Restructuring of titanium oxide overlayers over nickel nanoparticles during catalysis

Matteo Monai; Kellie Jenkinson; Angela E M Melcherts; Jaap N Louwen; Ece A Irmak; Sandra Van Aert; Thomas Altantzis; Charlotte Vogt; Ward van der Stam; Tomáš Duchoň; Břetislav Šmíd; Esther Groeneveld; Peter Berben; Sara Bals; Bert M Weckhuysen

doi:10.1126/science.adf6984

Restructuring of titanium oxide overlayers over nickel nanoparticles during catalysis

Matteo Monai
, Kellie Jenkinson
, Angela E M Melcherts
, Jaap N Louwen
, Ece A Irmak
, Sandra Van Aert
, Thomas Altantzis
, Charlotte Vogt
, Ward van der Stam
, Tomáš Duchoň
, Břetislav Šmíd
, Esther Groeneveld
, Peter Berben
, Sara Bals
, Bert M Weckhuysen

University of Antwerp
Forschungszentrum Jülich GmbH
Charles University
Technion-Israel Institute of Technology
BASF Nederland B.V.

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

Abstract

Reducible supports can affect the performance of metal catalysts by the formation of suboxide overlayers upon reduction, a process referred to as the strong metal-support interaction (SMSI). A combination of operando electron microscopy and vibrational spectroscopy revealed that thin TiO x overlayers formed on nickel/titanium dioxide catalysts during 400°C reduction were completely removed under carbon dioxide hydrogenation conditions. Conversely, after 600°C reduction, exposure to carbon dioxide hydrogenation reaction conditions led to only partial reexposure of nickel, forming interfacial sites in contact with TiO x and favoring carbon-carbon coupling by providing a carbon species reservoir. Our findings challenge the conventional understanding of SMSIs and call for more-detailed operando investigations of nanocatalysts at the single-particle level to revisit static models of structure-activity relationships.

Original language	English
Pages (from-to)	644-651
Number of pages	8
Journal	Science (New York, N.Y.)
Volume	380
Issue number	6645
DOIs	https://doi.org/10.1126/science.adf6984
Publication status	Published - 12 May 2023

Bibliographical note

Publisher Copyright:
Copyright © 2023 the authors, some rights reserved.

Funding

This work was supported by BASF and NWO CHIPP (research grant to B.M.W.); the MCEC NWO Gravitation Program (B.M.W.); the ARC-CBBC NWO Program (B.M.W.); the European Research Council (grant 770887 PICOMETRICS to S.V.A.); and the European Research Council (grant 815128 REALNANO to S.B.).

Funders	Funder number
ARC-CBBC NWO
MCEC NWO
BASF
European Research Council	815128, 770887 PICOMETRICS
Nederlandse Organisatie voor Wetenschappelijk Onderzoek

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science.adf6984Final published version, 2.93 MBLicence: Taverne

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Monai, M., Jenkinson, K., Melcherts, A. E. M., Louwen, J. N., Irmak, E. A., Van Aert, S., Altantzis, T., Vogt, C., van der Stam, W., Duchoň, T., Šmíd, B., Groeneveld, E., Berben, P., Bals, S., & Weckhuysen, B. M. (2023). Restructuring of titanium oxide overlayers over nickel nanoparticles during catalysis. Science (New York, N.Y.), 380(6645), 644-651. https://doi.org/10.1126/science.adf6984

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title = "Restructuring of titanium oxide overlayers over nickel nanoparticles during catalysis",

abstract = "Reducible supports can affect the performance of metal catalysts by the formation of suboxide overlayers upon reduction, a process referred to as the strong metal-support interaction (SMSI). A combination of operando electron microscopy and vibrational spectroscopy revealed that thin TiO x overlayers formed on nickel/titanium dioxide catalysts during 400°C reduction were completely removed under carbon dioxide hydrogenation conditions. Conversely, after 600°C reduction, exposure to carbon dioxide hydrogenation reaction conditions led to only partial reexposure of nickel, forming interfacial sites in contact with TiO x and favoring carbon-carbon coupling by providing a carbon species reservoir. Our findings challenge the conventional understanding of SMSIs and call for more-detailed operando investigations of nanocatalysts at the single-particle level to revisit static models of structure-activity relationships. ",

