Highly selective Sn/HZSM-5 catalyst for ethane ammoxidation to acetonitrile and ethylene

Liang, Tian; Liu, Xia; He, Yue; Barbosa, Roland; Chen, Genwei; Fan, Wei; Xiang, Yizhi

doi:10.1016/j.apcata.2020.117942

Cited by 13 publications

(29 citation statements)

References 40 publications

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“…Since the production of CH 3 CN strongly depends on the acrylonitrile capacity, an on-purpose technique for CH 3 CN production from the cheap and abundant ethane could be an important alternative. Our recent studies have shown that Co 30 -and Sn 31 -modified HZSM-5 catalysts are active for ethane ammoxidation for CH 3 CN. However, as depicted in Figure 1, the formation of CO 2 and NO x is inevitable under oxidative conditions, 31 which was absent during the anaerobic ADeH.…”

Section: ■ Introductionmentioning

confidence: 96%

“…Our recent studies have shown that Co 30 -and Sn 31 -modified HZSM-5 catalysts are active for ethane ammoxidation for CH 3 CN. However, as depicted in Figure 1, the formation of CO 2 and NO x is inevitable under oxidative conditions, 31 which was absent during the anaerobic ADeH. Additionally, the proposed ADeH is fundamentally different from the existing ammoxidation because they involve different catalytically active sites and mechanisms: the effective ethane ammoxidation catalysts are incompetent for the anaerobic ADeH 32 and vice versa.…”

Section: ■ Introductionmentioning

confidence: 96%

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Catalytic Light Alkanes Conversion through Anaerobic Ammodehydrogenation

et al. 2021

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Catalytic transformation of light alkanes could have considerable practical value, yet remains one of the most challenging areas in catalysis research due to the inertness of the C–H bond. Here, we proposed an efficient ammodehydrogenation (ADeH) catalytic system for the direct C–N linkage between light alkanes and ammonia for CH3CN and H2 (CO x free) production. This breakthrough is achieved over bifunctional metal-modified HZSM-5 catalysts, through the tandem dehydrogenation–amination–dehydrogenation mechanism. We show that ethane ADeH over the Pt/HZSM-5 catalyst can be realized under atmospheric pressure at temperatures as low as 350 °C. The specific rate of CH3CN is ∼60 μmol/(g min), and the selectivity is up to 99% under such mild conditions. The yield of CH3CN increases with increasing temperature; however, the selectivity decreases due to the formation of HCN, C2H4, and CH4. Additionally, the Pt/HZSM-5 catalyst is coke-resistant during the ADeH owing to the strong interaction between NH3 and the acid sites of the catalyst. We anticipate that the proposed ADeH could be extended for the transformation of various n/iso-alkanes with tunable selectivity to alkene and nitriles.

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Section: ■ Introductionmentioning

confidence: 96%

Section: ■ Introductionmentioning

confidence: 96%

Catalytic Light Alkanes Conversion through Anaerobic Ammodehydrogenation

et al. 2021

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“…Alternatively, the Sn/HZSM-5 catalyst has been discovered for ethane ammoxidation. 91 At a similar level of ethane conversion (e.g., 10%), the Sn catalyst exhibited a higher ACN selectivity than the Co catalyst (80% and 60%, respectively). The Sn 4+ species was suggested to be active for ACN production, whereas SnO x would reduce ACN and increase CO 2 yields.…”

Section: Recent 5-years Studies On Acn Synthesis From C 2 Hydrocarbonsmentioning

confidence: 94%

Light hydrocarbon conversion to acrylonitrile and acetonitrile – a review

Trangwachirachai

Lin

2023

Dalton Trans.

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“…Heterogeneous catalytic ammoxidation of alkyl aromatics and heteroaromatics is an essential reaction to synthesize a variety of pharmaceutical and chemical products, characterized by the conversion of methyl to nitrile group. , Some bulk-chemical-product reactions, like propylene to acrylonitrile, − propane to acrylonitrile, − ethane ammoxidation to acetonitrile and ethylene, − have been researched extensively and deeply since the 1970s. However, because of the strong exothermic characteristics of the ammoxidation reaction, efficient heat-transfer and intrinsic-safety had been mainly focused even to now . Additionally, pharmaceutical-product reactions, like ammoxidation of 2-methylpyrazine (MP) to 2-cyanopyrazine (CP), which now is a chosen low cost and short-path route to synthesize antituberculosis (TB) drug pyrazinamide, have attracted gradually increasing attention (Scheme ).…”

Section: Introductionmentioning

confidence: 99%

“…However, because of the strong exothermic characteristics of the ammoxidation reaction, efficient heattransfer and intrinsic-safety had been mainly focused even to now. 14 Additionally, pharmaceutical-product reactions, like ammoxidation of 2-methylpyrazine (MP) to 2-cyanopyrazine (CP), which now is a chosen low cost and short-path route to synthesize antituberculosis (TB) drug pyrazinamide, 3 have attracted gradually increasing attention (Scheme 1).…”

Section: Introductionmentioning

confidence: 99%

Continuous-Flow Ammoxidation of 2-Methylpyrazine to 2-Cyanopyrazine with High Space-Time Yield in a Microreactor

Wei

et al. 2022

ACS Omega

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A microreactor (MR) with a vaporization microchamber and a sinusoidal wave microchannel was fabricated to synthesize 2-cyanopyrazine (CP) directly with an aqueous 2-methylpyrazine (MP) solution. A continuous-flow process with high space-time yield was achieved under the premise of strong exothermality of this ammoxidation reaction. The vanadium metal oxide catalysts with four different supports (α-Al2O3, γ-Al2O3, ZSM-5(50), ZSM-5(80)) were evaluated by simply stacking in the wave microchannel from 350 to 540 °C. The process parameters (temperature, reactant ratio, and size of catalysts) were optimized with the selected CrVPO/γ-Al2O3 catalyst, and an optimal ammoxidation process with MP conversion (X MP) of 71.5% and CP selectivity (S CP) of 93.7% was obtained by a volume space velocity (GHSV) of 13 081 h–1 at 480 °C. Correspondingly, the space-time yield of CP (STYCP) was 1724–77 082 gCPkgcat –1h–1, which was the highest value ever reported for this reaction. Meanwhile, the ammoxidation reaction showed a great continuous-synthesis stability of 50-h running in the microreactor with the CP yield (Y CP) remaining 56%–68%.

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Highly selective Sn/HZSM-5 catalyst for ethane ammoxidation to acetonitrile and ethylene

Cited by 13 publications

References 40 publications

Catalytic Light Alkanes Conversion through Anaerobic Ammodehydrogenation

Catalytic Light Alkanes Conversion through Anaerobic Ammodehydrogenation

Light hydrocarbon conversion to acrylonitrile and acetonitrile – a review

Continuous-Flow Ammoxidation of 2-Methylpyrazine to 2-Cyanopyrazine with High Space-Time Yield in a Microreactor

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