Influence of carbon support surface modification on the performance of nickel catalysts in carbon dioxide hydrogenation

Visser, Nienke L.; Verschoor, Juliette C.; Smulders, Luc C. J.; Mattarozzi, Francesco; Morgan, David; Meeldijk, Johannes D.; Hoeven, Jessi E. S. van der; Stewart, Joseph; Vandegehuchte, Bart D.; Jongh, Petra E. de

doi:10.1016/j.cattod.2023.114071

Cited by 9 publications

(14 citation statements)

References 70 publications

(109 reference statements)

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“…An experiment with nickel nanoparticles on oxidized carbon (GNP-O) showed significantly less nanoparticle mobility and growth compared to Ni/GNP (Movie S4 and Figure S16), confirming the stabilization of Ni nanoparticles using functionalized carbon. This was in line with results reported for high-pressure CO 2 hydrogenation, where the use of GNP-O limits Ni particle growth . Additionally, carbon support methanation can provide an extra driving force for particle movement, resulting in more directional movement (Figure ), which is also affected by the support morphology.…”

Section: Resultssupporting

confidence: 90%

“…However, a full statistical study is beyond the scope of this paper. We note that the particle growth likely continues at time scales longer than the measurement time used here (80 min), given the extended time scales of deactivation of these catalysts reported in reactor studies 47 and the continuous movement of particles during the measurement (e.g., Figure 3F−J).…”

Section: Resultsmentioning

confidence: 72%

“…The catalysts used for this study contained nickel metal nanoparticles on a sheetlike graphitic carbon support with a surface area of 456 m 2 g −1 (graphitic nanoplatelets, GNP). 47 The average size of the Ni nanoparticles in the fresh catalyst was 4.6 ± 1.2 nm, determined using TEM under vacuum, and the X-ray diffraction (XRD) crystallite size was 4.2 nm. Complete characterization can be found in ref 47.…”

Section: Resultsmentioning

confidence: 99%

“…47 The average size of the Ni nanoparticles in the fresh catalyst was 4.6 ± 1.2 nm, determined using TEM under vacuum, and the X-ray diffraction (XRD) crystallite size was 4.2 nm. Complete characterization can be found in ref 47. Before discussing the results of the in situ observations in detail, it is important to first study the averaged particle growth and validate the observed in situ TEM results, as is done in the first two sections.…”

Section: Resultsmentioning

confidence: 99%

“…As coalescence events are enhanced by collisions of moving particles, minimizing particle movement during catalysis, by ensuring a strong metal− support interaction (influenced by support nature and morphology), is important. This could be accomplished through, for example, support functionalization 47 or adding stability promoters. 65 Here, we achieved a dedicated nanoparticle growth study using a realistic nickel-based catalyst under typical CO 2 hydrogenation conditions.…”

Section: Resultsmentioning

confidence: 99%

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Direct Observation of Ni Nanoparticle Growth in Carbon-Supported Nickel under Carbon Dioxide Hydrogenation Atmosphere

et al. 2023

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Understanding nanoparticle growth is crucial to increase the lifetime of supported metal catalysts. In this study, we employ in situ gas-phase transmission electron microscopy to visualize the movement and growth of ensembles of tens of nickel nanoparticles supported on carbon for CO 2 hydrogenation at atmospheric pressure (H 2 :CO 2 = 4:1) and relevant temperature (450 °C) in real time. We observe two modes of particle movement with an order of magnitude difference in velocity: fast, intermittent movement (v max = 0.7 nm s −1 ) and slow, gradual movement (v average = 0.05 nm s −1 ). We visualize the two distinct particle growth mechanisms: diffusion and coalescence, and Ostwald ripening. The diffusion and coalescence mechanism dominates at small interparticle distances, whereas Ostwald ripening is driven by differences in particle size. Strikingly, we demonstrate an interplay between the two mechanisms, where first coalescence takes place, followed by fast Ostwald ripening due to the increased difference in particle size. Our direct visualization of the complex nanoparticle growth mechanisms highlights the relevance of studying nanoparticle growth in supported nanoparticle ensembles under reaction conditions and contributes to the fundamental understanding of the stability in supported metal catalysts.

