Rh single atoms on TiO<sub>2</sub> dynamically respond to reaction conditions by adapting their site.
basic_science · Level V
Where this comes from
- Record sourced from PubMed, PMID 31582746.
- Also identified by DOI 10.1038/s41467-019-12461-6 and PMC identifier 6776542.
- Licence recorded as CC BY.
- The licence permits redistribution, so the abstract is shown in full and the full text is available from the publisher.
Abstract
Single-atom catalysts are widely investigated heterogeneous catalysts; however, the identification of the local environment of single atoms under experimental conditions, as well as operando characterization of their structural changes during catalytic reactions are still challenging. Here, the preferred local coordination of Rh single atoms is investigated on TiO<sub>2</sub> during calcination in O<sub>2</sub>, reduction in H<sub>2</sub>, CO adsorption, and reverse water gas shift (RWGS) reaction conditions. Theoretical and experimental studies clearly demonstrate that Rh single atoms adapt their local coordination and reactivity in response to various redox conditions. Single-atom catalysts hence do not have static local coordinations, but can switch from inactive to active structure under reaction conditions, hence explaining some conflicting literature accounts. The combination of approaches also elucidates the structure of the catalytic active site during reverse water gas shift. This insight on the real nature of the active site is key for the design of high-performance catalysts.