title: Palladium-tin catalysts for the direct synthesis of H₂O₂ with high selectivity.
abstract: The direct synthesis of hydrogen peroxide (H2O2) from H2 and O2 represents a potentially atom-efficient alternative to the current industrial indirect process. We show that the addition of tin to palladium catalysts coupled with an appropriate heat treatment cycle switches off the sequential hydrogenation and decomposition reactions, enabling selectivities of >95% toward H2O2. This effect arises from a tin oxide surface layer that encapsulates small Pd-rich particles while leaving larger Pd-Sn alloy particles exposed. We show that this effect is a general feature for oxide-supported Pd catalysts containing an appropriate second metal oxide component, and we set out the design principles for producing high-selectivity Pd-based catalysts for direct H2O2 production that do not contain gold.
authors.affiliation: Cardiff Catalysis Institute and School of Chemistry, Cardiff University, Cardiff CF10 3AT, UK. hutch@cf.ac.uk freakleys@cf.ac.uk.
authors.forename: Simon J
authors.initials: SJ
authors.lastname: Freakley
authors.affiliation: Department of Materials Science and Engineering, Lehigh University, Bethlehem, PA 18015, USA. Materials Science and Technology Division, Oak Ridge National Laboratory, Oak Ridge, TN 37831, USA.
authors.forename: Qian
authors.initials: Q
authors.lastname: He
authors.affiliation: Cardiff Catalysis Institute and School of Chemistry, Cardiff University, Cardiff CF10 3AT, UK.
authors.forename: Jonathan H
authors.initials: JH
authors.lastname: Harrhy
authors.affiliation: Department of Materials Science and Engineering, Lehigh University, Bethlehem, PA 18015, USA.
authors.forename: Li
authors.initials: L
authors.lastname: Lu
authors.affiliation: Cardiff Catalysis Institute and School of Chemistry, Cardiff University, Cardiff CF10 3AT, UK.
authors.forename: David A
authors.initials: DA
authors.lastname: Crole
authors.affiliation: Cardiff Catalysis Institute and School of Chemistry, Cardiff University, Cardiff CF10 3AT, UK.
authors.forename: David J
authors.initials: DJ
authors.lastname: Morgan
authors.affiliation: Cardiff Catalysis Institute and School of Chemistry, Cardiff University, Cardiff CF10 3AT, UK.
authors.forename: Edwin N
authors.initials: EN
authors.lastname: Ntainjua
authors.affiliation: Cardiff Catalysis Institute and School of Chemistry, Cardiff University, Cardiff CF10 3AT, UK.
authors.forename: Jennifer K
authors.initials: JK
authors.lastname: Edwards
authors.affiliation: Cardiff Catalysis Institute and School of Chemistry, Cardiff University, Cardiff CF10 3AT, UK.
authors.forename: Albert F
authors.initials: AF
authors.lastname: Carley
authors.affiliation: Materials Science and Technology Division, Oak Ridge National Laboratory, Oak Ridge, TN 37831, USA. Center for Nanophase Materials Sciences, Oak Ridge National Laboratory, Oak Ridge, TN 37831, USA.
authors.forename: Albina Y
authors.initials: AY
authors.lastname: Borisevich
authors.affiliation: Department of Materials Science and Engineering, Lehigh University, Bethlehem, PA 18015, USA.
authors.forename: Christopher J
authors.initials: CJ
authors.lastname: Kiely
authors.affiliation: Cardiff Catalysis Institute and School of Chemistry, Cardiff University, Cardiff CF10 3AT, UK. hutch@cf.ac.uk freakleys@cf.ac.uk.
authors.forename: Graham J
authors.initials: GJ
authors.lastname: Hutchings