Surface Carbon as a Reactive Intermediate in Dry Reforming of Methane to Syngas on a 5% Ni/MnO Catalyst

Albert Gili; Lukas Schlicker; Maged F. Bekheet; Oliver Görke; Simon Penner; Matthias Grünbacher; Thomas Götsch; Patrick Littlewood; Tobin J. Marks; Peter C. Stair; Reinhard Schomäcker; Andrew Doran; Sören Selve; Ulla Simon; Aleksander Gurlo

doi:10.1021/acscatal.8b01820

Surface Carbon as a Reactive Intermediate in Dry Reforming of Methane to Syngas on a 5% Ni/MnO Catalyst

Albert Gili^*, Lukas Schlicker, Maged F. Bekheet, Oliver Görke, Simon Penner, Matthias Grünbacher, Thomas Götsch, Patrick Littlewood, Tobin J. Marks, Peter C. Stair, Reinhard Schomäcker, Andrew Doran, Sören Selve, Ulla Simon, Aleksander Gurlo

^*Corresponding author for this work

Chemistry

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Abstract

A 5% Ni/MnO catalyst has been tested for the dry reforming of methane at different temperatures and reactant partial pressures. Changing the reactant ratio with time on stream results in a decrease in the deactivation rate of the catalyst. Graphitic carbon growth and metal particle sintering have been observed by applying in situ transmission XRD using synchrotron radiation under actual reaction conditions. Both methane and carbon monoxide separately result in graphitic surface carbon, which can then be oxidized by carbon dioxide. The morphology of the surface carbon has been analyzed by TEM, and the reactions of both methane and carbon monoxide result in the same graphitic multiwalled carbon nanotubes. The present combination of catalytic experiments and in situ techniques suggests that surface carbon acts as an intermediate in the formation of CO and that catalyst deactivation happens via metallic particle sintering. These results enable a more rational choice of reaction conditions to ensure high catalyst activity and long-term stability. Future catalyst advances must aim to prevent metal particle sintering.

Original language	English (US)
Pages (from-to)	8739-8750
Number of pages	12
Journal	ACS Catalysis
Volume	8
Issue number	9
DOIs	https://doi.org/10.1021/acscatal.8b01820
State	Published - Sep 7 2018

Funding

A part of this work was supported by the Cluster of Excellence “Unifying Concepts in Catalysis”, financed by the German Research Foundation (DFG-Deutsche Forschungsgemein-schaft). A.G. gratefully acknowledges the Elsa-Neumann-Stipendium des Landes Berlin (NAFOEG). This research used resources of the Advanced Light Source, which is a DOE Office of Science User Facility under contract no. DE-AC02-05CH11231. In addition, this work has been made possible by an NPRP exceptional grant award (NPRP-EP X-100-2-024) from the Qatar National Research Fund (a member of the Qatar Foundation). S.P., T.G. and M.G. acknowledge funding from the Austrian Science Fund (FWF) within SFB F45. Their work was performed within the frameworks of the special research platform “Advanced Materials” and also within the special Ph.D. program “Reactivity and Catalysis”. The statements made herein are solely the responsibility of the authors.

ASJC Scopus subject areas

Catalysis
General Chemistry

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10.1021/acscatal.8b01820

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Gili, A., Schlicker, L., Bekheet, M. F., Görke, O., Penner, S., Grünbacher, M., Götsch, T., Littlewood, P., Marks, T. J., Stair, P. C., Schomäcker, R., Doran, A., Selve, S., Simon, U., & Gurlo, A. (2018). Surface Carbon as a Reactive Intermediate in Dry Reforming of Methane to Syngas on a 5% Ni/MnO Catalyst. ACS Catalysis, 8(9), 8739-8750. https://doi.org/10.1021/acscatal.8b01820

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title = "Surface Carbon as a Reactive Intermediate in Dry Reforming of Methane to Syngas on a 5% Ni/MnO Catalyst",

abstract = "A 5% Ni/MnO catalyst has been tested for the dry reforming of methane at different temperatures and reactant partial pressures. Changing the reactant ratio with time on stream results in a decrease in the deactivation rate of the catalyst. Graphitic carbon growth and metal particle sintering have been observed by applying in situ transmission XRD using synchrotron radiation under actual reaction conditions. Both methane and carbon monoxide separately result in graphitic surface carbon, which can then be oxidized by carbon dioxide. The morphology of the surface carbon has been analyzed by TEM, and the reactions of both methane and carbon monoxide result in the same graphitic multiwalled carbon nanotubes. The present combination of catalytic experiments and in situ techniques suggests that surface carbon acts as an intermediate in the formation of CO and that catalyst deactivation happens via metallic particle sintering. These results enable a more rational choice of reaction conditions to ensure high catalyst activity and long-term stability. Future catalyst advances must aim to prevent metal particle sintering.",

author = "Albert Gili and Lukas Schlicker and Bekheet, {Maged F.} and Oliver G{\"o}rke and Simon Penner and Matthias Gr{\"u}nbacher and Thomas G{\"o}tsch and Patrick Littlewood and Marks, {Tobin J.} and Stair, {Peter C.} and Reinhard Schom{\"a}cker and Andrew Doran and S{\"o}ren Selve and Ulla Simon and Aleksander Gurlo",

