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

electron Microscopy and Microanalysis

Research output: Contribution to journal › Article › peer-review

487 Scopus citations

Abstract

The direct synthesis of hydrogen peroxide (H₂O₂) from H₂ and O₂represents 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 secondmetal 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
DOIs	https://doi.org/10.1126/science.aad5705
State	Published - Feb 26 2016

Funding

Supported by NSF Major Research Instrumentation Program grant MRI/DMR-1040229 (C.J.K.); the U.S. Department of Energy, Office of Science, Basic Energy Sciences, Materials Sciences and Engineering Division (Q.H. and A.Y.B.); a user project supported by Oak Ridge National Laboratory’s Center for Nanophase Materials Sciences, sponsored by the Scientific User Facilities Division, Office of Science, Basic Energy Sciences, U.S. Department of Energy; and European Research Council grant ERC-2011-ADG, grant agreement no. 291319, acronym "AFTERTHEGOLDRUSH" (G.J.H.). The data contained in this paper are archived at DOI: 10.17035/ d.2016.0008119507.

Funders	Funder number
Oak Ridge National Laboratory
Scientific User Facilities Division
U.S. Department of Energy
Office of Science
Basic Energy Sciences
Division of Materials Sciences and Engineering
Engineering and Physical Sciences Research Council	EP/L027240/1
European Research Council	ERC-2011-ADG, 2016.0008119507, 291319
Neurosciences Foundation	MRI/DMR-1040229

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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 O2represents 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 secondmetal 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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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 O2represents 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 secondmetal 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 O2represents 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 secondmetal 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.

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

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