Complex structural dynamics of nanocatalysts revealed in Operando conditions by correlated imaging and spectroscopy probes

Y. Li; D. Zakharov; S. Zhao; R. Tappero; U. Jung; A. Elsen; Ph Baumann; R. G. Nuzzo; E. A. Stach; A. I. Frenkel

doi:10.1038/ncomms8583

Complex structural dynamics of nanocatalysts revealed in Operando conditions by correlated imaging and spectroscopy probes

Y. Li, D. Zakharov, S. Zhao, R. Tappero, U. Jung, A. Elsen, Ph Baumann, R. G. Nuzzo, E. A. Stach, A. I. Frenkel

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118 Scopus citations

Abstract

Understanding how heterogeneous catalysts change size, shape and structure during chemical reactions is limited by the paucity of methods for studying catalytic ensembles in working state, that is, in operando conditions. Here by a correlated use of synchrotron X-ray absorption spectroscopy and scanning transmission electron microscopy in operando conditions, we quantitatively describe the complex structural dynamics of supported Pt catalysts exhibited during an exemplary catalytic reaction-ethylene hydrogenation. This work exploits a microfabricated catalytic reactor compatible with both probes. The results demonstrate dynamic transformations of the ensemble of Pt clusters that spans a broad size range throughout changing reaction conditions. This method is generalizable to quantitative operando studies of complex systems using a wide variety of X-ray and electron-based experimental probes.

Original language	English
Article number	7583
Journal	Nature Communications
Volume	6
DOIs	https://doi.org/10.1038/ncomms8583
State	Published - Jun 29 2015
Externally published	Yes

Funding

The authors gratefully acknowledge support for this by the US Department of Energy, Office of Basic Energy Sciences under Grant No. DE-FG02-03ER15476 (Y.L., S.Z., U.J., A.E., R.G.N., A.I.F.) and Contract No. DE-SC0012704 (D.Z., R.T., E.A.S.). The development of the micro-cell was supported, in part, by an LDRD grant at Brookhaven National Laboratory. We acknowledge the facilities support provided at the Centre for Functional Nanomaterials, the National Synchrotron Light Source at the Brookhaven National Laboratory (US Department of Energy, Office of Basic Energy Sciences, Contract No. DE-SC0012704) and the Synchrotron Catalysis Consortium (US Department of Energy, Office of Basic Energy Sciences, Grant No. DE-FG02-05ER15688).

Funders	Funder number
National Synchrotron Light Source at the Brookhaven National Laboratory
Synchrotron Catalysis Consortium	DE-FG02-05ER15688
U.S. Department of Energy
Basic Energy Sciences	DE-FG02-03ER15476, DE-SC0012704
Brookhaven National Laboratory
Laboratory Directed Research and Development

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abstract = "Understanding how heterogeneous catalysts change size, shape and structure during chemical reactions is limited by the paucity of methods for studying catalytic ensembles in working state, that is, in operando conditions. Here by a correlated use of synchrotron X-ray absorption spectroscopy and scanning transmission electron microscopy in operando conditions, we quantitatively describe the complex structural dynamics of supported Pt catalysts exhibited during an exemplary catalytic reaction-ethylene hydrogenation. This work exploits a microfabricated catalytic reactor compatible with both probes. The results demonstrate dynamic transformations of the ensemble of Pt clusters that spans a broad size range throughout changing reaction conditions. This method is generalizable to quantitative operando studies of complex systems using a wide variety of X-ray and electron-based experimental probes.",

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AU - Li, Y.

AU - Zakharov, D.

AU - Zhao, S.

AU - Tappero, R.

AU - Jung, U.

AU - Elsen, A.

AU - Baumann, Ph

AU - Nuzzo, R. G.

AU - Stach, E. A.

AU - Frenkel, A. I.

PY - 2015/6/29

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AB - Understanding how heterogeneous catalysts change size, shape and structure during chemical reactions is limited by the paucity of methods for studying catalytic ensembles in working state, that is, in operando conditions. Here by a correlated use of synchrotron X-ray absorption spectroscopy and scanning transmission electron microscopy in operando conditions, we quantitatively describe the complex structural dynamics of supported Pt catalysts exhibited during an exemplary catalytic reaction-ethylene hydrogenation. This work exploits a microfabricated catalytic reactor compatible with both probes. The results demonstrate dynamic transformations of the ensemble of Pt clusters that spans a broad size range throughout changing reaction conditions. This method is generalizable to quantitative operando studies of complex systems using a wide variety of X-ray and electron-based experimental probes.

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Complex structural dynamics of nanocatalysts revealed in Operando conditions by correlated imaging and spectroscopy probes

Abstract

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