Optimising surface d charge of AuPd nanoalloy catalysts for enhanced catalytic activity.
basic_science · Level V
Where this comes from
- Record sourced from PubMed, PMID 30926804.
- Also identified by DOI 10.1038/s41467-019-09421-5 and PMC identifier 6441046.
- 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
Understanding the catalytic mechanism of bimetallic nanocatalysts remains challenging. Here, we adopt an adsorbate mediated thermal reduction approach to yield monodispersed AuPd catalysts with continuous change of the Pd-Au coordination numbers embedded in a mesoporous carbonaceous matrix. The structure of nanoalloys is well-defined, allowing for a direct determination of the structure-property relationship. The results show that the Pd single atom and dimer are the active sites for the base-free oxidation of primary alcohols. Remarkably, the d-orbital charge on the surface of Pd serves as a descriptor to the adsorbate states and hence the catalytic performance. The maximum d-charge gain occurred in a composition with 33-50 at% Pd corresponds to up to 9 times enhancement in the reaction rate compared to the neat Pd. The findings not only open an avenue towards the rational design of catalysts but also enable the identification of key steps involved in the catalytic reactions.