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Ni Single Atom Catalysts for CO2 Activation

MPS-Authors
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Millet,  Marie-Mathilde
Inorganic Chemistry, Fritz Haber Institute, Max Planck Society;

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Algara-Siller,  Gerardo
Inorganic Chemistry, Fritz Haber Institute, Max Planck Society;

/persons/resource/persons22257

Wrabetz,  Sabine
Inorganic Chemistry, Fritz Haber Institute, Max Planck Society;

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Mazheika,  Aliaksei
Theory, Fritz Haber Institute, Max Planck Society;

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Girgsdies,  Frank
Inorganic Chemistry, Fritz Haber Institute, Max Planck Society;

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Teschner,  Detre
Inorganic Chemistry, Fritz Haber Institute, Max Planck Society;
Department of Heterogeneous Reactions, Max-Planck-Institute for Chemical Energy Conversion;

Seitz,  Friedrich
Inorganic Chemistry, Fritz Haber Institute, Max Planck Society;

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Tarasov,  Andrey
Inorganic Chemistry, Fritz Haber Institute, Max Planck Society;

/persons/resource/persons21797

Levchenko,  Sergey V.
Theory, Fritz Haber Institute, Max Planck Society;
Center for Electrochemical Energy Storage, Skolkovo Institute of Science and Technology;
Materials Modeling and Development Laboratory, National University of Science and Technology “MISIS”;

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Schlögl,  Robert
Inorganic Chemistry, Fritz Haber Institute, Max Planck Society;
Department of Heterogeneous Reactions, Max-Planck-Institute for Chemical Energy Conversion;

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Frei,  Elias
Inorganic Chemistry, Fritz Haber Institute, Max Planck Society;

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jacs.8b11729.pdf
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Citation

Millet, M.-M., Algara-Siller, G., Wrabetz, S., Mazheika, A., Girgsdies, F., Teschner, D., et al. (2019). Ni Single Atom Catalysts for CO2 Activation. Journal of the American Chemical Society, 141(6), 2451-2461. doi:10.1021/jacs.8b11729.


Cite as: https://hdl.handle.net/21.11116/0000-0002-FC0A-8
Abstract
We report on the activation of CO2 on Ni single-atom catalysts. These catalysts were synthesized using a solid solution approach by controlled substitution of 1–10 atom % of Mg2+ by Ni2+ inside the MgO structure. The Ni atoms are preferentially located on the surface of the MgO and, as predicted by hybrid-functional calculations, favor low-coordinated sites. The isolated Ni atoms are active for CO2 conversion through the reverse water–gas shift (rWGS) but are unable to conduct its further hydrogenation to CH4 (or MeOH), for which Ni clusters are needed. The CO formation rates correlate linearly with the concentration of Ni on the surface evidenced by XPS and microcalorimetry. The calculations show that the substitution of Mg atoms by Ni atoms on the surface of the oxide structure reduces the strength of the CO2 binding at low-coordinated sites and also promotes H2 dissociation. Astonishingly, the single-atom catalysts stayed stable over 100 h on stream, after which no clusters or particle formation could be detected. Upon catalysis, a surface carbonate adsorbate-layer was formed, of which the decompositions appear to be directly linked to the aggregation of Ni. This study on atomically dispersed Ni species brings new fundamental understanding of Ni active sites for reactions involving CO2 and clearly evidence the limits of single-atom catalysis for complex reactions.