Palladium-platinum core-shell icosahedra with substantially enhanced activity and durability towards oxygen reduction

Xue Wang; Sang-Il Choi; Luke T. Roling; Ming Luo; Cheng Ma; Lei Zhang; Miaofang Chi; Jingyue Liu; Zhaoxiong Xie; Jeffrey A. Herron; Manos Mavrikakis; Younan Xia

doi:10.1038/ncomms8594

Palladium-platinum core-shell icosahedra with substantially enhanced activity and durability towards oxygen reduction

Xue Wang, Sang-Il Choi, Luke T. Roling, Ming Luo, Cheng Ma, Lei Zhang, Miaofang Chi, Jingyue Liu, Zhaoxiong Xie, Jeffrey A. Herron, Manos Mavrikakis^*, Younan Xia

^*Corresponding author for this work

Research output: Journal Publications and Reviews › RGC 21 - Publication in refereed journal › peer-review

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Abstract

Conformal deposition of platinum as ultrathin shells on facet-controlled palladium nanocrystals offers a great opportunity to enhance the catalytic performance while reducing its loading. Here we report such a system based on palladium icosahedra. Owing to lateral confinement imposed by twin boundaries and thus vertical relaxation only, the platinum overlayers evolve into a corrugated structure under compressive strain. For the core-shell nanocrystals with an average of 2.7 platinum overlayers, their specific and platinum mass activities towards oxygen reduction are enhanced by eight- And sevenfold, respectively, relative to a commercial catalyst. Density functional theory calculations indicate that the enhancement can be attributed to the weakened binding of hydroxyl to the compressed platinum surface supported on palladium. After 10,000 testing cycles, the mass activity of the core-shell nanocrystals is still four times higher than the commercial catalyst. These results demonstrate an effective approach to the development of electrocatalysts with greatly enhanced activity and durability.

Original language	English
Article number	7594
Journal	Nature Communications
Volume	6
DOIs	https://doi.org/10.1038/ncomms8594
Publication status	Published - 2015
Externally published	Yes

Bibliographical note

Publication details (e.g. title, author(s), publication statuses and dates) are captured on an “AS IS” and “AS AVAILABLE” basis at the time of record harvesting from the data source. Suggestions for further amendments or supplementary information can be sent to [email protected].

Funding

The syntheses were supported by start-up funds from the Georgia Institute of Technology (to Y.X.) while the computations were supported by DOE-BES (Office of Chemical Scienses, grant DE-FG02-05ER15731, to M.M.). As visiting students, X.W., M.L. and L.Z. were also partially supported by the China Scholarship Council. Part of the electron microscopy work was performed through a user project supported by the ORNL’s Center for Nanophase Materials Sciences, which is a DOE Office of Science User Facility. J.L. gratefully acknowledges the support by Arizona State University and the use of facilities in the John M. Cowley Center for High Resolution Electron Microscopy at Arizona State University. The calculations were performed at supercomputing centres located at EMSL (which is sponsored by the DOE Office of Biological and Environmental Research at PNNL), CNM (supported by DOE contract DE-AC02-06CH11357 to ANL) and NERSC (supported by DOE contract DE-AC02-05CH11231 to LBL).

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This full text is made available under CC-BY 4.0. https://creativecommons.org/licenses/by/4.0/

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title = "Palladium-platinum core-shell icosahedra with substantially enhanced activity and durability towards oxygen reduction",

abstract = "Conformal deposition of platinum as ultrathin shells on facet-controlled palladium nanocrystals offers a great opportunity to enhance the catalytic performance while reducing its loading. Here we report such a system based on palladium icosahedra. Owing to lateral confinement imposed by twin boundaries and thus vertical relaxation only, the platinum overlayers evolve into a corrugated structure under compressive strain. For the core-shell nanocrystals with an average of 2.7 platinum overlayers, their specific and platinum mass activities towards oxygen reduction are enhanced by eight- And sevenfold, respectively, relative to a commercial catalyst. Density functional theory calculations indicate that the enhancement can be attributed to the weakened binding of hydroxyl to the compressed platinum surface supported on palladium. After 10,000 testing cycles, the mass activity of the core-shell nanocrystals is still four times higher than the commercial catalyst. These results demonstrate an effective approach to the development of electrocatalysts with greatly enhanced activity and durability.",

author = "Xue Wang and Sang-Il Choi and Roling, {Luke T.} and Ming Luo and Cheng Ma and Lei Zhang and Miaofang Chi and Jingyue Liu and Zhaoxiong Xie and Herron, {Jeffrey A.} and Manos Mavrikakis and Younan Xia",

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AU - Wang, Xue

AU - Choi, Sang-Il

AU - Roling, Luke T.

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AU - Ma, Cheng

AU - Zhang, Lei

AU - Chi, Miaofang

AU - Liu, Jingyue

AU - Xie, Zhaoxiong

AU - Herron, Jeffrey A.

AU - Mavrikakis, Manos

AU - Xia, Younan

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N2 - Conformal deposition of platinum as ultrathin shells on facet-controlled palladium nanocrystals offers a great opportunity to enhance the catalytic performance while reducing its loading. Here we report such a system based on palladium icosahedra. Owing to lateral confinement imposed by twin boundaries and thus vertical relaxation only, the platinum overlayers evolve into a corrugated structure under compressive strain. For the core-shell nanocrystals with an average of 2.7 platinum overlayers, their specific and platinum mass activities towards oxygen reduction are enhanced by eight- And sevenfold, respectively, relative to a commercial catalyst. Density functional theory calculations indicate that the enhancement can be attributed to the weakened binding of hydroxyl to the compressed platinum surface supported on palladium. After 10,000 testing cycles, the mass activity of the core-shell nanocrystals is still four times higher than the commercial catalyst. These results demonstrate an effective approach to the development of electrocatalysts with greatly enhanced activity and durability.

AB - Conformal deposition of platinum as ultrathin shells on facet-controlled palladium nanocrystals offers a great opportunity to enhance the catalytic performance while reducing its loading. Here we report such a system based on palladium icosahedra. Owing to lateral confinement imposed by twin boundaries and thus vertical relaxation only, the platinum overlayers evolve into a corrugated structure under compressive strain. For the core-shell nanocrystals with an average of 2.7 platinum overlayers, their specific and platinum mass activities towards oxygen reduction are enhanced by eight- And sevenfold, respectively, relative to a commercial catalyst. Density functional theory calculations indicate that the enhancement can be attributed to the weakened binding of hydroxyl to the compressed platinum surface supported on palladium. After 10,000 testing cycles, the mass activity of the core-shell nanocrystals is still four times higher than the commercial catalyst. These results demonstrate an effective approach to the development of electrocatalysts with greatly enhanced activity and durability.

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Palladium-platinum core-shell icosahedra with substantially enhanced activity and durability towards oxygen reduction

Abstract

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