Resolving one of the holy grails of catalysis: Direct nonoxidative methane conversion to ethylene over plasma-assisted atomically dispersed Pt catalyst

Abstract

One of the holy grails of catalysis - direct nonoxidative methane conversion to ethylene is resolved in this study using dielectric barrier discharge plasma (DBDP) assisted catalysis. Motivated by the formation of ethane and very low amount of ethylene in the DBDP over acid or base treated kaolin supported Ni and oxalate ligand functionalized Ni in CO2 reforming of methane wherein Ni catalysts that were calcined at 800 °C showing higher methane conversion (XCH4), ethylene to ethane (C2 = /C2–) ratio, and hydrogen yield (YH2). A novel CeO2 confined atomically dispersed Pt supported on oxalate ligand functionalized Cu modified zeolite Y catalyst (PtCe/CuX-ZY) was synthesized to exhibit strong-metal-support interaction, which rendered the d-band center far away from the Fermi level, densification, and localization of d electrons thus weakening the adsorption of C2H4 upon formation to prevent subsequent hydrogenation to ethane. The novel PtCe/CuX-ZY catalyst showed an impressively high average XCH4, YC2H4, and YH2 of 73.5%, 23.9%, and 33.8%, respectively with a high C2 = /C2– ratio of ca. 12.3 compared to an average of 0.032 observed over Ni-based catalysts. This finding is impressive and opened up a further investigation in both academia and the industry.