Efficient oxidative dehydrogenation of ethanol by VOx@MIL-101: On par with VOx/ZrO2 and much better than MIL-47(V)

Bulánek, Roman; Čičmanec, Pavel; Kotera, Jiří; Boldog, Ishtvan

doi:10.1016/j.cattod.2018.07.034

Cited by 10 publications

(8 citation statements)

References 71 publications

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“…Due to this attractiveness, different catalyst systems have been studied for ethanol ODH. The main classes of investigated catalysts are supported metal oxides, mainly supported VO x , [7][8][9][10][11][12][13][14][15][16][17][18][19][20][21][22][23][24] mixed metal oxides, [25,26] supported metal catalysts [27][28][29][30] or carbon-based catalysts. [31][32][33] Supported vanadium oxide catalysts show high activity in the ODH of ethanol.…”

Section: Introductionmentioning

confidence: 99%

Activity, Selectivity and Initial Degradation of Iron Molybdate in the Oxidative Dehydrogenation of Ethanol

et al. 2022

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Iron molybdate catalysts are applied in the industrial FormOx process to produce formaldehyde by oxidative dehydrogenation (ODH) of methanol. Only few studies are available about the applicability of iron molybdate catalysts for the ODH of ethanol to produce acetaldehyde. Herein, an iron molybdate synthesized by co-precipitation (p) and an iron molybdate prepared by a ball-milling solid-state synthesis (bm) are applied as ethanol ODH catalysts. Both materials show attractive acetaldehyde selectivites of > 90 % (280 °C: p-Fe 2 (MoO 4 ) 3 : Y AcH = 90.3 %; bm-Fe 2 (MoO 4 ) 3 : Y AcH = 60.4 %) and a stable performance.The bulk composition and crystal structure could be confirmed by various characterization techniques and is maintained during ethanol ODH. XPS reveals an enrichment of Mo on the catalyst surface which is slightly decreasing after the catalytic tests. This observation could be a first sign of long-term deactivation like known from methanol ODH. Comparing the performance of both materials, p-Fe 2 (MoO 4 ) 3 shows higher activity and aldehyde selectivity. We propose the higher Mo/Fe surface ratio and the lower acidity to be the reasons for these differences.

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Section: Introductionmentioning

confidence: 99%

Activity, Selectivity and Initial Degradation of Iron Molybdate in the Oxidative Dehydrogenation of Ethanol

et al. 2022

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“…84 Among them, MIL-47 has been widely studied because of its large pores (aperture sizes: 10.5 × 11.0 Å, taking into account the van der Waals radii), flexible and open structure, as well as the large specific surface area (S BET = 930 m 2 /g, S Langmuir = 1320 m 2 /g). [90][91][92][93][94][95][96][97][98][99][100] From a structural point of view, it is built from infinite chains of corner-sharing VO 6 octahedra and interconnected by terephthalate groups, creating a three-dimensional topology of orthorhombic structure. MIL-47 also exhibits the similar breathing effects to MIL-53 (Cr), 101,102 the guest molecules trapped in V-MOFs possessing {V − O − V} ∞ chains which can be removed by thermal activation to form empty pores.…”

Section: The Pristine V-mofsmentioning

confidence: 99%

“…In the case of the former, the synthetic form of V‐MOFs contains octahedral [V III (OH)(R‐(CO 2 ) 2 )] infinite long chains, and some of the representatives include MIL‐47, 79 MIL‐68, 80 COMOC‐2, 78 COMOC‐3, 82,88 (COMOC stands for Center for Ordered Materials, Organometallics and Catalysis, Ghent University) MIL‐60, 83 and MIL‐71 84 . Among them, MIL‐47 has been widely studied because of its large pores (aperture sizes: 10.5 × 11.0 Å, taking into account the van der Waals radii), flexible and open structure, as well as the large specific surface area ( S BET = 930 m 2 /g, S Langmuir = 1320 m 2 /g) 90–100 . From a structural point of view, it is built from infinite chains of corner‐sharing VO 6 octahedra and interconnected by terephthalate groups, creating a three‐dimensional topology of orthorhombic structure.…”

