Understanding carbon dioxide activation and carbon-carbon coupling over nickel

Charlotte Vogt; Matteo Monai; Ellen B. Sterk; Jonas Palle; Angela E.M. Melcherts; Bart Zijlstra; Esther Groeneveld; Peter H. Berben; Jelle M. Boereboom; Emiel J.M. Hensen; Florian Meirer; Ivo A.W. Filot; Bert M. Weckhuysen

doi:10.1038/s41467-019-12858-3

Understanding carbon dioxide activation and carbon-carbon coupling over nickel

Charlotte Vogt
, Matteo Monai
, Ellen B. Sterk
, Jonas Palle
, Angela E.M. Melcherts
, Bart Zijlstra
, Esther Groeneveld
, Peter H. Berben
, Jelle M. Boereboom
, Emiel J.M. Hensen
, Florian Meirer
, Ivo A.W. Filot (Corresponding author)
, Bert M. Weckhuysen (Corresponding author)

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

177 Citations (Scopus)

237 Downloads (Pure)

Abstract

Carbon dioxide is a desired feedstock for platform molecules, such as carbon monoxide or higher hydrocarbons, from which we will be able to make many different useful, value-added chemicals. Its catalytic hydrogenation over abundant metals requires the amalgamation of theoretical knowledge with materials design. Here we leverage a theoretical understanding of structure sensitivity, along with a library of different supports, to tune the selectivity of methanation in the Power-to-Gas concept over nickel. For example, we show that carbon dioxide hydrogenation over nickel can and does form propane, and that activity and selectivity can be tuned by supporting different nickel particle sizes on various oxides. This theoretical and experimental toolbox is not only useful for the highly selective production of methane, but also provides new insights for carbon dioxide activation and subsequent carbon–carbon coupling towards value-added products thereby reducing the deleterious effects of this environmentally harmful molecule.

Original language	English
Article number	5330
Number of pages	10
Journal	Nature Communications
Volume	10
DOIs	https://doi.org/10.1038/s41467-019-12858-3
Publication status	Published - 1 Dec 2019

Funding

We thank BASF and NWO for a CHIPP research grant. The research presented in this work was calculated on the Cartesius cluster and we gratefully acknowledge NWO for computational time, and SurfSara for maintenance. We also thank ARC-CBBC, an NWO funded Gravitation Program MCEC as well as the Strategic Alliance Utrecht University-Eindhoven University of Technology for research funding. Robin Broos (TU/e) is thanked for assistance with calculations and for useful discussions, while Wilbert Vrijburg (TU/e) is thanked for help with high-throughput experiments.

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10.1038/s41467-019-12858-3

publishers versionFinal published version, 2.76 MBLicence: CC BY

Cite this

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title = "Understanding carbon dioxide activation and carbon-carbon coupling over nickel",

abstract = "Carbon dioxide is a desired feedstock for platform molecules, such as carbon monoxide or higher hydrocarbons, from which we will be able to make many different useful, value-added chemicals. Its catalytic hydrogenation over abundant metals requires the amalgamation of theoretical knowledge with materials design. Here we leverage a theoretical understanding of structure sensitivity, along with a library of different supports, to tune the selectivity of methanation in the Power-to-Gas concept over nickel. For example, we show that carbon dioxide hydrogenation over nickel can and does form propane, and that activity and selectivity can be tuned by supporting different nickel particle sizes on various oxides. This theoretical and experimental toolbox is not only useful for the highly selective production of methane, but also provides new insights for carbon dioxide activation and subsequent carbon–carbon coupling towards value-added products thereby reducing the deleterious effects of this environmentally harmful molecule.",

author = "Charlotte Vogt and Matteo Monai and Sterk, \{Ellen B.\} and Jonas Palle and Melcherts, \{Angela E.M.\} and Bart Zijlstra and Esther Groeneveld and Berben, \{Peter H.\} and Boereboom, \{Jelle M.\} and Hensen, \{Emiel J.M.\} and Florian Meirer and Filot, \{Ivo A.W.\} and Weckhuysen, \{Bert M.\}",

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AU - Zijlstra, Bart

AU - Groeneveld, Esther

AU - Berben, Peter H.

AU - Boereboom, Jelle M.

AU - Hensen, Emiel J.M.

AU - Meirer, Florian

AU - Filot, Ivo A.W.

AU - Weckhuysen, Bert M.

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AB - Carbon dioxide is a desired feedstock for platform molecules, such as carbon monoxide or higher hydrocarbons, from which we will be able to make many different useful, value-added chemicals. Its catalytic hydrogenation over abundant metals requires the amalgamation of theoretical knowledge with materials design. Here we leverage a theoretical understanding of structure sensitivity, along with a library of different supports, to tune the selectivity of methanation in the Power-to-Gas concept over nickel. For example, we show that carbon dioxide hydrogenation over nickel can and does form propane, and that activity and selectivity can be tuned by supporting different nickel particle sizes on various oxides. This theoretical and experimental toolbox is not only useful for the highly selective production of methane, but also provides new insights for carbon dioxide activation and subsequent carbon–carbon coupling towards value-added products thereby reducing the deleterious effects of this environmentally harmful molecule.

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Understanding carbon dioxide activation and carbon-carbon coupling over nickel

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UTRECHT UNIVERSITY : 'Collaboration is an essential condition for this degree of impact'; Team science leads to breakthrough in CO2 conversion

Team science leads to breakthrough in CO2 conversion

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Understanding carbon dioxide activation and carbon-carbon coupling over nickel

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UTRECHT UNIVERSITY : 'Collaboration is an essential condition for this degree of impact'; Team science leads to breakthrough in CO2 conversion

Team science leads to breakthrough in CO2 conversion

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