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Section: Resultssupporting

confidence: 90%

Section: Resultsmentioning

confidence: 72%

Section: Resultsmentioning

confidence: 99%

Section: Resultsmentioning

confidence: 99%

Section: Resultsmentioning

confidence: 99%

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Direct Observation of Ni Nanoparticle Growth in Carbon-Supported Nickel under Carbon Dioxide Hydrogenation Atmosphere

et al. 2023

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Effect of carbon oxygen functionalization on the activity of Pd/C catalysts in hydrogenation reactions

Stucchi,

Capelli,

Villa

et al. 2024

ChemCatChem

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This paper presents a study on the effects of oxygen functionalities on a mesoporous and graphitized carbon support (GNP, Graphene Nanoplatelets), on the catalytic activity of Pd/GNP catalysts in hydrogenation reactions. A functionalization method in liquid phase has been employed, using different oxidants (HNO3, H2O2, KMnO4), with the aim to tune the amount and the type of introduced oxygen functionalities. Preformed Pd nanoparticles have been used as Pd‐precursor to limit differences in metal particle size and dispersion on differently functionalized carbon. The catalytic behaviour in benzaldehyde hydrogenation/hydrogenolysis to benzyl alcohol and toluene revealed that the introduction of oxygen functionalities has a generally detrimental effect. NMR relaxometry studies highlighted the weaker interaction between the carbonyl group and the functionalized Pd/GNP surface than the non‐functionalized Pd/GNP demonstrating that the origin of the different catalytic activity lies on the first step of the reaction. O‐functionalities also impacted on the Pd0/Pd2+ ratio at the surface which is an established parameter correlated to the reaction rate.

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Design of Experiments for Optimized Synthesis of Carbon‐Supported Ni Nanoparticles: A Green Chemistry Approach

Rigoulet,

Rafaïdeen,

Coutanceau

et al. 2024

ChemElectroChem

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Metallic nickel nanoparticles supported on a high specific surface area carbon powder were synthesized by a classical polyol method without external reducing agent or surfactant. Ni/C materials were characterized by TGA, XRD, cyclic and linear voltammetry. To decrease the number of experiments, a Taguchi design of experiments (DoE) was implemented and the effects of different synthesis parameters (nature of the nickel salt, loading of Ni on carbon, nNaOH/nNi ratio and reaction time at reflux) on different responses (crystallite size, electrochemically active surface area and current density for the glucose oxidation reaction at 1.5 V) determined. Optimization of parameter values for decreasing the crystallite size down to 14 nm was achieved using the DoE. For the other responses, strong interactions between parameters avoided straightforward optimization of parameter values. However, some trends could be drawn from the experimental matrix showing that the synthesis of a catalyst loaded with only 10 wt% Ni, with NiCl2 as precursor salt, with a nNaOH/nNi ratio of 6 for 80 minutes at reflux was a good compromise between atom, time and energy savings, costs efficiencies, and electrochemically active surface area and catalytic activity towards the glucose oxidation reaction, particularly in terms of mass activity.

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Influence of carbon support surface modification on the performance of nickel catalysts in carbon dioxide hydrogenation

Cited by 9 publications

References 70 publications

Direct Observation of Ni Nanoparticle Growth in Carbon-Supported Nickel under Carbon Dioxide Hydrogenation Atmosphere

Direct Observation of Ni Nanoparticle Growth in Carbon-Supported Nickel under Carbon Dioxide Hydrogenation Atmosphere

Effect of carbon oxygen functionalization on the activity of Pd/C catalysts in hydrogenation reactions

Design of Experiments for Optimized Synthesis of Carbon‐Supported Ni Nanoparticles: A Green Chemistry Approach

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