Suppression of Carbon Deposition in the Iron‐Catalyzed Production of Lower Olefins from Synthesis Gas

Koeken, Ard C. J.; Galvis, Hirsa M. Torres; Davidian, Thomas; Ruitenbeek, Matthijs; Jong, Krijn P. de

doi:10.1002/anie.201200280

Cited by 84 publications

(60 citation statements)

References 24 publications

(22 reference statements)

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“…It is worth noting that most of the Fe-based catalysts for alkene production have astrong tendency to produce alarge amount of CO 2 , [20] and the CO 2 selectivity of Fe catalyst for alkene production in previous reports is normally above 36 % at high temperature. [21] Therefore,t he suppression of CO 2 formation is am ajor task for FTS research at high temperature.S ignificantly,b esides the higher activity,F e-Zn-x Na catalysts show relatively low selectivity towards CO 2 compared to the Fe-Zn catalyst (Table 1, entries 1-4) .…”

Section: Angewandte Chemiementioning

confidence: 99%

Highly Tunable Selectivity for Syngas‐Derived Alkenes over Zinc and Sodium‐Modulated Fe₅C₂ Catalyst

et al. 2016

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Zn- and Na-modulated Fe catalysts were fabricated by a simple coprecipitation/washing method. Zn greatly changed the size of iron species, serving as the structural promoter, while the existence of Na on the surface of the Fe catalyst alters the electronic structure, making the catalyst very active for CO activation. Most importantly, the electronic structure of the catalyst surface suppresses the hydrogenation of double bonds and promotes desorption of products, which renders the catalyst unexpectedly reactive toward alkenes-especially C5+ alkenes (with more than 50% selectivity in hydrocarbons)-while lowering the selectivity for undesired products. This study enriches C1 chemistry and the design of highly selective new catalysts for high-value chemicals.

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Section: Angewandte Chemiementioning

confidence: 99%

Highly Tunable Selectivity for Syngas‐Derived Alkenes over Zinc and Sodium‐Modulated Fe₅C₂ Catalyst

et al. 2016

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“…20-22 %) even at high Cu loading. [16,26,[30][31][32][33][34] Wane tal. After exposing the spent catalysts to hydrogenation conditions, the carboxylate species remained strongly adsorbed whilea liphatic hydrocarbonsa nd formate speciesd isappeared.T he accumulation of oxygenates species on the catalysts urfacei ncreased with Cu loading.…”

Section: Introductionmentioning

confidence: 99%

The Effect of Copper Loading on Iron Carbide Formation and Surface Species in Iron‐Based Fischer–Tropsch Synthesis Catalysts

et al. 2018

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The effect of copper as promoter on iron carbide formation and the nature of surface species on iron‐based catalyst during Fischer–Tropsch synthesis (FTS) was investigated. Iron‐based catalysts (15 wt % of Fe) supported on alumina promoted with copper (0, 0.6, 2, and 5 wt %) were characterised in situ at relevant FTS conditions. The catalysts promoted with 2 and 5 wt % of Cu showed higher catalytic activity due to the formation of Hägg carbide (Fe5C2) detected by in situ XANES and XRD. The carbide formation is attributed to a weakening of the iron–alumina mixed‐compound interactions, and hence increasing iron reducibility and dispersion. The in situ XANES measurements indicated a maximum carburization degree (ca. 20–22 %) even at high Cu loading. The catalyst promoted with 5 wt % of Cu exhibited higher water‐gas shift activity. Aliphatic hydrocarbons, formate, and carboxylate species were detected on the catalyst surface during FTS. After exposing the spent catalysts to hydrogenation conditions, the carboxylate species remained strongly adsorbed while aliphatic hydrocarbons and formate species disappeared. The accumulation of oxygenates species on the catalyst surface increased with Cu loading. The interaction of oxygenates with alumina and iron oxide particles (FexOy) were revealed, with the latter being a possible reason for inhibition of further iron carburization.

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“…The choice of the chemical nature of the support is often subject to considerations such as chemical and mechanical stability under process conditions [37,38]. Textural properties like pore size and surface area are also very relevant in determining the size and stability of the supported metal nanoparticles.…”

Section: Introductionmentioning

confidence: 99%

Interplay between pore size and nanoparticle spatial distribution: Consequences for the stability of CuZn/SiO2 methanol synthesis catalysts

Prieto

Meeldijk

Jong

et al. 2013

Journal of Catalysis

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Particle growth is a major deactivation mechanism for supported metal catalysts. This study reveals that the impact of pore size on catalyst stability is very sensitive to the nanoscale metal distribution. A set of ex-nitrate CuZn/SiO 2 catalysts was synthesised using SiO 2 -gel supports (pore size 5-23 nm). The catalyst compositions were adjusted to attain series of catalysts with either constant pore volumetric (1.6 Cu nm -3 ) or surface (2.0 Cu nm -2 ) overall metal loading. The procedures of thermal decomposition of the metal nitrate precursors were adjusted to achieve < 10 nm Cu particles displaying markedly different nanospatial distributions, i.e either gathered in high-metaldensity domains with small interparticle spacings or evenly distributed over the support with maximum interparticle spacings. Under industrially relevant methanol synthesis conditions, a strong increase of the deactivation rate with the support pore size is observed for catalysts with high-density domains of Cu particles. For these samples the local, nanoscale Cu surface loading is determined by pore size rather than by the overall metal content, as ascertained by HAADF-STEM/EDX.Conversely, Cu nanoparticles evenly spaced on the surface of the SiO 2 carrier show improved stability, being the deactivation rate chiefly independent of the support pore size. The differences in catalyst stability are ascribed to the dominance of different particle growth mechanisms. Our study highlights the significance of local, nanoscale properties for rationalizing the relevance of structural parameters such as pore size for catalyst stability.

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Suppression of Carbon Deposition in the Iron‐Catalyzed Production of Lower Olefins from Synthesis Gas

Cited by 84 publications

References 24 publications

Highly Tunable Selectivity for Syngas‐Derived Alkenes over Zinc and Sodium‐Modulated Fe₅C₂ Catalyst

Highly Tunable Selectivity for Syngas‐Derived Alkenes over Zinc and Sodium‐Modulated Fe₅C₂ Catalyst

The Effect of Copper Loading on Iron Carbide Formation and Surface Species in Iron‐Based Fischer–Tropsch Synthesis Catalysts

Interplay between pore size and nanoparticle spatial distribution: Consequences for the stability of CuZn/SiO2 methanol synthesis catalysts

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Suppression of Carbon Deposition in the Iron‐Catalyzed Production of Lower Olefins from Synthesis Gas

Cited by 84 publications

References 24 publications

Highly Tunable Selectivity for Syngas‐Derived Alkenes over Zinc and Sodium‐Modulated Fe5C2 Catalyst

Highly Tunable Selectivity for Syngas‐Derived Alkenes over Zinc and Sodium‐Modulated Fe5C2 Catalyst

The Effect of Copper Loading on Iron Carbide Formation and Surface Species in Iron‐Based Fischer–Tropsch Synthesis Catalysts

Interplay between pore size and nanoparticle spatial distribution: Consequences for the stability of CuZn/SiO2 methanol synthesis catalysts

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Highly Tunable Selectivity for Syngas‐Derived Alkenes over Zinc and Sodium‐Modulated Fe₅C₂ Catalyst

Highly Tunable Selectivity for Syngas‐Derived Alkenes over Zinc and Sodium‐Modulated Fe₅C₂ Catalyst