Precursor controlled synthesis of graphene oxide supported iron catalysts for Fischer–Tropsch synthesis

Wei, Yuxue; Luo, Dan; Zhang, Chenghua; Liu, Jingge; He, Yurong; Wen, Xiaodong; Yang, Yong; Li, Yongwang

doi:10.1039/c8cy00617b

Cited by 23 publications

(22 citation statements)

References 47 publications

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“…With varying the catalyst material compositions (e. g., active d-block metal, support material and structural and/or chemical promoters) the catalysts behaviour can be modified. [1,7,16,17,[8][9][10][11][12][13][14][15] General requirements for an industrially good FTS reaction catalyst material are: i) sufficient activity towards FTS reaction, ii) high selectivity for converting the input CO only to the desired hydrocarbons and iii) mechanical and catalytical stability. [4] Despite most of the d-block transition metals being somewhat active towards the FTS reaction, [1,18,19] catalysts based on Fe and Co are the most suitable ones for FTS reaction applications.…”

Section: Introductionmentioning

confidence: 99%

“…With varying the catalyst material compositions (e. g., active d‐block metal, support material and structural and/or chemical promoters) the catalysts behaviour can be modified . General requirements for an industrially good FTS reaction catalyst material are: i) sufficient activity towards FTS reaction, ii) high selectivity for converting the input CO only to the desired hydrocarbons and iii) mechanical and catalytical stability .…”

Section: Introductionmentioning

confidence: 99%

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Carbon Pathways, Sodium‐Sulphur Promotion and Identification of Iron Carbides in Iron‐based Fischer‐Tropsch Synthesis

Paalanen

Weckhuysen

2020

ChemCatChem

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Fisher‐Tropsch Synthesis (FTS) is industrially used for converting a carbon‐containing feedstock, such as coal, natural gas, biomass, and municipal waste, via the production of synthesis gas (a mixture of CO+H2) into hydrocarbons. This review article focuses on Fe‐based FTS catalysis, thereby focusing on the process conditions available for steering the various carbon pathways from input CO and their associated reactions. We will also discuss the effects of alkali‐sulphur chemical promotion and the identification of the FTS reaction active Fe carbides, which are assigned with precise crystal structures and nomenclature. Each observed Fe carbide crystal structure is further assigned with corresponding Mössbauer Absorption Spectroscopy (MAS) hyperfine fields. The expected formation temperatures and experimental conditions for the identified Fe carbides encountered in FTS research, namely ϵ‐Fe3C, η‐Fe2C, χ‐Fe5C2, θ‐Fe3C and θ‐Fe7C3, are reviewed.

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Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Carbon Pathways, Sodium‐Sulphur Promotion and Identification of Iron Carbides in Iron‐based Fischer‐Tropsch Synthesis

Paalanen

Weckhuysen

2020

ChemCatChem

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“…During the in situ synthesis of the NCs, iron ions in solution could covalently interact with oxygen-containing groups on the GO surface via forming Fe–O–C bonds to produce spatially distributed ferrihydrite nuclei (Fe 10 O 14 (OH) 2 ), which serve as “seeds” for nanoparticle growth on rGO nanosheets . In the growth phase, aggregates of seeds could form around these spatially distributed nuclei to eventually produce larger sizes of SPIONs. To validate this, GO concentration in the CEM vessel was increased while keeping other components/parameters constant.…”

Section: Resultsmentioning

confidence: 99%

Polymeric Reactor for the Synthesis of Superparamagnetic-Thermal Treatment of Breast Cancer

et al. 2019

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Engineered superparamagnetic iron oxide nanoparticles (SPIONs) have been studied extensively for their localized homogeneous heat generation in breast cancer therapy. However, challenges such as aggregation and inability to produce sub-10 nm SPIONs limit their potential in magnetothermal ablation. We report a facile, efficient, and robust in situ method for the synthesis of SPIONs within a poly(ethylene glycol) (PEG) reactor adsorbed onto reduced graphene oxide nanosheets (rGO) via the microwave hydrothermal route. This promising modality yields crystalline, stable, biocompatible, and superparamagnetic PEGylated SPION-rGO nanocomposites (NCs) with uniform dispersibility. Our findings show that rGO acts as a breeding ground for the spatially distributed nanosites around which the ferrihydrite seeds accumulate to ultimately transform into immobilized SPIONs. PEG, in parallel, acts as a critical confining agent physically trapping the accumulated seeds to prevent their aggregation and create multiple domains on rGO for the synthesis of quantum-sized SPIONs (9 ± 1 nm in diameter). This dual functionality (rGO and PEG) exhibits a pronounced effect on reducing both the aggregation and the sizes of fabricated SPIONs as confirmed by the scanning transmission electron microscopy images, dynamic light scattering analyses, and the specific absorption rates (SARs). Reduced aggregation lowered the toxicity of NCs, where PEGylated SPION-rGO NCs are more biocompatible than PEGylated SPIONs, showing no significant induction of cell apoptosis, mitochondrial membrane injury, or oxidative stress. Significantly less lactate dehydrogenase release and hence less necrosis are observed after 48 h exposure to high doses of PEGylated SPION-rGO NCs compared with PEGylated SPIONs. NCs induce local heat generation with a SAR value of 1760 ± 97 W/g, reaching up to 43 ± 0.3 °C and causing significant MCF-7 breast tumor cell ablation of about 78 ± 10% upon applying an external magnetic field. Collectively, rGO and PEG functionalities have a synergistic effect on improving the synthesis, stability, biocompatibility, and magnetothermal properties of SPIONs.

