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Title: Palladium-tin catalysts for the direct synthesis of H 2O 2 with high selectivity

Abstract

The direct synthesis of hydrogen peroxide (H 2O 2 ) from H 2 and O 2 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 H 2O 2 . 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 H 2O 2 production that do not contain gold.

Authors:
 [1];  [2];  [1];  [3];  [1];  [1];  [1];  [1];  [1];  [4];  [3];  [1]
  1. Cardiff University, Cardiff (United Kingdom)
  2. Lehigh Univ., Bethlehem, PA (United States); Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Materials Science & Technology Division
  3. Lehigh Univ., Bethlehem, PA (United States)
  4. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Materials Science & Technology Division; Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Science
Publication Date:
Research Org.:
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS)
Sponsoring Org.:
USDOE; European Research Council (ERC)
OSTI Identifier:
1355853
Alternate Identifier(s):
OSTI ID: 1240555
Grant/Contract Number:  
AC05-00OR22725; ERC-2011-ADG
Resource Type:
Published Article
Journal Name:
Science
Additional Journal Information:
Journal Volume: 351; Journal Issue: 6276; Journal ID: ISSN 0036-8075
Publisher:
AAAS
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Freakley, Simon J., He, Qian, Harrhy, Jonathan H., Lu, Li, Crole, David A., Morgan, David J., Ntainjua, Edwin N., Edwards, Jennifer K., Carley, Albert F., Borisevich, Albina Y., Kiely, Christopher J., and Hutchings, Graham J. Palladium-tin catalysts for the direct synthesis of H2O2 with high selectivity. United States: N. p., 2016. Web. doi:10.1126/science.aad5705.
Freakley, Simon J., He, Qian, Harrhy, Jonathan H., Lu, Li, Crole, David A., Morgan, David J., Ntainjua, Edwin N., Edwards, Jennifer K., Carley, Albert F., Borisevich, Albina Y., Kiely, Christopher J., & Hutchings, Graham J. Palladium-tin catalysts for the direct synthesis of H2O2 with high selectivity. United States. doi:10.1126/science.aad5705.
Freakley, Simon J., He, Qian, Harrhy, Jonathan H., Lu, Li, Crole, David A., Morgan, David J., Ntainjua, Edwin N., Edwards, Jennifer K., Carley, Albert F., Borisevich, Albina Y., Kiely, Christopher J., and Hutchings, Graham J. Thu . "Palladium-tin catalysts for the direct synthesis of H2O2 with high selectivity". United States. doi:10.1126/science.aad5705.
@article{osti_1355853,
title = {Palladium-tin catalysts for the direct synthesis of H2O2 with high selectivity},
author = {Freakley, Simon J. and He, Qian and Harrhy, Jonathan H. and Lu, Li and Crole, David A. and Morgan, David J. and Ntainjua, Edwin N. and Edwards, Jennifer K. and Carley, Albert F. and Borisevich, Albina Y. and Kiely, Christopher J. and Hutchings, Graham J.},
abstractNote = {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.},
doi = {10.1126/science.aad5705},
journal = {Science},
number = 6276,
volume = 351,
place = {United States},
year = {2016},
month = {2}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record
DOI: 10.1126/science.aad5705

Citation Metrics:
Cited by: 41 works
Citation information provided by
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Works referenced in this record:

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The effect of heat treatment on the performance and structure of carbon-supported Au–Pd catalysts for the direct synthesis of hydrogen peroxide
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Strategies for Designing Supported Gold–Palladium Bimetallic Catalysts for the Direct Synthesis of Hydrogen Peroxide
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    Works referencing / citing this record:

    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

    • Rinn, Niklas; Hanau, Katharina; Guggolz, Lukas
    • Zeitschrift für anorganische und allgemeine Chemie, Vol. 643, Issue 21
    • DOI: 10.1002/zaac.201700252