Section: V‐mofsmentioning

confidence: 99%

Vanadium‐based metal‐organic frameworks and their derivatives for electrochemical energy conversion and storage

et al. 2022

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With the excessive consumption of nonrenewable resources, the exploration of effective and durable materials is highly sought after in the field of sustainable energy conversion and storage system. In this aspect, metalorganic frameworks (MOFs) are a new class of crystalline porous organicinorganic hybrid materials. MOFs have recently been gaining traction in energy-related fields. Owing to the coordination flexibility and multiple accessible oxidation states of vanadium ions or clusters, vanadium-MOFs (V-MOFs) possess unique structural characteristics and satisfactory electrochemical properties. Furthermore, V-MOFs-derived materials also exhibit superior electrical conductivity and stability when used as electrocatalysts and electrode materials. This review summarizes the research progress of V-MOFs (inclusive of pristine V-MOFs, V/M-MOFs, and POVbased MOFs) and their derivatives (vanadium oxides, carbon-coated vanadium oxide, vanadium phosphate, vanadate, and other vanadium doped nanomaterials) in electrochemical energy conversion (water splitting, oxygen reduction reaction) and energy storage (supercapacitor, rechargeable battery). Future possibilities and challenges for V-MOFs and their derivatives in terms of design and synthesis are discussed. Lastly, their applications in energy-related fields are also highlighted.

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“…Phan et al reported two vanadium-containing MOFs, MIL-47 and MOF-48, having a high catalytic activity toward the selective oxidation of methane to acetic acid in the presence of K 2 S 2 O 8 as an oxidant . Bulánek et al reported an efficient oxidative dehydrogenation of ethanol using VO x -incorporated MIL-101(Cr) MOF . A vanadium-based SSHC, exploiting the MFU-4 l framework, was reported to have high selectivity in olefin polymerization .…”

Section: Introductionmentioning

confidence: 99%

“…12 Bulańek et al reported an efficient oxidative dehydrogenation of ethanol using VO xincorporated MIL-101(Cr) MOF. 13 A vanadium-based SSHC, exploiting the MFU-4l framework, was reported to have high selectivity in olefin polymerization. 14 MOFs containing V (III) or V (IV) as metal nodes and their application in oxidation catalysis and gas separation have been reported as well.…”

Section: ■ Introductionmentioning

confidence: 99%

Structure and Reactivity of Single-Site Vanadium Catalysts Supported on Metal–Organic Frameworks

et al. 2020

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Single-site catalysts with active species anchored over metal−organic framework (MOF) supports have garnered significant interest in recent years. Catalysts with vanadium oxide (VO x ) species immobilized over Zr-NU-1000 and Hf-MOF-808 (which have nodes containing six Zr (IV) or Hf (IV) ions, respectively) were recently characterized experimentally (Otake et al. J. Am. Chem. Soc. 2018, 140, 8652) and were reported to be active for the selective oxidation of benzyl alcohol to benzaldehyde. Here, we report a detailed computational investigation of these VO xincorporated MOF catalysts (V-MOF) by employing density functional theory. Based on the mode of VO x attachment, various structures are explored, and their relative stabilities and computed IR spectral features are reported. Mechanisms for the selective oxidation reaction are investigated. The analysis of electron flow in the turnover-limiting C−H activation step shows that the hydrogen-atom abstraction process involves a concerted proton-coupled electron-transfer mechanism. The results of this study suggest that in addition to the identity of the metal in the node, the MOF node architecture plays a crucial role in driving the catalytic activities of V-MOFs.

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Efficient oxidative dehydrogenation of ethanol by VOx@MIL-101: On par with VOx/ZrO2 and much better than MIL-47(V)

Cited by 10 publications

References 71 publications

Activity, Selectivity and Initial Degradation of Iron Molybdate in the Oxidative Dehydrogenation of Ethanol

Activity, Selectivity and Initial Degradation of Iron Molybdate in the Oxidative Dehydrogenation of Ethanol

Vanadium‐based metal‐organic frameworks and their derivatives for electrochemical energy conversion and storage

Structure and Reactivity of Single-Site Vanadium Catalysts Supported on Metal–Organic Frameworks

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