Low-temperature carbon monoxide oxidation catalysed by regenerable atomically dispersed palladium on alumina

Eric J. Peterson; Andrew T. DeLaRiva; Sen Lin; Ryan S. Johnson; Hua Guo; Jeffrey T. Miller; Ja Hun Kwak; Charles H.F. Peden; Boris Kiefer; Lawrence F. Allard; Fabio H. Ribeiro; Abhaya K. Datye

doi:10.1038/ncomms5885

Low-temperature carbon monoxide oxidation catalysed by regenerable atomically dispersed palladium on alumina

Eric J. Peterson, Andrew T. DeLaRiva, Sen Lin, Ryan S. Johnson, Hua Guo, Jeffrey T. Miller, Ja Hun Kwak, Charles H.F. Peden, Boris Kiefer, Lawrence F. Allard, Fabio H. Ribeiro, Abhaya K. Datye

Nuclear Energy Materials Microanalysis

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

513 Scopus citations

Abstract

Catalysis by single isolated atoms of precious metals has attracted much recent interest, as it promises the ultimate in atom efficiency. Most previous reports are on reducible oxide supports. Here we show that isolated palladium atoms can be catalytically active on industrially relevant γ-alumina supports. The addition of lanthanum oxide to the alumina, long known for its ability to improve alumina stability, is found to also help in the stabilization of isolated palladium atoms. Aberration-corrected scanning transmission electron microscopy and operando X-ray absorption spectroscopy confirm the presence of intermingled palladium and lanthanum on the γ-alumina surface. Carbon monoxide oxidation reactivity measurements show onset of catalytic activity at 40 °C. The catalyst activity can be regenerated by oxidation at 700 °C in air. The high-temperature stability and regenerability of these ionic palladium species make this catalyst system of potential interest for low-temperature exhaust treatment catalysts.

Original language	English
Article number	4885
Journal	Nature Communications
Volume	5
DOIs	https://doi.org/10.1038/ncomms5885
State	Published - 2014

Funding

We gratefully acknowledge funding for this work provided by the U.S. DOE, Office of Science grant DE-FG02-05ER15712. S.L. thanks the National Natural Science Foundation of China (21203026). R.S.J. and H.G. thank the US National Science Foundation (CHE-0910828). Use of the Advanced Photon Source is supported by the Office of Basic Energy Sciences of the U.S. DOE under contract number W-31-109-Eng-38. Materials Research Collaborative Access Team (MRCAT, Sector 10 ID-B) operations are supported by the Department of Energy and the MRCAT member institutions. STEM imaging was performed at the High Temperature Materials Laboratory, operated by Oak Ridge National Laboratory and supported by DOE, EERE Office of Vehicle Technologies. J.T.M. was supported by the U.S. Department of Energy, Office of Basic Energy Sciences, Chemical Sciences under contract DE-AC-02-06CH11357. F.H.R. acknowledges support from the Department of Energy, Office of Basic Energy Sciences, Chemical Sciences, under Grant DE-FG02-03ER15408. C.H.F.P. and J.H.K. were supported by the U.S. Department of Energy, Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences and Biosciences. Their studies were performed in the Environmental Molecular Sciences Laboratory, a national scientific user facility sponsored by the U.S. Department of Energy’s Office of Biological and Environmental Research and located at Pacific Northwest National Laboratory. E.J.P. thanks Bruce Ravel and Anatoly Frenkel for discussion and guidance with regard to the XAS analysis.

Funders	Funder number
Office of Basic Energy Sciences
U.S. DOE
US National Science Foundation	CHE-0910828
U.S. Department of Energy	W-31-109-Eng-38, DE-AC-02-06CH11357, DE-FG02-03ER15408
Office of Science	DE-FG02-05ER15712
Oak Ridge National Laboratory
Vehicle Technologies Office
Chemical Sciences, Geosciences, and Biosciences Division
National Natural Science Foundation of China	21203026

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title = "Low-temperature carbon monoxide oxidation catalysed by regenerable atomically dispersed palladium on alumina",

abstract = "Catalysis by single isolated atoms of precious metals has attracted much recent interest, as it promises the ultimate in atom efficiency. Most previous reports are on reducible oxide supports. Here we show that isolated palladium atoms can be catalytically active on industrially relevant γ-alumina supports. The addition of lanthanum oxide to the alumina, long known for its ability to improve alumina stability, is found to also help in the stabilization of isolated palladium atoms. Aberration-corrected scanning transmission electron microscopy and operando X-ray absorption spectroscopy confirm the presence of intermingled palladium and lanthanum on the γ-alumina surface. Carbon monoxide oxidation reactivity measurements show onset of catalytic activity at 40 °C. The catalyst activity can be regenerated by oxidation at 700 °C in air. The high-temperature stability and regenerability of these ionic palladium species make this catalyst system of potential interest for low-temperature exhaust treatment catalysts.",

author = "Peterson, {Eric J.} and DeLaRiva, {Andrew T.} and Sen Lin and Johnson, {Ryan S.} and Hua Guo and Miller, {Jeffrey T.} and Kwak, {Ja Hun} and Peden, {Charles H.F.} and Boris Kiefer and Allard, {Lawrence F.} and Ribeiro, {Fabio H.} and Datye, {Abhaya K.}",

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journal = "Nature Communications",

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AU - Peterson, Eric J.

AU - DeLaRiva, Andrew T.

AU - Lin, Sen

AU - Johnson, Ryan S.

AU - Guo, Hua

AU - Miller, Jeffrey T.

AU - Kwak, Ja Hun

AU - Peden, Charles H.F.

AU - Kiefer, Boris

AU - Allard, Lawrence F.

AU - Ribeiro, Fabio H.

AU - Datye, Abhaya K.

PY - 2014

Y1 - 2014

N2 - Catalysis by single isolated atoms of precious metals has attracted much recent interest, as it promises the ultimate in atom efficiency. Most previous reports are on reducible oxide supports. Here we show that isolated palladium atoms can be catalytically active on industrially relevant γ-alumina supports. The addition of lanthanum oxide to the alumina, long known for its ability to improve alumina stability, is found to also help in the stabilization of isolated palladium atoms. Aberration-corrected scanning transmission electron microscopy and operando X-ray absorption spectroscopy confirm the presence of intermingled palladium and lanthanum on the γ-alumina surface. Carbon monoxide oxidation reactivity measurements show onset of catalytic activity at 40 °C. The catalyst activity can be regenerated by oxidation at 700 °C in air. The high-temperature stability and regenerability of these ionic palladium species make this catalyst system of potential interest for low-temperature exhaust treatment catalysts.

AB - Catalysis by single isolated atoms of precious metals has attracted much recent interest, as it promises the ultimate in atom efficiency. Most previous reports are on reducible oxide supports. Here we show that isolated palladium atoms can be catalytically active on industrially relevant γ-alumina supports. The addition of lanthanum oxide to the alumina, long known for its ability to improve alumina stability, is found to also help in the stabilization of isolated palladium atoms. Aberration-corrected scanning transmission electron microscopy and operando X-ray absorption spectroscopy confirm the presence of intermingled palladium and lanthanum on the γ-alumina surface. Carbon monoxide oxidation reactivity measurements show onset of catalytic activity at 40 °C. The catalyst activity can be regenerated by oxidation at 700 °C in air. The high-temperature stability and regenerability of these ionic palladium species make this catalyst system of potential interest for low-temperature exhaust treatment catalysts.

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Low-temperature carbon monoxide oxidation catalysed by regenerable atomically dispersed palladium on alumina

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