Tip-activated single-atom catalysis: CO oxidation on Au adatom on oxidized rutile TiO2 surface

Yuuki Adachi, Ján Brndiar, Martin Konôpka, Robert Turanský, Qiang Zhu, Huan Fei Wen, Yasuhiro Sugawara, Lev Kantorovich, Ivan Štich, Yan Jun Li*

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

Abstract

Single-atom catalysis of carbon monoxide oxidation on metal-oxide surfaces is crucial for greenhouse recycling, automotive catalysis, and beyond, but reports of the atomic-scale mechanism are still scarce. Here, using scanning probe microscopy, we show that charging single gold atoms on oxidized rutile titanium dioxide surface, both positively and negatively, considerably promotes adsorption of carbon monoxide. No carbon monoxide adsorption is observed on neutral gold atoms. Two different carbon monoxide adsorption geometries on gold atoms are identified. We demonstrate full control over the redox state of adsorbed gold single atoms, carbon monoxide adsorption geometry, and carbon monoxide adsorption/desorption by the atomic force microscopy tip. On charged gold atoms, we activate Eley-Rideal oxidation reaction between carbon monoxide and a neighboring oxygen adatom by the tip. Our results provide unprecedented insights into carbon monoxide adsorption and suggest that the gold dual activity for carbon monoxide oxidation after electron or hole attachment is also the key ingredient in photocatalysis under realistic conditions.

Original languageEnglish
Article numbereadi4799
JournalScience Advances
Volume9
Issue number39
DOIs
Publication statusPublished - 2023

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