Mechanochemically-derived iron atoms on defective boron nitride for stable propylene production.
EES Catal
; 2(6): 1263-1276, 2024 Oct 31.
Article
en En
| MEDLINE
| ID: mdl-39148890
ABSTRACT
Single-atom catalysts (SACs), possessing a uniform metal site structure, are a promising class of materials for selective oxidations of hydrocarbons. However, their design for targeted applications requires careful choice of metal-host combinations and suitable synthetic techniques. Here, we report iron atoms stabilised on defective hexagonal boron nitride (h-BN) via mechanochemical activation in a ball mill as an effective catalyst for propylene production via N2O-mediated oxidative propane dehydrogenation (N2O-ODHP), reaching 95% selectivity at 6% propane conversion and maintaining stable performance for 40 h on stream. This solvent-free synthesis allows simultaneous carrier exfoliation and surface defect generation, creating anchoring sites for catalytically-active iron atoms. The incorporation of a small metal quantity (0.5 wt%) predominantly generates a mix of atomically-dispersed Fe2+ and Fe3+ species, as confirmed by combining advanced microscopy and electron paramagnetic resonance, UV-vis and X-ray photoelectron spectroscopy analyses. Single-atom iron favours selective propylene formation, while metal oxide nanoparticles yield large quantities of CO x and cracking by-products. The lack of acidic functionalities on h-BN, hindering coke formation, and firm stabilisation of Fe sites, preventing metal sintering, ensure stable operation. These findings showcase N2O-ODHP as a promising propylene production technology and foster wider adoption of mechanochemical activation as a viable method for SACs synthesis.
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Colección:
01-internacional
Base de datos:
MEDLINE
Idioma:
En
Revista:
EES Catal
Año:
2024
Tipo del documento:
Article
Pais de publicación:
Reino Unido