skip to main content
OSTI.GOV title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Palladium-tin catalysts for the direct synthesis of H2O2 with high selectivity

Journal Article · · Science

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. In conclusion, 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.

Research Organization:
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS)
Sponsoring Organization:
USDOE; European Research Council (ERC)
Grant/Contract Number:
AC05-00OR22725; ERC-2011-ADG
OSTI ID:
1355853
Alternate ID(s):
OSTI ID: 1240555
Journal Information:
Science, Journal Name: Science Vol. 351 Journal Issue: 6276; ISSN 0036-8075
Publisher:
American Association for the Advancement of Science (AAAS)Copyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 366 works
Citation information provided by
Web of Science

References (21)

Palladium, Palladium–Tin, and Palladium–Silver Catalysts in the Selective Hydrogenation of Hexadienes: TPR, Mössbauer, and Infrared Studies of Adsorbed CO journal October 2000
Electronic structure of tin oxides: High-resolution study of XPS and Auger spectra: ELECTRONIC STRUCTURE OF TIN OXIDES journal July 1995
The direct formation of H 2 O 2 from H 2 and O 2 over palladium catalysts journal May 2003
Evidence for the Role of Colloidal Palladium in the Catalytic Formation of H2O2 from H2 and O2 journal March 2002
Effect of acid pre-treatment on AuPd/SiO 2 catalysts for the direct synthesis of hydrogen peroxide journal January 2013
Formation from direct oxidation of H2 and destruction by decomposition/hydrogenation of H2O2 over Pd/C catalyst in aqueous medium containing different acids and halide anions journal February 2007
High resolution photoemission and Auger parameter studies of electronic structure of tin oxides
  • Kövér, L.; Moretti, G.; Kovács, Zs.
  • Journal of Vacuum Science & Technology A: Vacuum, Surfaces, and Films, Vol. 13, Issue 3 https://doi.org/10.1116/1.579568
journal May 1995
The effect of heat treatment on the performance and structure of carbon-supported Au–Pd catalysts for the direct synthesis of hydrogen peroxide journal August 2012
Formation of different promoted metallic phases in PtFe and PtSn catalysts supported on carbonaceous materials used for selective hydrogenation journal October 2013
?Catalytically active Au on Titania:? yet another example of a strong metal support interaction (SMSI)? journal January 2005
Switching Off Hydrogen Peroxide Hydrogenation in the Direct Synthesis Process journal February 2009
Selective hydrogenation of 1,3-butadiene over Pd and Pd–Sn catalysts supported on different phases of alumina journal April 2011
Strategies for Designing Supported Gold–Palladium Bimetallic Catalysts for the Direct Synthesis of Hydrogen Peroxide journal October 2013
Direct Synthesis of Hydrogen Peroxide and Benzyl Alcohol Oxidation Using Au−Pd Catalysts Prepared by Sol Immobilization journal November 2010
Metal−Oxide Interfacial Reactions:  Encapsulation of Pd on TiO 2 (110) journal January 2005
Interaction of nanostructured metal overlayers with oxide surfaces journal November 2007
Electron spectroscopic investigation of polymers and glasses journal January 1997
Direct synthesis of hydrogen peroxide from H2 and O2 using TiO2-supported Au–Pd catalysts journal November 2005
Strong metal-support interactions. Group 8 noble metals supported on titanium dioxide journal January 1978
Palladium and Gold-Palladium Catalysts for the Direct Synthesis of Hydrogen Peroxide journal September 2008
Strong metal-support interactions journal November 1987

Cited By (46)

