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n-Butane transformation on Zn/H-BEA. The effect of different Zn species (Zn2+ and ZnO) on the reaction performance. / Gabrienko, Anton A.; Arzumanov, Sergei S.; Lashchinskaya, Zoya N. et al.

In: Journal of Catalysis, Vol. 391, 01.11.2020, p. 69-79.

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Gabrienko AA, Arzumanov SS, Lashchinskaya ZN, Toktarev AV, Freude D, Haase J et al. n-Butane transformation on Zn/H-BEA. The effect of different Zn species (Zn2+ and ZnO) on the reaction performance. Journal of Catalysis. 2020 Nov 1;391:69-79. doi: 10.1016/j.jcat.2020.08.011

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@article{84dece5c84f046ad8d70590951a92c66,
title = "n-Butane transformation on Zn/H-BEA. The effect of different Zn species (Zn2+ and ZnO) on the reaction performance",
abstract = "Using solid-state 1H and 13C MAS NMR spectroscopy, the performance of H-BEA zeolite, modified with either Zn2+ cations (Zn2+/H-BEA) or ZnO clusters (ZnO/H-BEA), has been investigated with respect to n-butane transformation by aromatization and hydrogenolysis pathways. 13C-labeled n-butane has been used to follow the main stages of n-butane transformation on both Zn2+/H-BEA and ZnO/H-BEA with 13C MAS NMR at 298–623 K. Similar surface species, including n-butylzinc, n-butene, allyl-like oligomers, are formed as the intermediates on both zeolites. The kinetics of n-butane transformation has been monitored with 1H MAS NMR in situ at 543–573 K. Kinetics modeling reveals that Zn2+/H-BEA is more active for n-butane transformation than ZnO/H-BEA. A remarkable difference in the rates and the pathways of hydrogenolysis for Zn2+/H-BEA and ZnO/H-BEA has also been established. Propane and methane are hydrogenolysis products on ZnO/H-BEA whereas ethane is produced by the reaction on Zn2+/H-BEA. 13C NMR data and the kinetics analysis provide an insight on the occurrence of joint methane and n-butane conversion on Zn-modified zeolites under non-oxidative conditions.",
keywords = "Aromatization, Hydrogenolysis, Kinetics, Mechanism, n-butane, Solid-state NMR, Zeolite BEA, Zn cations, ZnO clusters, SOLID-STATE NMR, SULFATED ZIRCONIA, C-13 MAS NMR, BUTENE CONVERSION, IN-SITU NMR, METHANE ACTIVATION, MODIFIED ZSM-5 ZEOLITES, LIGHT ALKANES, BRONSTED ACID SITES, PROPANE AROMATIZATION",
author = "Gabrienko, {Anton A.} and Arzumanov, {Sergei S.} and Lashchinskaya, {Zoya N.} and Toktarev, {Alexander V.} and Dieter Freude and J{\"u}rgen Haase and Stepanov, {Alexander G.}",
year = "2020",
month = nov,
day = "1",
doi = "10.1016/j.jcat.2020.08.011",
language = "English",
volume = "391",
pages = "69--79",
journal = "Journal of Catalysis",
issn = "0021-9517",
publisher = "Academic Press Inc.",

}

RIS

TY - JOUR

T1 - n-Butane transformation on Zn/H-BEA. The effect of different Zn species (Zn2+ and ZnO) on the reaction performance

AU - Gabrienko, Anton A.

AU - Arzumanov, Sergei S.

AU - Lashchinskaya, Zoya N.

AU - Toktarev, Alexander V.

AU - Freude, Dieter

AU - Haase, Jürgen

AU - Stepanov, Alexander G.

PY - 2020/11/1

Y1 - 2020/11/1

N2 - Using solid-state 1H and 13C MAS NMR spectroscopy, the performance of H-BEA zeolite, modified with either Zn2+ cations (Zn2+/H-BEA) or ZnO clusters (ZnO/H-BEA), has been investigated with respect to n-butane transformation by aromatization and hydrogenolysis pathways. 13C-labeled n-butane has been used to follow the main stages of n-butane transformation on both Zn2+/H-BEA and ZnO/H-BEA with 13C MAS NMR at 298–623 K. Similar surface species, including n-butylzinc, n-butene, allyl-like oligomers, are formed as the intermediates on both zeolites. The kinetics of n-butane transformation has been monitored with 1H MAS NMR in situ at 543–573 K. Kinetics modeling reveals that Zn2+/H-BEA is more active for n-butane transformation than ZnO/H-BEA. A remarkable difference in the rates and the pathways of hydrogenolysis for Zn2+/H-BEA and ZnO/H-BEA has also been established. Propane and methane are hydrogenolysis products on ZnO/H-BEA whereas ethane is produced by the reaction on Zn2+/H-BEA. 13C NMR data and the kinetics analysis provide an insight on the occurrence of joint methane and n-butane conversion on Zn-modified zeolites under non-oxidative conditions.

AB - Using solid-state 1H and 13C MAS NMR spectroscopy, the performance of H-BEA zeolite, modified with either Zn2+ cations (Zn2+/H-BEA) or ZnO clusters (ZnO/H-BEA), has been investigated with respect to n-butane transformation by aromatization and hydrogenolysis pathways. 13C-labeled n-butane has been used to follow the main stages of n-butane transformation on both Zn2+/H-BEA and ZnO/H-BEA with 13C MAS NMR at 298–623 K. Similar surface species, including n-butylzinc, n-butene, allyl-like oligomers, are formed as the intermediates on both zeolites. The kinetics of n-butane transformation has been monitored with 1H MAS NMR in situ at 543–573 K. Kinetics modeling reveals that Zn2+/H-BEA is more active for n-butane transformation than ZnO/H-BEA. A remarkable difference in the rates and the pathways of hydrogenolysis for Zn2+/H-BEA and ZnO/H-BEA has also been established. Propane and methane are hydrogenolysis products on ZnO/H-BEA whereas ethane is produced by the reaction on Zn2+/H-BEA. 13C NMR data and the kinetics analysis provide an insight on the occurrence of joint methane and n-butane conversion on Zn-modified zeolites under non-oxidative conditions.

KW - Aromatization

KW - Hydrogenolysis

KW - Kinetics

KW - Mechanism

KW - n-butane

KW - Solid-state NMR

KW - Zeolite BEA

KW - Zn cations

KW - ZnO clusters

KW - SOLID-STATE NMR

KW - SULFATED ZIRCONIA

KW - C-13 MAS NMR

KW - BUTENE CONVERSION

KW - IN-SITU NMR

KW - METHANE ACTIVATION

KW - MODIFIED ZSM-5 ZEOLITES

KW - LIGHT ALKANES

KW - BRONSTED ACID SITES

KW - PROPANE AROMATIZATION

UR - http://www.scopus.com/inward/record.url?scp=85090047528&partnerID=8YFLogxK

U2 - 10.1016/j.jcat.2020.08.011

DO - 10.1016/j.jcat.2020.08.011

M3 - Article

AN - SCOPUS:85090047528

VL - 391

SP - 69

EP - 79

JO - Journal of Catalysis

JF - Journal of Catalysis

SN - 0021-9517

ER -

ID: 25292853