Metal organic framework-mediated synthesis of highly active and stable Fischer-Tropsch catalysts

Santos, Vera P.; Wezendonk, Tim A.; Jaén, Juan Josè Delgado; Dugulan, A. Iulian; Nasalevich, Maxim A.; Islam, Husn U.; Chojecki, Adam; Sartipi, Sina; Sun, Xiaohui; Hakeem, Abrar A.; Koeken, Ard C. J.; Ruitenbeek, Matthijs; Davidian, Thomas; Meima, Garry R.; Sankar, Gopinathan; Kapteijn, Freek; Makkee, Michiel; Gascón, Jorge

doi:10.1038/ncomms7451

Cited by 358 publications

(292 citation statements)

References 44 publications

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“…[4,7] This work is intended to probe the iron environments within nanoparticle cementite and Hägg carbide as inactive and active FTS catalyst iron carbide phases in order to improve the understanding of these potential industrial catalysts. Through an increased understanding, and use of the Debye model to ascertain a Debye temperature for these phases, mixed-phase catalysts that have been in service may be studied to determine any differences in phase abundance to relate their abundance to catalytic activity.…”

Section: Introductionmentioning

confidence: 99%

Variable Temperature 57Fe-Mössbauer Spectroscopy Study of Nanoparticle Iron Carbides

Scrimshire¹,

Lobera²,

Kultyshev³

et al. 2015

Croat. Chem. Acta

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Near-phase-pure nanoparticle iron carbides (Fe3C and Fe5C2) were synthesised. Debye model calculations were used with hyperfine parameters gathered by 57 Fe Mössbauer spectroscopy within a temperature range of 10 K to 293 K, with analysis providing Debye temperatures of 422 K and 364 K for two Fe sites in Fe5C2 and 355 K for ferromagnetic Fe3C. The intrinsic isomer shifts were calculated as 0.45 mm s −1 and 0.43 mm s −1 for iron sites 1 and 2 respectively in Fe5C2 and 0.42 mm s −1 for Fe3C. Recoil-free fractions for the two iron sites were also calculated at f300 0.785 and 0.726 for site 1 and 2 respectively.

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Section: Introductionmentioning

confidence: 99%

Variable Temperature 57Fe-Mössbauer Spectroscopy Study of Nanoparticle Iron Carbides

Scrimshire¹,

Lobera²,

Kultyshev³

et al. 2015

Croat. Chem. Acta

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“…Transition metal/ metal oxides, in particular cobalt/cobalt oxide and iron/iron oxide [26,[32][33][34][35][36], are found to be active for oxygen reaction. However, inherent poor conductivity is one factor that limits the application of oxides as electrocatalysts in fuel cells.…”

Section: Mof-derived Transition Metal/metal Oxide-nanocarbon Electrocmentioning

confidence: 99%

“…By delicate design of MOFs precursors, together with careful post-treatment, the advantages and catalytic activity of MOFs materials can be fully inherited by the MOF-derived nanomaterials. For example, MOF-derived heteroatom-doped nanocarbon [28][29][30][31], transition metal/metal oxide-carbon hybrids and composites (as shown in Figure 2) [26,[32][33][34][35][36], with high surface area and porosity, have been reported to exhibit excellent catalytic activity and stability, while also displaying outstanding bifunctional activity toward ORR and oxygen evolution reaction (OER). It should be noted that MOFs precursors employed in developing heteroatom-doped nanocarbon can be conveniently tailored by coupling them with a second heteroatom-containing precursor.…”

Section: A Possible Solution With the Use Of Mof-derived Nanomaterialsmentioning

confidence: 99%

Recent Progress on MOF-Derived Nanomaterials as Advanced Electrocatalysts in Fuel Cells

