Propane Transformation on Zn-Modified Zeolite. Effect of the Nature of Zn Species on Alkane Aromatization and Hydrogenolysis

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Propane Transformation on Zn-Modified Zeolite. Effect of the Nature of Zn Species on Alkane Aromatization and Hydrogenolysis. / Arzumanov, Sergei S.; Gabrienko, Anton A.; Toktarev, Alexander V. и др.

в: Journal of Physical Chemistry C, Том 123, № 50, 19.12.2019, стр. 30473-30485.

Результаты исследований: Научные публикации в периодических изданиях › статья › Рецензирование

BibTeX

@article{a94586565e5f4fbab13f559df2b4a304,

title = "Propane Transformation on Zn-Modified Zeolite. Effect of the Nature of Zn Species on Alkane Aromatization and Hydrogenolysis",

abstract = "With regard to establishing the effect of the nature of Zn species loaded in a zeolite on the aromatization of propane, the transformation of 13C-labeled propane (propane-1-13C and propane-2-13C) has been monitored by 1H and 13C (CP) MAS NMR at 296-623 K for two zeolite samples, containing exclusively either isolated Zn2+ cations (Zn2+/H-BEA zeolite sample) or small (ZnO)n clusters of zinc oxide (ZnO/H-BEA zeolite sample). It has been established that similar intermediates, π-complex of propene and σ-allylzinc species, are formed at propane transformation to aromatics on both zeolite samples. However, the formation of the identified intermediates and their evolution to final aromatic products have been detected to occur on Zn2+/H-BEA at lower temperature (by 100 K) as compared to the same transformation on ZnO/H-BEA zeolite. Analysis of the kinetics of propane transformation by 1H MAS NMR in situ has shown similar regularities for propane aromatization and hydrogenolysis on the different zeolite samples, but the reactions on Zn2+/H-BEA occur 10 times faster than on ZnO/H-BEA. This allows us to conclude on a higher efficiency of Zn2+ cations compared to ZnO species for propane aromatization on Zn-modified zeolites.",

keywords = "SOLID-STATE NMR, IN-SITU NMR, BRONSTED ACID SITES, METHANE ACTIVATION, LIGHT ALKANES, ZN/MFI CATALYST, INITIAL-STAGES, H/D EXCHANGE, CONVERSION, H-ZSM-5",

author = "Arzumanov, {Sergei S.} and Gabrienko, {Anton A.} and Toktarev, {Alexander V.} and Lashchinskaya, {Zoya N.} and Dieter Freude and J{\"u}rgen Haase and Stepanov, {Alexander G.}",

year = "2019",

month = dec,

day = "19",

doi = "10.1021/acs.jpcc.9b09718",

language = "English",

volume = "123",

pages = "30473--30485",

journal = "Journal of Physical Chemistry C",

issn = "1932-7447",

publisher = "American Chemical Society",

number = "50",

}

RIS

TY - JOUR

T1 - Propane Transformation on Zn-Modified Zeolite. Effect of the Nature of Zn Species on Alkane Aromatization and Hydrogenolysis

AU - Arzumanov, Sergei S.

AU - Gabrienko, Anton A.

AU - Toktarev, Alexander V.

AU - Lashchinskaya, Zoya N.

AU - Freude, Dieter

AU - Haase, Jürgen

AU - Stepanov, Alexander G.

PY - 2019/12/19

Y1 - 2019/12/19

N2 - With regard to establishing the effect of the nature of Zn species loaded in a zeolite on the aromatization of propane, the transformation of 13C-labeled propane (propane-1-13C and propane-2-13C) has been monitored by 1H and 13C (CP) MAS NMR at 296-623 K for two zeolite samples, containing exclusively either isolated Zn2+ cations (Zn2+/H-BEA zeolite sample) or small (ZnO)n clusters of zinc oxide (ZnO/H-BEA zeolite sample). It has been established that similar intermediates, π-complex of propene and σ-allylzinc species, are formed at propane transformation to aromatics on both zeolite samples. However, the formation of the identified intermediates and their evolution to final aromatic products have been detected to occur on Zn2+/H-BEA at lower temperature (by 100 K) as compared to the same transformation on ZnO/H-BEA zeolite. Analysis of the kinetics of propane transformation by 1H MAS NMR in situ has shown similar regularities for propane aromatization and hydrogenolysis on the different zeolite samples, but the reactions on Zn2+/H-BEA occur 10 times faster than on ZnO/H-BEA. This allows us to conclude on a higher efficiency of Zn2+ cations compared to ZnO species for propane aromatization on Zn-modified zeolites.

AB - With regard to establishing the effect of the nature of Zn species loaded in a zeolite on the aromatization of propane, the transformation of 13C-labeled propane (propane-1-13C and propane-2-13C) has been monitored by 1H and 13C (CP) MAS NMR at 296-623 K for two zeolite samples, containing exclusively either isolated Zn2+ cations (Zn2+/H-BEA zeolite sample) or small (ZnO)n clusters of zinc oxide (ZnO/H-BEA zeolite sample). It has been established that similar intermediates, π-complex of propene and σ-allylzinc species, are formed at propane transformation to aromatics on both zeolite samples. However, the formation of the identified intermediates and their evolution to final aromatic products have been detected to occur on Zn2+/H-BEA at lower temperature (by 100 K) as compared to the same transformation on ZnO/H-BEA zeolite. Analysis of the kinetics of propane transformation by 1H MAS NMR in situ has shown similar regularities for propane aromatization and hydrogenolysis on the different zeolite samples, but the reactions on Zn2+/H-BEA occur 10 times faster than on ZnO/H-BEA. This allows us to conclude on a higher efficiency of Zn2+ cations compared to ZnO species for propane aromatization on Zn-modified zeolites.

KW - SOLID-STATE NMR

KW - IN-SITU NMR

KW - BRONSTED ACID SITES

KW - METHANE ACTIVATION

KW - LIGHT ALKANES

KW - ZN/MFI CATALYST

KW - INITIAL-STAGES

KW - H/D EXCHANGE

KW - CONVERSION

KW - H-ZSM-5

UR - http://www.scopus.com/inward/record.url?scp=85076539474&partnerID=8YFLogxK

U2 - 10.1021/acs.jpcc.9b09718

DO - 10.1021/acs.jpcc.9b09718

M3 - Article

AN - SCOPUS:85076539474

VL - 123

SP - 30473

EP - 30485

JO - Journal of Physical Chemistry C

JF - Journal of Physical Chemistry C

SN - 1932-7447

IS - 50

ER -

ID: 22995472