Moving Frontiers in Transition Metal Catalysis: Synthesis, Characterization and Modeling journal February 2019
Solar‐Driven Production of Hydrogen Peroxide from Water and Dioxygen journal February 2018
Trigonal Bipyramidal Metalselenide Clusters with Palladium and Tin Atoms in Various Positions: Trigonal Bipyramidal Metalselenide Clusters with Palladium and Tin Atoms in Various Positions journal September 2017
Tuning of catalytic sites in Pt/TiO2 catalysts for the chemoselective hydrogenation of 3-nitrostyrene journal September 2019
“Naked” Magnetically Recyclable Mesoporous Au-γ-Fe 2 O 3 Nanocrystal Clusters: A Highly Integrated Catalyst System journal January 2017
Role of Charge Density Wave in Monatomic Assembly in Transition Metal Dichalcogenides journal February 2019
Crafting Mussel‐Inspired Metal Nanoparticle‐Decorated Ultrathin Graphitic Carbon Nitride for the Degradation of Chemical Pollutants and Production of Chemical Resources journal January 2019
High-Temperature Atomic Mixing toward Well-Dispersed Bimetallic Electrocatalysts journal July 2018
Selective Electrochemical H 2 O 2 Production through Two-Electron Oxygen Electrochemistry journal September 2018
Hybrid Palladium Nanoparticles for Direct Hydrogen Peroxide Synthesis: The Key Role of the Ligand journal December 2016
Supramolecular Tuning Enables Selective Oxygen Reduction Catalyzed by Cobalt Porphyrins for Direct Electrosynthesis of Hydrogen Peroxide journal January 2020
Supramolecular Tuning Enables Selective Oxygen Reduction Catalyzed by Cobalt Porphyrins for Direct Electrosynthesis of Hydrogen Peroxide journal January 2020
Surface/Interfacial Catalysis of (Metal)/Oxide System: Structure and Performance Control journal March 2018
Recent Advances in the Direct Synthesis of H 2 O 2 journal October 2018
Highly Active and Stable Pd−GaO x /Al 2 O 3 Catalysts Derived from Intermetallic Pd 5 Ga 3 Nanocrystals for Methane Combustion journal November 2018
Aqueous‐Phase Selective Oxidation of Methane with Oxygen over Iron Salts and Pd/C in the Presence of Hydrogen journal July 2019
Doping Carbon Nitride Quantum Dots into Melamine‐Silver Matrix: An Efficient Photocatalyst with Tunable Morphology and Photocatalysis for H 2 O 2 Evolution under Visible Light journal January 2020
Direct and Selective Synthesis of Hydrogen Peroxide over Palladium-Tellurium Catalysts at Ambient Pressure journal August 2017
2 D Hybrid of Ni‐LDH Chips on Carbon Nanosheets as Cathode of Zinc–Air Battery for Electrocatalytic Conversion of O 2 into H 2 O 2 journal March 2020
Effects of the Facet Orientation of γ-Al 2 O 3 Support on the Direct Synthesis of H 2 O 2 Catalyzed by Pd Nanoparticles: Effects of the Facet Orientation of γ-Al 2 O 3 Support on the Direct Synthesis of H 2 O 2 Catalyzed by Pd Nanoparticles journal April 2018
Bimetallic Pd‐Sn Nanocatalysts for Selective Synthesis of Amines and Imines in Water journal January 2020
Promoting the Direct H 2 O 2 Generation Catalysis by Using Hollow Pd-Sn Intermetallic Nanoparticles journal March 2018
Catalytically Active Bacterial Nanocellulose-Based Ultrafiltration Membrane journal March 2018
Tailoring the Electrochemical Production of H 2 O 2 : Strategies for the Rational Design of High‐Performance Electrocatalysts journal September 2019
Suzuki–Miyaura reaction and solventfree oxidation of benzyl alcohol by Pd/nitrogen-doped CNTs catalyst journal August 2018
A chemo-enzymatic oxidation cascade to activate C–H bonds with in situ generated H2O2 journal September 2019
High-efficiency oxygen reduction to hydrogen peroxide catalysed by oxidized carbon materials journal January 2018
Control of metal-support interactions in heterogeneous catalysts to enhance activity and selectivity journal November 2019
Soft chemistry of ion-exchangeable layered metal oxides journal January 2018
Enhancement of catalytic activity of Pd-PVP colloid for direct H 2 O 2 synthesis from H 2 and O 2 in water with addition of 0.5 atom% Pt or Ir journal January 2018
Highly effective electrosynthesis of hydrogen peroxide from oxygen on a redox-active cationic covalent triazine network journal January 2018
An etching-assisted route for fast and large-scale fabrication of non-layered palladium nanosheets journal January 2018
Kinetics, energetics, and size dependence of the transformation from Pt to ordered PtSn intermetallic nanoparticles journal January 2019
Understanding the high activity of mildly reduced graphene oxide electrocatalysts in oxygen reduction to hydrogen peroxide journal January 2019
Highly efficient hydrogen peroxide direct synthesis over a hierarchical TS-1 encapsulated subnano Pd/PdO hybrid journal January 2019
Porous organic polymer with in situ generated palladium nanoparticles as a phase-transfer catalyst for Sonogashira cross-coupling reaction in water journal January 2019
Hollow titanosilicate nanospheres encapsulating PdAu alloy nanoparticles as reusable high-performance catalysts for a H 2 O 2 -mediated one-pot oxidation reaction journal January 2019
One minute from pristine carbon to an electrocatalyst for hydrogen peroxide production journal January 2019
Direct synthesis of hydrogen peroxide in water at ambient temperature
  • Crole, David A.; Freakley, Simon J.; Edwards, Jennifer K.
  • Proceedings of the Royal Society A: Mathematical, Physical and Engineering Sciences, Vol. 472, Issue 2190 https://doi.org/10.1098/rspa.2016.0156
journal June 2016
Direct electrosynthesis of pure aqueous H 2 O 2 solutions up to 20% by weight using a solid electrolyte journal October 2019
Recent Advances in the Direct Synthesis of Hydrogen Peroxide Using Chemical Catalysis—A Review journal September 2018
Boosting the Characterization of Heterogeneous Catalysts for H2O2 Direct Synthesis by Infrared Spectroscopy journal January 2019
Looking for the “Dream Catalyst” for Hydrogen Peroxide Production from Hydrogen and Oxygen journal March 2019
Facile Fabrication of Metal Oxide Based Catalytic Electrodes by AC Plasma Deposition and Electrochemical Detection of Hydrogen Peroxide journal October 2019
An Efficient Leaching of Palladium from Spent Catalysts through Oxidation with Fe(III) journal April 2019
Supported Bimetallic AuPd Nanoparticles as a Catalyst for the Selective Hydrogenation of Nitroarenes journal September 2018

Similar Records

Methane Aromatization in a Membrane Reactor
Technical Report · Tue Jan 22 00:00:00 EST 2019 · OSTI ID:1355853

Alumina-supported bimetallics of palladium alloyed with germanium, tin, lead, or antimony from organometallic precursors I. Preparation and characterization
Journal Article · Fri Sep 01 00:00:00 EDT 1989 · Journal of Catalysis; (USA) · OSTI ID:1355853

PALLADIUM DOPED TIN OXIDE BASED HYDROGEN GAS SENSORS FOR SAFETY APPLICATIONS
Journal Article · Fri Apr 09 00:00:00 EDT 2010 · AIP Conference Proceedings · OSTI ID:1355853