author = "Matteo Monai and Kellie Jenkinson and Melcherts, \{Angela E M\} and Louwen, \{Jaap N\} and Irmak, \{Ece A\} and \{Van Aert\}, Sandra and Thomas Altantzis and Charlotte Vogt and \{van der Stam\}, Ward and Tom{\'a}{\v s} Ducho{\v n} and B{\v r}etislav {\v S}m{\'i}d and Esther Groeneveld and Peter Berben and Sara Bals and Weckhuysen, \{Bert M\}",

note = "Publisher Copyright: Copyright {\textcopyright} 2023 the authors, some rights reserved.",

year = "2023",

month = may,

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doi = "10.1126/science.adf6984",

language = "English",

volume = "380",

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Monai, M, Jenkinson, K, Melcherts, AEM, Louwen, JN, Irmak, EA, Van Aert, S, Altantzis, T, Vogt, C, van der Stam, W, Duchoň, T, Šmíd, B, Groeneveld, E, Berben, P, Bals, S & Weckhuysen, BM 2023, 'Restructuring of titanium oxide overlayers over nickel nanoparticles during catalysis', Science (New York, N.Y.), vol. 380, no. 6645, pp. 644-651. https://doi.org/10.1126/science.adf6984

TY - JOUR

T1 - Restructuring of titanium oxide overlayers over nickel nanoparticles during catalysis

AU - Monai, Matteo

AU - Jenkinson, Kellie

AU - Melcherts, Angela E M

AU - Louwen, Jaap N

AU - Irmak, Ece A

AU - Van Aert, Sandra

AU - Altantzis, Thomas

AU - Vogt, Charlotte

AU - van der Stam, Ward

AU - Duchoň, Tomáš

AU - Šmíd, Břetislav

AU - Groeneveld, Esther

AU - Berben, Peter

AU - Bals, Sara

AU - Weckhuysen, Bert M

PY - 2023/5/12

Y1 - 2023/5/12

N2 - Reducible supports can affect the performance of metal catalysts by the formation of suboxide overlayers upon reduction, a process referred to as the strong metal-support interaction (SMSI). A combination of operando electron microscopy and vibrational spectroscopy revealed that thin TiO x overlayers formed on nickel/titanium dioxide catalysts during 400°C reduction were completely removed under carbon dioxide hydrogenation conditions. Conversely, after 600°C reduction, exposure to carbon dioxide hydrogenation reaction conditions led to only partial reexposure of nickel, forming interfacial sites in contact with TiO x and favoring carbon-carbon coupling by providing a carbon species reservoir. Our findings challenge the conventional understanding of SMSIs and call for more-detailed operando investigations of nanocatalysts at the single-particle level to revisit static models of structure-activity relationships.

AB - Reducible supports can affect the performance of metal catalysts by the formation of suboxide overlayers upon reduction, a process referred to as the strong metal-support interaction (SMSI). A combination of operando electron microscopy and vibrational spectroscopy revealed that thin TiO x overlayers formed on nickel/titanium dioxide catalysts during 400°C reduction were completely removed under carbon dioxide hydrogenation conditions. Conversely, after 600°C reduction, exposure to carbon dioxide hydrogenation reaction conditions led to only partial reexposure of nickel, forming interfacial sites in contact with TiO x and favoring carbon-carbon coupling by providing a carbon species reservoir. Our findings challenge the conventional understanding of SMSIs and call for more-detailed operando investigations of nanocatalysts at the single-particle level to revisit static models of structure-activity relationships.

UR - https://www.scopus.com/pages/publications/85159739034

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DO - 10.1126/science.adf6984

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SN - 0036-8075

VL - 380

SP - 644

EP - 651

JO - Science (New York, N.Y.)

JF - Science (New York, N.Y.)

IS - 6645

ER -

Restructuring of titanium oxide overlayers over nickel nanoparticles during catalysis

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