Atomically synergistic Zn-Cr catalyst for iso-stoichiometric co-conversion of ethane and CO<sub>2</sub> to ethylene and CO.
basic_science · Level V
Where this comes from
- Record sourced from PubMed, PMID 38291043.
- Also identified by DOI 10.1038/s41467-024-44918-8 and PMC identifier 10828418.
- 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
Developing atomically synergistic bifunctional catalysts relies on the creation of colocalized active atoms to facilitate distinct elementary steps in catalytic cycles. Herein, we show that the atomically-synergistic binuclear-site catalyst (ABC) consisting of [Formula: see text]-O-Cr<sup>6+</sup> on zeolite SSZ-13 displays unique catalytic properties for iso-stoichiometric co-conversion of ethane and CO<sub>2</sub>. Ethylene selectivity and utilization of converted CO<sub>2</sub> can reach 100 % and 99.0% under 500 °C at ethane conversion of 9.6%, respectively. In-situ/ex-situ spectroscopic studies and DFT calculations reveal atomic synergies between acidic Zn and redox Cr sites. [Formula: see text] ([Formula: see text]) sites facilitate β-C-H bond cleavage in ethane and the formation of Zn-H<sup>δ-</sup> hydride, thereby the enhanced basicity promotes CO<sub>2</sub> adsorption/activation and prevents ethane C-C bond scission. The redox Cr site accelerates CO<sub>2</sub> dissociation by replenishing lattice oxygen and facilitates H<sub>2</sub>O formation/desorption. This study presents the advantages of the ABC concept, paving the way for the rational design of novel advanced catalysts.