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

Simon J Freakley; Qian He; Jonathan H Harrhy; Li Lu; David A Crole; David J Morgan; Edwin N Ntainjua; Jennifer K Edwards; Albert F Carley; Albina Y Borisevich; Christopher  J. Kiely; Graham J. Hutchings

doi:10.1126/science.aad5705

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

Simon J Freakley, Qian He, Jonathan H Harrhy, Li Lu, David A Crole, David J Morgan, Edwin N Ntainjua, Jennifer K Edwards, Albert F Carley, Albina Y Borisevich, Christopher J. Kiely, Graham J. Hutchings

Department of Chemistry

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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.

Original language	English
Pages (from-to)	965-968
Number of pages	4
Journal	Science
Volume	351
Issue number	6276
Early online date	26 Feb 2016
DOIs	https://doi.org/10.1126/science.aad5705
Publication status	Published - 26 Feb 2016

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This is the author's version of the work. It is posted here by permission of the AAAS for personal use, not for redistribution. The definitive version was published in Science on 26 February 2016, Vol. 351, Issue 6276, DOI: 10.1126/science.aad5705.
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Simon Freakley
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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.",

author = "Freakley, {Simon J} and Qian He and Harrhy, {Jonathan H} and Li Lu 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.}",

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language = "English",

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T1 - Palladium-tin catalysts for the direct synthesis of H2O2 with high selectivity

AU - Freakley, Simon J

AU - He, Qian

AU - Harrhy, Jonathan H

AU - Lu, Li

AU - Crole, David A

AU - Morgan, David J

AU - Ntainjua, Edwin N

AU - Edwards, Jennifer K

AU - Carley, Albert F

AU - Borisevich, Albina Y

AU - Kiely, Christopher J.

AU - Hutchings, Graham J.

PY - 2016/2/26

Y1 - 2016/2/26

N2 - 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.

AB - 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.

U2 - 10.1126/science.aad5705

DO - 10.1126/science.aad5705

M3 - Article

SN - 0036-8075

VL - 351

SP - 965

EP - 968

JO - Science

JF - Science

IS - 6276

ER -

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

Abstract

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