐ATP adlayers with H2O2 solution. Finally, TERS measurements of oxidized 4‐ATP adlayers in the presence of H2O18 provided the first empirical evidence for the generation of oxidative species on bulk Au(111) surface via water‐mediated activation of molecular oxygen. This study expands our mechanistic understanding of oxidation chemistry on bulk Au surface by elucidating the oxygen activation pathway.

Funder

European Research Council

Fundamental Research Funds for the Central Universities

Publisher

Wiley

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