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“…Several new examples of nano-carbon based catalysts for the FT chemistry with activity towards the RWGS reaction has previously been generated and tested by Jones et al and others, and the activity was assigned to be due to the embedded and bridging nanoparticles emerging from CVD to as-made carbon nanomaterials or local defects in the nanotube structure. [12,[31][32][33][34][35] These works highlight the ability of graphene to act as a 2D catalyst support compared to previously investigated 3-dimensional structures such as nano-silica and zeolites and present comparable activities with that of similar systems based on multiwalled carbon nanotubes. [10,36]…”

Section: Introductionmentioning

confidence: 95%

Shedding Light Onto the Nature of Iron Decorated Graphene and Graphite Oxide Nanohybrids for CO₂ Conversion at Atmospheric Pressure

et al. 2020

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We report on the design and testing of new graphite and graphene oxide‐based extended π‐conjugated synthetic scaffolds for applications in sustainable chemistry transformations. Nanoparticle‐functionalised carbonaceous catalysts for new Fischer Tropsch and Reverse GasWater Shift (RGWS) transformations were prepared: functional graphene oxides emerged from graphite powders via an adapted Hummer's method and subsequently impregnated with uniform‐sized nanoparticles. Then the resulting nanomaterials were imaged by TEM, SEM, EDX, AFM and characterised by IR, XPS and Raman spectroscopies prior to incorporation of Pd(II) promoters and further microscopic and spectroscopic analysis. Newly synthesised 2D and 3D layered nanostructures incorporating carbon‐supported iron oxide nanoparticulate pre‐catalysts were tested, upon hydrogen reduction in situ, for the conversion of CO2 to CO as well as for the selective formation of CH4 and longer chain hydrocarbons. The reduction reaction was also carried out and the catalytic species isolated and fully characterised. The catalytic activity of a graphene oxide‐supported iron oxide pre‐catalyst converted CO2 into hydrocarbons at different temperatures (305, 335, 370 and 405 °C), and its activity compared well with that of the analogues supported on graphite oxide, the 3‐dimensional material precursor to the graphene oxide. Investigation into the use of graphene oxide as a framework for catalysis showed that it has promising activity with respect to reverse gas water shift (RWGS) reaction of CO2 to CO, even at the low levels of catalyst used and under the rather mild conditions employed at atmospheric pressure. Whilst the γ‐Fe2O3 decorated graphene oxide‐based pre‐catalyst displays fairly constant activity up to 405 °C, it was found by GC‐MS analysis to be unstable with respect to decomposition at higher temperatures. The addition of palladium as a promoter increased the activity of the iron functionalised graphite oxide in the RWGS. The activity of graphene oxide supported catalysts was found to be enhanced with respect to that of iron‐functionalised graphite oxide with, or without palladium as a promoter, and comparable to that of Fe@carbon nanotube‐based systems tested under analogous conditions. These results display a significant step forward for the catalytic activity estimations for the iron functionalised and rapidly processable and scalable graphene oxide. The hereby investigated phenomena are of particular relevance for the understanding of the intimate surface morphologies and the potential role of non‐covalent interactions in the iron oxide‐graphene oxide networks, which could inform the design of nano‐materials with performance in future sustainable catalysis applications.

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Precursor controlled synthesis of graphene oxide supported iron catalysts for Fischer–Tropsch synthesis

Abstract: Iron precursors are used to tune the structure and FTS performance of graphene oxide supported iron catalysts.

Cited by 23 publications

References 47 publications

Carbon Pathways, Sodium‐Sulphur Promotion and Identification of Iron Carbides in Iron‐based Fischer‐Tropsch Synthesis

Carbon Pathways, Sodium‐Sulphur Promotion and Identification of Iron Carbides in Iron‐based Fischer‐Tropsch Synthesis

Polymeric Reactor for the Synthesis of Superparamagnetic-Thermal Treatment of Breast Cancer

Shedding Light Onto the Nature of Iron Decorated Graphene and Graphite Oxide Nanohybrids for CO₂ Conversion at Atmospheric Pressure

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Precursor controlled synthesis of graphene oxide supported iron catalysts for Fischer–Tropsch synthesis

Abstract: Iron precursors are used to tune the structure and FTS performance of graphene oxide supported iron catalysts.

Cited by 23 publications

References 47 publications

Carbon Pathways, Sodium‐Sulphur Promotion and Identification of Iron Carbides in Iron‐based Fischer‐Tropsch Synthesis

Carbon Pathways, Sodium‐Sulphur Promotion and Identification of Iron Carbides in Iron‐based Fischer‐Tropsch Synthesis

Polymeric Reactor for the Synthesis of Superparamagnetic-Thermal Treatment of Breast Cancer

Shedding Light Onto the Nature of Iron Decorated Graphene and Graphite Oxide Nanohybrids for CO2 Conversion at Atmospheric Pressure

Contact Info

Product

Resources

About

Shedding Light Onto the Nature of Iron Decorated Graphene and Graphite Oxide Nanohybrids for CO₂ Conversion at Atmospheric Pressure