Unraveling the coordination structure-performance relationship in Pt<sub>1</sub>/Fe<sub>2</sub>O<sub>3</sub> single-atom catalyst.
basic_science · Level V
Where this comes from
- Record sourced from PubMed, PMID 31582748.
- Also identified by DOI 10.1038/s41467-019-12459-0 and PMC identifier 6776505.
- 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
Heterogeneous single-atom catalyst (SAC) opens a unique entry to establishing structure-performance relationship at the molecular level similar to that in homogeneous catalysis. The challenge lies in manipulating the coordination chemistry of single atoms without changing single-atom dispersion. Here, we develop an efficient synthetic method for SACs by using ethanediamine to chelate Pt cations and then removing the ethanediamine by a rapid thermal treatment (RTT) in inert atmosphere. The coordination chemistry of Pt single atoms on a Fe<sub>2</sub>O<sub>3</sub> support is finely tuned by merely adjusting the RTT temperature. With the decrease in Pt-O coordination number, the oxidation state of Pt decreases, and consequently the hydrogenation activity increases to a record level without loss of chemoselectivity. The tunability of the local coordination chemistry, oxidation states of the metal, and the catalytic performance of single atoms reveals the unique role of SACs as a bridge between heterogeneous and homogeneous catalysis.