et al. 2016

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Developing a low cost, highly active and durable cathode material is a high-priority research direction toward the commercialization of low-temperature fuel cells. However, the high cost and low stability of useable materials remain a considerable challenge for the widespread adoption of fuel cell energy conversion devices. The electrochemical performance of fuel cells is still largely hindered by the high loading of noble metal catalyst (Pt/Pt alloy) at the cathode, which is necessary to facilitate the inherently sluggish oxygen reduction reaction (ORR). Under these circumstances, the exploration of alternatives to replace expensive Pt-alloy for constructing highly efficient non-noble metal catalysts has been studied intensively and received great interest. Metal-organic frameworks (MOFs) a novel type of porous crystalline materials, have revealed potential application in the field of clean energy and demonstrated a number of advantages owing to their accessible high surface area, permanent porosity, and abundant metal/organic species. Recently, newly emerging MOFs materials have been used as templates and/or precursors to fabricate porous carbon and related functional nanomaterials, which exhibit excellent catalytic activities toward ORR or oxygen evolution reaction (OER). In this review, recent advances in the use of MOF-derived functional nanomaterials as efficient electrocatalysts in fuel cells are summarized. Particularly, we focus on the rational design and synthesis of highly active and stable porous carbon-based electrocatalysts with various nanostructures by using the advantages of MOFs precursors. Finally, further understanding and development, future trends, and prospects of advanced MOF-derived nanomaterials for more promising applications of clean energy are presented.

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“…Previous results had shown improved activity and product selectivity for Kpromoted Fe@C catalysts 8 , however, 3 unpromoted samples were tested in HT-FTS as well; Fe@C-MIL88, -101NH 2 and -F300 ( Figure 5). Although Fe@C-MIL101NH 2 showed the highest activity after 20 h (X CO = 72.6%), a linear deactivation rate resulted in the lowest CO conversion after 80 h. Fe@C-MIL88 and -F300 displayed an activation period over 50 h after which the CO conversion levels stabilized.…”

Section: Catalytic Testingmentioning

confidence: 99%

“…Since a few years, metal-organic frameworks (MOFs) have emerged from the deep waters of scientific research and have been proposed increasingly as heterogeneous catalysts for many applications, such as Knoevenagel condensation, "click" chemistry, selective hydrogenations, Friedländer coupling, electrocatalysis and photocatalysis 7 . However, we have showed recently that MOFs are not only potent catalysts in their final form, but they also serve the purpose as excellent precursors for high-temperature FTS (HTFTS) catalysts 8 . The concept of the synthesis technique is a simple pyrolysis, heat treatment in an inert atmosphere, which carbonizes the MOF towards embedded metal nanoparticles in a porous C matrix (M@C).…”

Section: Introductionmentioning

confidence: 99%

Structural and elemental influence from various MOFs on the performance of Fe@C catalysts for Fischer–Tropsch synthesis

et al. 2017

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The structure and elementary composition of various commercial Fe-based MOFs used as precursors for Fischer–Tropsch synthesis (FTS) catalysts have a large influence on the high-temperature FTS activity and selectivity of the resulting Fe on carbon composites. The selected Fe-MOF topologies (MIL-68, MIL-88A, MIL-100, MIL-101, MIL-127, and Fe-BTC) differ from each other in terms of porosity, surface area, Fe and heteroatom content, crystal density and thermal stability. They are re-engineered towards FTS catalysts by means of simple pyrolysis at 500 °C under a N2 atmosphere and afterwards characterized in terms of porosity, crystallite phase, bulk and surface Fe content, Fe nanoparticle size and oxidation state. We discovered that the Fe loading (36–46 wt%) and nanoparticle size (3.6–6.8 nm) of the obtained catalysts are directly related to the elementary composition and porosity of the initial MOFs. Furthermore, the carbonization leads to similar surface areas for the C matrix (SBET between 570 and 670 m2 g−1), whereas the pore width distribution is completely different for the various MOFs. The high catalytic performance (FTY in the range of 1.9–4.6 × 10−4 molCO gFe−1 s−1) of the resulting materials could be correlated to the Fe particle size and corresponding surface area, and only minor deactivation was found for the N-containing catalysts. Elemental analysis of the catalysts containing deliberately added promoters and inherent impurities from the commercial MOFs revealed the subtle interplay between Fe particle size and complex catalyst composition in order to obtain high activity and stability next to a low CH4 selectivity.

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Metal organic framework-mediated synthesis of highly active and stable Fischer-Tropsch catalysts

Cited by 358 publications

References 44 publications

Variable Temperature 57Fe-Mössbauer Spectroscopy Study of Nanoparticle Iron Carbides

Variable Temperature 57Fe-Mössbauer Spectroscopy Study of Nanoparticle Iron Carbides

Recent Progress on MOF-Derived Nanomaterials as Advanced Electrocatalysts in Fuel Cells

Structural and elemental influence from various MOFs on the performance of Fe@C catalysts for Fischer–Tropsch synthesis

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