Tip-activated single-atom catalysis: CO oxidation on Au adatom on oxidized rutile TiO 2 surface.

Autor: Adachi Y; Department of Applied Physics, Osaka University, 2-1 Yamadaoka, Suita, Osaka 565-0871, Japan., Brndiar J; Institute of Informatics, Slovak Academy of Sciences, 845 07 Bratislava, Slovakia., Konôpka M; Faculty of Electrical Engineering and Information Technology, Institute of Nuclear and Physical Engineering, Slovak University of Technology in Bratislava, 812 19 Bratislava, Slovakia., Turanský R; Institute of Physics, Slovak Academy of Sciences, 845 11 Bratislava, Slovakia., Zhu Q; Department of Applied Physics, Osaka University, 2-1 Yamadaoka, Suita, Osaka 565-0871, Japan., Wen HF; Key Laboratory of Instrumentation Science and Dynamic Measurement, School of Instrument and Electronics, North University of China, Taiyuan, Shanxi 030051, China., Sugawara Y; Department of Applied Physics, Osaka University, 2-1 Yamadaoka, Suita, Osaka 565-0871, Japan., Kantorovich L; Department of Physics, School of Natural and Mathematical Sciences, King's College London, The Strand, London WC2R 2LS, UK., Štich I; Institute of Informatics, Slovak Academy of Sciences, 845 07 Bratislava, Slovakia.; Institute of Physics, Slovak Academy of Sciences, 845 11 Bratislava, Slovakia.; Faculty of Natural Sciences, University of Ss. Cyril and Methodius, 917 01 Trnava, Slovakia., Li YJ; Department of Applied Physics, Osaka University, 2-1 Yamadaoka, Suita, Osaka 565-0871, Japan.
Jazyk: angličtina
Zdroj: Science advances [Sci Adv] 2023 Sep 29; Vol. 9 (39), pp. eadi4799. Date of Electronic Publication: 2023 Sep 27.
DOI: 10.1126/sciadv.adi4799
Abstrakt: 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.
Databáze: MEDLINE