note = "Funding Information: A part of this work was supported by the Cluster of Excellence “Unifying Concepts in Catalysis”, financed by the German Research Foundation (DFG-Deutsche Forschungsgemein-schaft). A.G. gratefully acknowledges the Elsa-Neumann-Stipendium des Landes Berlin (NAFOEG). This research used resources of the Advanced Light Source, which is a DOE Office of Science User Facility under contract no. DE-AC02-05CH11231. In addition, this work has been made possible by an NPRP exceptional grant award (NPRP-EP X-100-2-024) from the Qatar National Research Fund (a member of the Qatar Foundation). S.P., T.G. and M.G. acknowledge funding from the Austrian Science Fund (FWF) within SFB F45. Their work was performed within the frameworks of the special research platform “Advanced Materials” and also within the special Ph.D. program “Reactivity and Catalysis”. The statements made herein are solely the responsibility of the authors.",

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Gili, A, Schlicker, L, Bekheet, MF, Görke, O, Penner, S, Grünbacher, M, Götsch, T, Littlewood, P, Marks, TJ , Stair, PC, Schomäcker, R, Doran, A, Selve, S, Simon, U & Gurlo, A 2018, 'Surface Carbon as a Reactive Intermediate in Dry Reforming of Methane to Syngas on a 5% Ni/MnO Catalyst', ACS Catalysis, vol. 8, no. 9, pp. 8739-8750. https://doi.org/10.1021/acscatal.8b01820

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T1 - Surface Carbon as a Reactive Intermediate in Dry Reforming of Methane to Syngas on a 5% Ni/MnO Catalyst

AU - Gili, Albert

AU - Schlicker, Lukas

AU - Bekheet, Maged F.

AU - Görke, Oliver

AU - Penner, Simon

AU - Grünbacher, Matthias

AU - Götsch, Thomas

AU - Littlewood, Patrick

AU - Marks, Tobin J.

AU - Stair, Peter C.

AU - Schomäcker, Reinhard

AU - Doran, Andrew

AU - Selve, Sören

AU - Simon, Ulla

AU - Gurlo, Aleksander

N1 - Funding Information: A part of this work was supported by the Cluster of Excellence “Unifying Concepts in Catalysis”, financed by the German Research Foundation (DFG-Deutsche Forschungsgemein-schaft). A.G. gratefully acknowledges the Elsa-Neumann-Stipendium des Landes Berlin (NAFOEG). This research used resources of the Advanced Light Source, which is a DOE Office of Science User Facility under contract no. DE-AC02-05CH11231. In addition, this work has been made possible by an NPRP exceptional grant award (NPRP-EP X-100-2-024) from the Qatar National Research Fund (a member of the Qatar Foundation). S.P., T.G. and M.G. acknowledge funding from the Austrian Science Fund (FWF) within SFB F45. Their work was performed within the frameworks of the special research platform “Advanced Materials” and also within the special Ph.D. program “Reactivity and Catalysis”. The statements made herein are solely the responsibility of the authors.

PY - 2018/9/7

Y1 - 2018/9/7

N2 - A 5% Ni/MnO catalyst has been tested for the dry reforming of methane at different temperatures and reactant partial pressures. Changing the reactant ratio with time on stream results in a decrease in the deactivation rate of the catalyst. Graphitic carbon growth and metal particle sintering have been observed by applying in situ transmission XRD using synchrotron radiation under actual reaction conditions. Both methane and carbon monoxide separately result in graphitic surface carbon, which can then be oxidized by carbon dioxide. The morphology of the surface carbon has been analyzed by TEM, and the reactions of both methane and carbon monoxide result in the same graphitic multiwalled carbon nanotubes. The present combination of catalytic experiments and in situ techniques suggests that surface carbon acts as an intermediate in the formation of CO and that catalyst deactivation happens via metallic particle sintering. These results enable a more rational choice of reaction conditions to ensure high catalyst activity and long-term stability. Future catalyst advances must aim to prevent metal particle sintering.

AB - A 5% Ni/MnO catalyst has been tested for the dry reforming of methane at different temperatures and reactant partial pressures. Changing the reactant ratio with time on stream results in a decrease in the deactivation rate of the catalyst. Graphitic carbon growth and metal particle sintering have been observed by applying in situ transmission XRD using synchrotron radiation under actual reaction conditions. Both methane and carbon monoxide separately result in graphitic surface carbon, which can then be oxidized by carbon dioxide. The morphology of the surface carbon has been analyzed by TEM, and the reactions of both methane and carbon monoxide result in the same graphitic multiwalled carbon nanotubes. The present combination of catalytic experiments and in situ techniques suggests that surface carbon acts as an intermediate in the formation of CO and that catalyst deactivation happens via metallic particle sintering. These results enable a more rational choice of reaction conditions to ensure high catalyst activity and long-term stability. Future catalyst advances must aim to prevent metal particle sintering.

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Surface Carbon as a Reactive Intermediate in Dry Reforming of Methane to Syngas on a 5% Ni/MnO Catalyst

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