Journal ArticleDOI
Switching Off Hydrogen Peroxide Hydrogenation in the Direct Synthesis Process
Jennifer K. Edwards,Benjamín Solsona,Edwin Ntainjua N,Albert Frederick Carley,Andrew A. Herzing,Andrew A. Herzing,Christopher J. Kiely,Graham J. Hutchings +7 more
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TLDR
It is shown that acid pretreatment of a carbon support for gold-palladium alloy catalysts switches off the decomposition of H2O2, and the acid-pretreated catalysts give high yields of H 2O2 with hydrogen selectivities greater than 95%.Abstract:
Hydrogen peroxide (H2O2) is an important disinfectant and bleach and is currently manufactured from an indirect process involving sequential hydrogenation/oxidation of anthaquinones. However, a direct process in which H2 and O2 are reacted would be preferable. Unfortunately, catalysts for the direct synthesis of H2O2 are also effective for its subsequent decomposition, and this has limited their development. We show that acid pretreatment of a carbon support for gold-palladium alloy catalysts switches off the decomposition of H2O2. This treatment decreases the size of the alloy nanoparticles, and these smaller nanoparticles presumably decorate and inhibit the sites for the decomposition reaction. Hence, when used in the direct synthesis of H2O2, the acid-pretreated catalysts give high yields of H2O2 with hydrogen selectivities greater than 95%.read more
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High-efficiency oxygen reduction to hydrogen peroxide catalysed by oxidized carbon materials
Zhiyi Lu,Guangxu Chen,Samira Siahrostami,Zhihua Chen,Kai Liu,Jin Xie,Lei Liao,Tong Wu,Dingchang Lin,Yayuan Liu,Thomas F. Jaramillo,Jens K. Nørskov,Jens K. Nørskov,Yi Cui,Yi Cui +14 more
TL;DR: In this article, a facile and general approach to catalyst development via surface oxidation of abundant carbon materials to significantly enhance both the activity and selectivity for H2O2 production by electrochemical oxygen reduction was demonstrated.
Journal ArticleDOI
Designing bimetallic catalysts for a green and sustainable future
Meenakshisundaram Sankar,Nikolaos Dimitratos,Nikolaos Dimitratos,Peter J. Miedziak,Peter P. Wells,Peter P. Wells,Christopher J. Kiely,Graham J. Hutchings +7 more
TL;DR: A specific objective of this review article is to motivate researchers to synthesize some of the "designer" bimetallic catalysts with specific nanostructures, inspired from recent advances in the area of materials chemistry, and to utilize them for the transformation of biomass derived materials that are very complex and pose different challenges compared to those of simple organic molecules.
Journal ArticleDOI
Enabling direct H2O2 production through rational electrocatalyst design
Samira Siahrostami,Arnau Verdaguer-Casadevall,Mohammadreza Karamad,Davide Deiana,Paolo Malacrida,Björn Wickman,Björn Wickman,María Escudero-Escribano,Elisa Antares Paoli,Rasmus Frydendal,Thomas Willum Hansen,Ib Chorkendorff,Ifan E. L. Stephens,Jan Rossmeisl +13 more
TL;DR: Electrochemical measurements on Pt-Hg nanoparticles show more than an order of magnitude improvement in mass activity, that is, A g(-1) precious metal, for H2O2 production, over the best performing catalysts in the literature.
Journal ArticleDOI
Catalysis by Supported Gold Nanoparticles: Beyond Aerobic Oxidative Processes
Journal ArticleDOI
Solvent-Free Oxidation of Primary Carbon-Hydrogen Bonds in Toluene Using Au-Pd Alloy Nanoparticles
Lokesh Kesavan,Ramchandra Tiruvalam,Mohd Hasbi Ab. Rahim,Mohd Izham Saiman,Dan I. Enache,Robert Leyshon Jenkins,Nikolaos Dimitratos,Jose Antonio Lopez-Sanchez,Stuart Hamilton Taylor,David W. Knight,Christopher J. Kiely,Graham J. Hutchings +11 more
TL;DR: It is reported here that supported gold-palladium nanoparticles on carbon or TiO2 are active for the oxidation of the primary carbon-hydrogen bonds in toluene and related molecules, giving high selectivities to benzyl benzoate under mild solvent-free conditions.
References
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Journal ArticleDOI
Identification of Active Gold Nanoclusters on Iron Oxide Supports for CO Oxidation
Andrew A. Herzing,Christopher J. Kiely,Albert Frederick Carley,Philip Landon,Graham J. Hutchings +4 more
TL;DR: High catalytic activity for carbon monoxide oxidation is correlated with the presence of bilayer clusters that are ∼0.5 nanometer in diameter and contain only ∼10 gold atoms, consistent with that demonstrated previously with the use of model catalyst systems.
Journal ArticleDOI
Selective oxidation with dioxygen by gold nanoparticle catalysts derived from 55-atom clusters
Mark Turner,Vladimir B. Golovko,Vladimir B. Golovko,Owain P. H. Vaughan,Pavel Abdulkin,Ángel Berenguer-Murcia,Mintcho S. Tikhov,Brian F. G. Johnson,Richard M. Lambert +8 more
TL;DR: The observations suggest that catalytic activity arises from the altered electronic structure intrinsic to small gold nanoparticles, and that the use of 55-atom gold clusters may prove a viable route to the synthesis of robust gold catalysts suited to practical application.
Journal ArticleDOI
The Promotional Effect of Gold in Catalysis by Palladium-Gold
TL;DR: Acetoxylation of ethylene to vinyl acetate was used to investigate the mechanism of the promotional effect of gold (Au) in a palladium (Pd)-Au alloy catalyst, demonstrating that the critical reaction site for VA synthesis consists of two noncontiguous, suitably spaced, Pd monomers.
Journal ArticleDOI
Direct synthesis of hydrogen peroxide from H2 and O2 using TiO2-supported Au-Pd catalysts
Jennifer K. Edwards,Benjamín Solsona,Philip Landon,Albert Frederick Carley,Andrew A. Herzing,Christopher J. Kiely,Graham J. Hutchings +6 more
TL;DR: In this paper, the direct synthesis of H2O2 at low temperature (2 °C) from H2 and O2 using TiO2-supported Au, Pd, and Au-Pd catalysts is discussed.
Journal ArticleDOI
Direct synthesis of hydrogen peroxide from H2 and O2 using Pd and Au catalysts
Philip Landon,Paul J. Collier,Albert Frederick Carley,David Chadwick,Adam J. Papworth,Andrew Burrows,Christopher J. Kiely,Graham J. Hutchings +7 more
TL;DR: In this paper, a detailed study of the factors influencing the formation and decomposition of hydrogen peroxide is presented for a Pd/sulfonated carbon catalyst in a methanol/water solvent.