1. Mechanochemically-derived iron atoms on defective boron nitride for stable propylene production.
- Author
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Beshara GM, Surin I, Agrachev M, Eliasson H, Otroshchenko T, Krumeich F, Erni R, Kondratenko EV, and Pérez-Ramírez J
- 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 N
2 O-mediated oxidative propane dehydrogenation (N2 O-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 COx 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 N2 O-ODHP as a promising propylene production technology and foster wider adoption of mechanochemical activation as a viable method for SACs synthesis., Competing Interests: The authors declare no conflict of interest., (This journal is © The Royal Society of Chemistry.)- Published
- 2024
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