Cobalt nanocrystals on carbon nanotubes in the Fischer-Tropsch synthesis: Impact of support oxidation

T. W. van Deelen; H. Yoshida; R. Oord; J. Zečević; B. M. Weckhuysen; K. P. de Jong

doi:10.1016/j.apcata.2020.117441

Cobalt nanocrystals on carbon nanotubes in the Fischer-Tropsch synthesis: Impact of support oxidation

T. W. van Deelen
, H. Yoshida
, R. Oord
, J. Zečević
, B. M. Weckhuysen
, K. P. de Jong^*

^*Corresponding author for this work

Sub Advanced Research Center Chemical Building Blocks Consortium

extern

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

Abstract

The effect of oxidation of a carbon nanotube (CNT) support on the structure and catalytic performance in the Fischer-Tropsch (FT) synthesis of pre-synthesized cobalt nanocrystals (NC) has been investigated. 6 nm CoO-NC were prepared using colloidal techniques and impregnated on pristine and surface-oxidized CNT. The CoO-NC on pristine CNT were reduced completely to Co, while ∼50 % CoO reduction was observed on oxidized CNT (oxCNT), indicating a stronger Co-support interaction on oxCNT. In FT, the turnover frequency (TOF) after 100 h was exceptionally high on pristine CNT (150·10⁻³ s^-1) against 63·10⁻³ s^-1 on oxCNT. In the initial stage of FT, the TOF was 35 % lower on oxCNT than on pristine CNT, which matched with 32 % lower crystallinity of cobalt determined using in situ XRD. Furthermore, deactivation was observed mainly on oxCNT. These results demonstrate the large impact of the support on the structure and performance of nanocrystal-based catalysts.

Original language	English
Article number	117441
Journal	Applied Catalysis A: General
Volume	593
DOIs	https://doi.org/10.1016/j.apcata.2020.117441
Publication status	Published - 5 Mar 2020

Funding

T.W.v.D., B.M.W. and K.P.d.J. acknowledge Shell Global Solutions and the Netherlands Association for Scientific Research (NWO) for funding through the CHIPP framework. H.Y., J.Z. and K.P.d.J. acknowledge the European Research Council, EU FP7 ERC Advanced Grant no. 338846. H.Y. acknowledges the Program for Advancing Strategic International Networks to Accelerate the Circulation of Talented Researchers by Japan Society for the Promotion of Science (JSPS) . We thank Arjan den Otter and Nazila Masoud (N 2 -physisorption), Helen de Waard (ICP-OES), and Carlos Hernández Mejía (TPR) for the measurements indicated.

Keywords

Carbon nanotubes
Cobalt
Fischer-Tropsch synthesis
Functionalization
Nanocrystals

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title = "Cobalt nanocrystals on carbon nanotubes in the Fischer-Tropsch synthesis: Impact of support oxidation",

abstract = "The effect of oxidation of a carbon nanotube (CNT) support on the structure and catalytic performance in the Fischer-Tropsch (FT) synthesis of pre-synthesized cobalt nanocrystals (NC) has been investigated. 6 nm CoO-NC were prepared using colloidal techniques and impregnated on pristine and surface-oxidized CNT. The CoO-NC on pristine CNT were reduced completely to Co, while ∼50 \% CoO reduction was observed on oxidized CNT (oxCNT), indicating a stronger Co-support interaction on oxCNT. In FT, the turnover frequency (TOF) after 100 h was exceptionally high on pristine CNT (150·10−3 s-1) against 63·10−3 s-1 on oxCNT. In the initial stage of FT, the TOF was 35 \% lower on oxCNT than on pristine CNT, which matched with 32 \% lower crystallinity of cobalt determined using in situ XRD. Furthermore, deactivation was observed mainly on oxCNT. These results demonstrate the large impact of the support on the structure and performance of nanocrystal-based catalysts.",

keywords = "Carbon nanotubes, Cobalt, Fischer-Tropsch synthesis, Functionalization, Nanocrystals",

author = "\{van Deelen\}, \{T. W.\} and H. Yoshida and R. Oord and J. Ze{\v c}evi{\'c} and Weckhuysen, \{B. M.\} and \{de Jong\}, \{K. P.\}",

year = "2020",

month = mar,

day = "5",

doi = "10.1016/j.apcata.2020.117441",

language = "English",

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T1 - Cobalt nanocrystals on carbon nanotubes in the Fischer-Tropsch synthesis

T2 - Impact of support oxidation

AU - van Deelen, T. W.

AU - Yoshida, H.

AU - Oord, R.

AU - Zečević, J.

AU - Weckhuysen, B. M.

AU - de Jong, K. P.

PY - 2020/3/5

Y1 - 2020/3/5

N2 - The effect of oxidation of a carbon nanotube (CNT) support on the structure and catalytic performance in the Fischer-Tropsch (FT) synthesis of pre-synthesized cobalt nanocrystals (NC) has been investigated. 6 nm CoO-NC were prepared using colloidal techniques and impregnated on pristine and surface-oxidized CNT. The CoO-NC on pristine CNT were reduced completely to Co, while ∼50 % CoO reduction was observed on oxidized CNT (oxCNT), indicating a stronger Co-support interaction on oxCNT. In FT, the turnover frequency (TOF) after 100 h was exceptionally high on pristine CNT (150·10−3 s-1) against 63·10−3 s-1 on oxCNT. In the initial stage of FT, the TOF was 35 % lower on oxCNT than on pristine CNT, which matched with 32 % lower crystallinity of cobalt determined using in situ XRD. Furthermore, deactivation was observed mainly on oxCNT. These results demonstrate the large impact of the support on the structure and performance of nanocrystal-based catalysts.

AB - The effect of oxidation of a carbon nanotube (CNT) support on the structure and catalytic performance in the Fischer-Tropsch (FT) synthesis of pre-synthesized cobalt nanocrystals (NC) has been investigated. 6 nm CoO-NC were prepared using colloidal techniques and impregnated on pristine and surface-oxidized CNT. The CoO-NC on pristine CNT were reduced completely to Co, while ∼50 % CoO reduction was observed on oxidized CNT (oxCNT), indicating a stronger Co-support interaction on oxCNT. In FT, the turnover frequency (TOF) after 100 h was exceptionally high on pristine CNT (150·10−3 s-1) against 63·10−3 s-1 on oxCNT. In the initial stage of FT, the TOF was 35 % lower on oxCNT than on pristine CNT, which matched with 32 % lower crystallinity of cobalt determined using in situ XRD. Furthermore, deactivation was observed mainly on oxCNT. These results demonstrate the large impact of the support on the structure and performance of nanocrystal-based catalysts.

KW - Carbon nanotubes

KW - Cobalt

KW - Fischer-Tropsch synthesis

KW - Functionalization

KW - Nanocrystals

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DO - 10.1016/j.apcata.2020.117441

M3 - Article

AN - SCOPUS:85079118583

SN - 0926-860X

VL - 593

JO - Applied Catalysis A: General

JF - Applied Catalysis A: General

M1 - 117441

ER -

Cobalt nanocrystals on carbon nanotubes in the Fischer-Tropsch synthesis: Impact of support oxidation

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