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Parastaev, A.; Muravev, V.; Osta, E.H.; Kimpel, T.F.; Simons, J.F.M.; van Hoof, A.J.F.; Uslamin, E.; Zhang, L.; Struijs, J.J.C.; Burueva, D.B.; Pokochueva, E.V.; Kovtunov, K.V.; Koptyug, I.V.; Villar-Garcia, I.J.; Escudero, C.; Altantzis, T.; Liu, P.; Béché, A.; Bals, S.; Kosinov, N.; Hensen, E.J.M. |
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Title |
Breaking structure sensitivity in CO2 hydrogenation by tuning metal–oxide interfaces in supported cobalt nanoparticles |
Type |
A1 Journal article |
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Year  |
2022 |
Publication |
Nature Catalysis |
Abbreviated Journal |
Nat Catal |
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Volume |
5 |
Issue |
11 |
Pages |
1051-1060 |
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Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT); Applied Electrochemistry & Catalysis (ELCAT) |
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Abstract |
A high dispersion of the active metal phase of transition metals on oxide supports is important when designing efficient heterogeneous catalysts. Besides nanoparticles, clusters and even single metal atoms can be attractive for a wide range of reactions. However, many industrially relevant catalytic transformations suffer from structure sensitivity, where reducing the size of the metal particles below a certain size substantially lowers catalytic performance. A case in point is the low activity of small cobalt nanoparticles in the hydrogenation of CO and CO2. Here we show how engineering of catalytic sites at the metal–oxide interface in cerium oxide–zirconium dioxide (ceria–zirconia)-supported cobalt can overcome this structure sensitivity. Few-atom cobalt clusters dispersed on 3 nm cobalt(II)-oxide particles stabilized by ceria–zirconia yielded a highly active CO2 methanation catalyst with a specific activity higher than that of larger particles under the same conditions. |
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Wos |
000884939300006 |
Publication Date |
2022-11-17 |
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ISSN |
2520-1158 |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
37.8 |
Times cited |
32 |
Open Access |
OpenAccess |
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Notes |
This research was supported by the Applied and Engineering Sciences division of the Netherlands Organization for Scientific Research through the Alliander (now Qirion) Perspective program on Plasma Conversion of CO2. We acknowledge Diamond Light Source for time on beamline B18 under proposal SP20715-1. This project has received funding from the European Union’s Horizon 2020 research and innovation programme under grant agreement No 823717 – ESTEEM3. S.B. acknowledges support from the European Research Council (ERC Consolidator Grant #815128 REALNANO) and T.A. acknowledges funding from the University of Antwerp Research fund (BOF). A.B. received funding from the European Union under grant agreement No 823717 – ESTEEM3. The authors acknowledge funding through the Hercules grant (FWO, University of Antwerp) I003218N “Infrastructure for imaging nanoscale processes in gas/vapour or liquid environments”. I.V.K., D.B.B., and E.V.P. acknowledge the Russian Ministry of Science and Higher Education (contract 075-15-2021-580) for financial support of parahydrogen-based studies. Experiments using synchrotron radiation XPS were performed at the CIRCE beamline at ALBA Synchrotron with the collaboration of ALBA staff. F. Oropeza Palacio and Rim C.J. van de Poll are acknowledged for the help with RPES measurements.; esteem3reported; esteem3jra |
Approved |
Most recent IF: 37.8 |
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Call Number |
EMAT @ emat @c:irua:192068 |
Serial |
7230 |
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Author |
Volykhov, A.A.; Sanchez-Barriga, J.; Batuk, M.; Callaert, C.; Hadermann, J.; Sirotina, A.P.; Neudachina, V.S.; Belova, A.I.; Vladimirova, N.V.; Tamm, M.E.; Khmelevsky, N.O.; Escudero, C.; Perez-Dieste, V.; Knop-Gericke, A.; Yashina, L.V. |
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Title |
Can surface reactivity of mixed crystals be predicted from their counterparts? A case study of (Bi1-xSbx)2Te3 topological insulators |
Type |
A1 Journal article |
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Year |
2018 |
Publication |
Journal of materials chemistry C : materials for optical and electronic devices |
Abbreviated Journal |
J Mater Chem C |
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Volume |
6 |
Issue |
33 |
Pages |
8941-8949 |
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Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
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Abstract |
The behavior of ternary mixed crystals or solid solutions and its correlation with the properties of their binary constituents is of fundamental interest. Due to their unique potential for application in future information technology, mixed crystals of topological insulators with the spin-locked, gapless states on their surfaces attract huge attention of physicists, chemists and material scientists. (Bi1-xSbx)(2)Te-3 solid solutions are among the best candidates for spintronic applications since the bulk carrier concentration can be tuned by varying x to obtain truly bulk-insulating samples, where the topological surface states largely contribute to the transport and the realization of the surface quantum Hall effect. As this ternary compound will be evidently used in the form of thin-film devices its chemical stability is an important practical issue. Based on the atomic resolution HAADF-TEM and EDX data together with the XPS results obtained both ex situ and in situ, we propose an atomistic picture of the mixed crystal reactivity compared to that of its binary constituents. We find that the surface reactivity is determined by the probability of oxygen attack on the Te-Sb bonds, which is directly proportional to the number of Te atoms bonded to at least one Sb atom. The oxidation mechanism includes formation of an amorphous antimony oxide at the very surface due to Sb diffusion from the first two quintuple layers, electron tunneling from the Fermi level of the crystal to oxygen, oxygen ion diffusion to the crystal, and finally, slow Te oxidation to the +4 oxidation state. The oxide layer thickness is limited by the electron transport, and the overall process resembles the Cabrera-Mott mechanism in metals. These observations are critical not only for current understanding of the chemical reactivity of complex crystals, but also to improve the performance of future spintronic devices based on topological materials. |
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000443279300007 |
Publication Date |
2018-07-20 |
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ISSN |
2050-7526; 2050-7534 |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
5.256 |
Times cited |
3 |
Open Access |
Not_Open_Access |
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Notes |
; The authors acknowledge financial support within the bilateral program "Russian-German Laboratory at BESSY II''. We thank Helmholtz-Zentrum Berlin for granting access to the beamlines RGBL, UE112-PGM2a and ISISS. Support of ALBA staff during measurements at the CIRCE beamline is gratefully acknowledged. We thank Dr Ivan Bobrikov for support in the XRD measurements and Daria Tsukanova for the participation in crystal preparation and XPS measurements. A. Volykhov thanks RSF (grant 18-73-00248) for financial support. A. I. Belova acknowledges support from the G-RISC Centre of Excellence. The work was supported by Helmholtz Gemeinschaft (Grant No. HRJRG-408) and RFBR (grant 14-03-31518). J. H. and C. C. acknowledge support from the University of Antwerp through the BOF grant 31445. ; |
Approved |
Most recent IF: 5.256 |
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Call Number |
UA @ lucian @ c:irua:153647 |
Serial |
5080 |
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