Research output: Contribution to journal › Article › peer-review
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.Research output: Contribution to journal › Article › peer-review
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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