Operando elucidation of hydrogen production mechanisms on sub-nanometric high-entropy metallenes.
basic_science · Level V
Where this comes from
- Record sourced from PubMed, PMID 39587090.
- Also identified by DOI 10.1038/s41467-024-54589-0 and PMC identifier 11589590.
- Licence recorded as CC BY-NC-ND.
- Because redistribution is not established, this page shows the abstract only. Follow the links below for the full text.
Abstract
Precise morphological control and identification of structure-property relationships pose formidable challenges for high-entropy alloys, severely limiting their rational design and application in multistep and tandem reactions. Herein, we report the synthesis of sub-nanometric high-entropy metallenes with up to eight metallic elements via a one-pot wet-chemical approach. The PdRhMoFeMn high-entropy metallenes exhibit high electrocatalytic hydrogen evolution performances with 6, 23, and 26 mV overpotentials at -10 mA cm<sup>-2</sup> in acidic, neutral, and alkaline media, respectively, and high stability. The electrochemical measurements, theoretical simulations, and operando X-ray absorption spectroscopy reveal the actual active sites along with their dynamics and synergistic mechanisms in various electrolytes. Specially, Mn sites have strong binding affinity to hydroxyl groups, which enhances the water dissociation process at Pd sites with low energy barrier while Rh sites with optimal hydrogen adsorption free energy accelerate hydride coupling, thereby markedly boosting its intrinsic ability for hydrogen production.