In situ observation of self-assembled hydrocarbon Fischer–Tropsch products on a cobalt catalyst

Navarro, Violeta; Spronsen, Matthijs A. van; Frenken, J.W.M.

doi:10.1038/nchem.2613

Cited by 99 publications

(81 citation statements)

References 30 publications

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“…Other catalytic reactions that are extremely promising to study in the context of fuel-related catalysis are, e.g., hydrodesulfurization for the treatment of fuels using MoS 2 -based catalysts, 164 or Fischer-Tropsch synthesis for the production of clean fuels from CO-H 2 mixtures using Fe or Co catalysts. [165][166][167] …”

Section: Discussionmentioning

confidence: 99%

Surface science under reaction conditions: CO oxidation on Pt and Pd model catalysts

2017

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Platinum and palladium are frequently used as catalytic materials, for example for the oxidation of CO. This is one of the most widely studied reactions in the field of surface science. Although seemingly uncomplicated, it remains an active and interesting topic, which is partially explained by the push to conduct experiments on model systems under relevant reaction conditions. Recent developments in the surface-science methodology have allowed obtaining chemical and structural information on the active phase of model catalysts. Tools of the trade include near-ambient-pressure X-ray photoelectron spectroscopy, high-pressure scanning tunneling microscopy, high-pressure surface X-ray diffraction, and high-pressure vibrational spectroscopy. Interpretation is often aided by density functional theory in combination with thermodynamic and kinetic modeling. In this review, results for the catalytic oxidation of CO obtained by these techniques are compared. On several of the Pt and Pd surfaces, new structures develop in excess O 2 . For Pt, this requires a much larger excess of O 2 than for Pd. Most of these structures also develop in pure O 2 and are identified as (surface) oxides. A large body of evidence supports the conjecture that these oxides are more reactive than the corresponding O-covered metallic surfaces under similar conditions, although still debated in the literature. An outlook on this developing field, including directions that move away from CO oxidation towards more complex chemistry, concludes this review.

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Section: Discussionmentioning

confidence: 99%

Surface science under reaction conditions: CO oxidation on Pt and Pd model catalysts

2017

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“…The cobalt‐catalyzed FTS reaction has been recognized as a complex structure‐sensitive reaction, which is controlled by crystal size and exposed facets of the active phase . It has been suggested that cobalt particles smaller than 6 nm at low pressure conditions or 8 nm at high pressure conditions displayed a significantly lower turnover frequency (TOF) for CO hydrogenation than larger particles catalysts .…”

Section: Introductionmentioning

confidence: 99%

“…[2,3] The cobalt-catalyzed FTS reaction has been recognized as a complex structure-sensitive reaction, which is controlled by crystal size and exposed facets of the active phase. [4] It has been suggested that cobalt particles smaller than 6 nm at low pressure conditions or 8 nm at high pressure conditions displayed a significantly lower turnover frequency (TOF) for CO hydrogenation than larger particles catalysts. [5,6] Cobalt catalysts with face-centered cubic (fcc) phase is suggested to be more stable than hexagonal close-packed (hcp) phase with the average particle size lower than 20 nm, [7] while the hcp Co exhibits higher CO conversions and C 5 + hydrocarbons selectivity than fcc Co. [8,9] The decrease of cobalt particle size might be accompanied by the phase transformation from hcp Co with higher activity to fcc Co with lower activity.…”

Section: Introductionmentioning

confidence: 99%

Morphology Evolution of Hcp Cobalt Nanoparticles Induced by Ru Promoter

Liu

Qin

et al. 2020

ChemCatChem

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The modification of the equilibrium morphology to expose active facets of cobalt nanoparticles is essential for tailoring and controlling its catalytic performance. Periodic density functional theory (DFT) was applied to systematically investigate the structure and stability of exposed facets of hcp Co nanoparticles induced by Ru promoter in order to clarify the facet‐dependent equilibrium morphology of hcp Co nanoparticles stabilized by Ru promoter. The adsorption and migration of Ru atom can give rise to the change of the surface energy of exposed facets, thus affecting the equilibrium morphology of the hcp Co nanoparticles. Selectively exposed the high Miller index facets, such as Co(10‐12), Co(11‐20) and Co(11‐21) surfaces, can be tuned by adding Ru promoter. Our theoretical calculation results show that Co(11‐21) becomes the predominantly exposed facet accompanied with the decrease of exposed Co(10‐10) and Co(10‐11) with the increase of Ru loading. Further experimental studies suggest that the area of selectively exposed the Co(10‐11) surface for uniform Co nanoplates loaded with 3.0 wt % Ru will be reduced, which is in agreement with the theoretical predicted result. This work is helpful to design the desired Co‐based FTS catalysts rationally with well‐controlled surface structure.

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“…Several research groups have used in situ techniques to explore the FT syngas reaction on cobalt, e.g. scanning tunnelling microscopy (STM), [3][4][5] X-ray diffraction (XRD), 6 and X-ray absorption spectroscopy (XAS), 7,8 yielding meaningful insight into the working state of the catalyst surface under industrially relevant conditions. However, the use of in situ transmission electron microscopy (TEM) has not yet been reported.…”

Section: Introductionmentioning

confidence: 99%

In situ TEM observation of the Boudouard reaction: multi-layered graphene formation from CO on cobalt nanoparticles at atmospheric pressure

et al. 2017

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Using a MEMS nanoreactor in combination with a specially designed in situ Transmission Electron Microscope (TEM) holder and gas supply system, we imaged the formation of multiple layers of graphene encapsulating a cobalt nanoparticle, at 1 bar CO : N (1 : 1) and 500 °C. The cobalt nanoparticle was imaged live in a TEM during the Boudouard reaction. The in situ/operando TEM studies give insight into the behaviour of the catalyst at the nanometer-scale, under industrially relevant conditions. When switching from Fischer-Tropsch syngas conditions (CO : H : N 1 : 2 : 3 at 1 bar) to CO-rich conditions (CO : N 1 : 1 at 1 bar), we observed the formation of multi-layered graphene on Co nanoparticles at 500 °C. Due to the high temperature, the surface of the Co nanoparticles facilitated the Boudouard reaction, causing CO dissociation and the formation of layers of graphene. After the formation of the first patches of graphene at the surface of the nanoparticle, more and more layers grew over the course of about 40 minutes. In its final state, around 10 layers of carbon capped the nanoparticle. During this process, the carbon shell caused mechanical stress in the nanoparticle, inducing permanent deformation.

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In situ observation of self-assembled hydrocarbon Fischer–Tropsch products on a cobalt catalyst

Cited by 99 publications

References 30 publications

Surface science under reaction conditions: CO oxidation on Pt and Pd model catalysts

Surface science under reaction conditions: CO oxidation on Pt and Pd model catalysts

Morphology Evolution of Hcp Cobalt Nanoparticles Induced by Ru Promoter

In situ TEM observation of the Boudouard reaction: multi-layered graphene formation from CO on cobalt nanoparticles at atmospheric pressure

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