The Role of Copper Speciation in the Low Temperature Oxidative Upgrading of Short Chain Alkanes over Cu/ZSM-5 Catalysts

Robert D Armstrong; Virginie Peneau; Nadine Ritterskamp; Christopher J Kiely; Stuart H Taylor; Graham J Hutchings

doi:10.1002/cphc.201701046

The Role of Copper Speciation in the Low Temperature Oxidative Upgrading of Short Chain Alkanes over Cu/ZSM-5 Catalysts

Chemphyschem. 2018 Feb 19;19(4):469-478. doi: 10.1002/cphc.201701046. Epub 2018 Jan 18.

Authors

Robert D Armstrong¹, Virginie Peneau¹, Nadine Ritterskamp¹, Christopher J Kiely², Stuart H Taylor¹, Graham J Hutchings¹

Affiliations

¹ Cardiff Catalysis Institute, School of Chemistry, Cardiff University, Park Place, Cardiff, CF10 1AQ, UK.
² Department of Materials Science and Engineering, Lehigh University, 5 East Packer Avenue, 18015-3195, Bethlehem, Pennsylvania, USA.

PMID: 29193556
DOI: 10.1002/cphc.201701046

Abstract

Partial oxidative upgrading of C₁ -C₃ alkanes over Cu/ZSM-5 catalysts prepared by chemical vapour impregnation (CVI) has been studied. The undoped ZSM-5 support is itself able to catalyse selective oxidations, for example, methane to methanol, using mild reaction conditions and the green oxidant H₂ O₂ . Addition of Cu suppresses secondary oxidation reactions, affording methanol selectivities of up to 97 %. Characterisation studies attribute this ability to population of specific Cu sites below the level of total exchange (Cu/Al<0.5). These species also show activity for radical-based methane oxidation, with productivities exceeding those of the parent zeolite supports. When tested for ethane and propane oxidation reactions, comparable trends are observed.

Keywords: Cu/ZSM-5; alkanes; chemical vapour impregnation; selective oxidation; zeolite.