title: High performing and stable supported nano-alloys for the catalytic hydrogenation of levulinic acid to γ-valerolactone.
abstract: The catalytic hydrogenation of levulinic acid, a key platform molecule in many biorefinery schemes, into γ-valerolactone is considered as one of the pivotal reactions to convert lignocellulose-based biomass into renewable fuels and chemicals. Here we report on the development of highly active, selective and stable supported metal catalysts for this reaction and on the beneficial effects of metal nano-alloying. Bimetallic random alloys of gold-palladium and ruthenium-palladium supported on titanium dioxide are prepared with a modified metal impregnation method. Gold-palladium/titanium dioxide shows a marked,~27-fold increase in activity (that is, turnover frequency of 0.1 s(-1)) compared with its monometallic counterparts. Although ruthenium-palladium/titanium dioxide is not only exceptionally active (that is, turnover frequency of 0.6 s(-1)), it shows excellent, sustained selectivity to γ-valerolactone (99%). The dilution and isolation of ruthenium by palladium is thought to be responsible for this superior catalytic performance. Alloying, furthermore, greatly improves the stability of both supported nano-alloy catalysts.
authors.affiliation: Inorganic Chemistry and Catalysis, Debye Institute for Nanomaterials Science, Utrecht University, Universiteitsweg 99, 3584 CG Utrecht, The Netherlands.
authors.forename: Wenhao
authors.initials: W
authors.lastname: Luo
authors.affiliation: Inorganic Chemistry and Catalysis, Debye Institute for Nanomaterials Science, Utrecht University, Universiteitsweg 99, 3584 CG Utrecht, The Netherlands.
authors.forename: Meenakshisundaram
authors.initials: M
authors.lastname: Sankar
authors.affiliation: 1] Inorganic Chemistry and Catalysis, Debye Institute for Nanomaterials Science, Utrecht University, Universiteitsweg 99, 3584 CG Utrecht, The Netherlands [2] UK Catalysis Hub, Research Complex at Harwell, Rutherford Appleton Laboratory, Oxfordshire OX11 0QX, UK [3] Department of Chemistry, University College London, 20 Gordon Street, London WC1H 0AJ, UK.
authors.forename: Andrew M
authors.initials: AM
authors.lastname: Beale
authors.affiliation: Department of Materials Science and Engineering, Lehigh University, 5 East Packer Avenue, Bethlehem, Pennsylvania 18015, USA.
authors.forename: Qian
authors.initials: Q
authors.lastname: He
authors.affiliation: Department of Materials Science and Engineering, Lehigh University, 5 East Packer Avenue, Bethlehem, Pennsylvania 18015, USA.
authors.forename: Christopher J
authors.initials: CJ
authors.lastname: Kiely
authors.affiliation: Inorganic Chemistry and Catalysis, Debye Institute for Nanomaterials Science, Utrecht University, Universiteitsweg 99, 3584 CG Utrecht, The Netherlands.
authors.forename: Pieter C A
authors.initials: PC
authors.lastname: Bruijnincx
authors.affiliation: Inorganic Chemistry and Catalysis, Debye Institute for Nanomaterials Science, Utrecht University, Universiteitsweg 99, 3584 CG Utrecht, The Netherlands.
authors.forename: Bert M
authors.initials: BM
authors.lastname: Weckhuysen