Production of Acetonitrile and Other Low Molecular Weight Nitriles

Denton, William I.; Bishop, Richard B.

doi:10.1021/ie50518a021

Cited by 11 publications

(12 citation statements)

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“…To the best of our knowledge, the anaerobic transformation of light alkanes and NH 3 at relatively low temperatures (<500 °C) has not been realized. The only attempt on the production of CH 3 CN from light alkanes and NH 3 , similar to the present study, was made by Denton and Bishop about 70 years ago, which, however, was not quite successful. Here, we demonstrate that the transformation of light alkanes and NH 3 , through the proposed ADeH, to CH 3 CN and CO x free H 2 can be efficiently realized over the metal-modified zeolite, e.g., Pt/HZSM-5, catalysts.…”

Section: Introductionmentioning

confidence: 46%

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: 46%

Catalytic Light Alkanes Conversion through Anaerobic Ammodehydrogenation

et al. 2021

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“…bases. Denton et al 47 proposed the reaction route of ACN production from propylene ammodehydrogenation to be a twostep process: (i) propylene reacts with ammonia to form propionitrile (eqn (1)), following by (ii) propionitrile dissociation to yield ACN and methane by hydrogenolysis (eqn (2)). The first reaction was validated by using a nickel catalyst at 345 °C.…”

Section: Dalton Transactions Perspectivementioning

confidence: 99%

“…This allows the propane ammoxidation to be operated under harsher conditions in a microchannel reactor with restrained CO x selectivity and good stability. 47 A 2-to-1 molar ratio of NH 3 -to-hydrocarbon was used as the feed. Among the tested feedstocks (C 2 -C 5 hydrocarbons), the highest ACN yield was obtained by using ethylene.…”

Section: Perspectivementioning

confidence: 99%

Light hydrocarbon conversion to acrylonitrile and acetonitrile – a review

Trangwachirachai

Lin

2023

Dalton Trans.

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Section: Introductionmentioning

confidence: 99%

“…However, to the best of our knowledge, the ammonia reforming of light alkanes at relatively low temperatures based on thermocatalytic process has not been fully realized according to the only attempt made by Denton and Bishop about 70 years ago. 17 Although plasma-catalytic ammonia reforming of methane can be realized at 400 °C over the Cu/ silicalite-1 catalyst, the energy efficiency is only around 6%. 18 Here, we show that the atomically dispersed ReO x sites grafted into AlO 4 − of the HZSM-5 zeolite are highly active and coke resistant for the thermocatalytic ammonia reforming of ethane and propane at the relevant temperatures (≤650 °C) as the conventional steam/dry reforming.…”

Section: ■ Introductionmentioning

confidence: 99%

Ammonia-Assisted Light Alkane Anti-coke Reforming on Isolated ReO_xSites in Zeolite

Fadaeerayeni

Sarnello

et al. 2022

ACS Catal.

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The conventional reforming produces H 2 with stoichiometric amounts of CO and CO 2 from hydrocarbons. Here, we show that CO x -free H 2 can be produced from ammoniaassisted reforming (ammoreforming) of natural gas liquids (C n H 2n+2 + nNH 3 = nHCN + (2n + 1) H 2 , n = 2 or 3) at the same conditions as the steam reforming. Such a process coproduces HCN, which can be easily separated from H 2 and used as value-added chemicals or for NH 3 recycling through hydrolysis. The ammoreforming of ethane and propane was realized over the Re-modified HZSM-5 zeolite rather than the traditional Pt-based catalyst for the BMA process (methane ammoreforming). The specific activity of the Re/HZSM-5 catalysts at 650 °C is up to 1 mol H 2 /g Re /min (or 180 min −1 ) during ethane ammoreforming. The catalyst is highly coke resistant and shows only slight deactivation with a time-on-stream up to 20 h. Characterization of the fresh and used catalysts by X-ray absorption and Raman spectroscopies suggested that the isolated ReO x site grafted by AlO 4− tetrahedral in the zeolite framework is responsible for the outstanding catalytic activity and coke resistibility. KEYWORDS: light alkanes, ammonia reforming, anti-coke, isolated ReO x , CO x -free H 2

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Production of Acetonitrile and Other Low Molecular Weight Nitriles

Cited by 11 publications

References 0 publications

Catalytic Light Alkanes Conversion through Anaerobic Ammodehydrogenation

Catalytic Light Alkanes Conversion through Anaerobic Ammodehydrogenation

Light hydrocarbon conversion to acrylonitrile and acetonitrile – a review

Ammonia-Assisted Light Alkane Anti-coke Reforming on Isolated ReO_xSites in Zeolite

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Production of Acetonitrile and Other Low Molecular Weight Nitriles

Cited by 11 publications

References 0 publications

Catalytic Light Alkanes Conversion through Anaerobic Ammodehydrogenation

Catalytic Light Alkanes Conversion through Anaerobic Ammodehydrogenation

Light hydrocarbon conversion to acrylonitrile and acetonitrile – a review

Ammonia-Assisted Light Alkane Anti-coke Reforming on Isolated ReOxSites in Zeolite

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Ammonia-Assisted Light Alkane Anti-coke Reforming on Isolated ReO_xSites in Zeolite