Pairwise Parahydrogen Addition Over Molybdenum Carbide Catalysts

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Pairwise Parahydrogen Addition Over Molybdenum Carbide Catalysts. / Burueva, Dudari B.; Smirnov, Andrey A.; Bulavchenko, Olga A. et al.

In: Topics in Catalysis, Vol. 63, No. 1-2, 01.03.2020, p. 2-11.

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

BibTeX

@article{ec2c3e97e0d84695b009f121da9eb733,

title = "Pairwise Parahydrogen Addition Over Molybdenum Carbide Catalysts",

abstract = "Herein, we have shown that the phase composition of molybdenum carbide catalysts has a pronounced effect on the pairwise hydrogen addition selectivity in the gas-phase propyne hydrogenation with parahydrogen. Molybdenum carbide catalysts were prepared using either the Pechini method or temperature-programmed reduction with CH4/H2 carburizing gas mixture. The structures of carbide catalysts were characterized by high-resolution transmission electron microscopy, X-ray diffraction, and X-ray photoelectron spectroscopy. It was found that molybdenum carbide prepared by the Pechini method predominantly contains a face-centered-cubic MoC1−x phase, while the TPR method yields a hexagonal-close-packed Mo2C phase. By varying the gas hourly space velocity of carburizing gas mixture, the defected phase can be produced. Computer modeling for XRD patterns was used to identify the phase composition of Mo2C catalysts. All the catalysts were found to be active in pairwise hydrogen addition; however the hcp-Mo2C phase exhibits a higher contribution of pairwise H2 addition providing ~ 150-fold proton NMR signal enhancement.",

keywords = "Carbide catalysts, Heterogeneous hydrogenation, Molybdenum, Parahydrogen, Parahydrogen-induced polarization, HYDROGENATION REACTIONS, SURFACE-AREA, MECHANISM, CO HYDROGENATION, PHASE, DEHYDROGENATION, KINETICS, INDUCED POLARIZATION, TRANSITION-METAL CARBIDES, TUNGSTEN",

author = "Burueva, {Dudari B.} and Smirnov, {Andrey A.} and Bulavchenko, {Olga A.} and Prosvirin, {Igor P.} and Gerasimov, {Evgeny Yu} and Yakovlev, {Vadim A.} and Kovtunov, {Kirill V.} and Koptyug, {Igor V.}",

year = "2020",

month = mar,

day = "1",

doi = "10.1007/s11244-019-01211-z",

language = "English",

volume = "63",

pages = "2--11",

journal = "Topics in Catalysis",

issn = "1022-5528",

publisher = "Springer Netherlands",

number = "1-2",

}

RIS

TY - JOUR

T1 - Pairwise Parahydrogen Addition Over Molybdenum Carbide Catalysts

AU - Burueva, Dudari B.

AU - Smirnov, Andrey A.

AU - Bulavchenko, Olga A.

AU - Prosvirin, Igor P.

AU - Gerasimov, Evgeny Yu

AU - Yakovlev, Vadim A.

AU - Kovtunov, Kirill V.

AU - Koptyug, Igor V.

PY - 2020/3/1

Y1 - 2020/3/1

N2 - Herein, we have shown that the phase composition of molybdenum carbide catalysts has a pronounced effect on the pairwise hydrogen addition selectivity in the gas-phase propyne hydrogenation with parahydrogen. Molybdenum carbide catalysts were prepared using either the Pechini method or temperature-programmed reduction with CH4/H2 carburizing gas mixture. The structures of carbide catalysts were characterized by high-resolution transmission electron microscopy, X-ray diffraction, and X-ray photoelectron spectroscopy. It was found that molybdenum carbide prepared by the Pechini method predominantly contains a face-centered-cubic MoC1−x phase, while the TPR method yields a hexagonal-close-packed Mo2C phase. By varying the gas hourly space velocity of carburizing gas mixture, the defected phase can be produced. Computer modeling for XRD patterns was used to identify the phase composition of Mo2C catalysts. All the catalysts were found to be active in pairwise hydrogen addition; however the hcp-Mo2C phase exhibits a higher contribution of pairwise H2 addition providing ~ 150-fold proton NMR signal enhancement.

AB - Herein, we have shown that the phase composition of molybdenum carbide catalysts has a pronounced effect on the pairwise hydrogen addition selectivity in the gas-phase propyne hydrogenation with parahydrogen. Molybdenum carbide catalysts were prepared using either the Pechini method or temperature-programmed reduction with CH4/H2 carburizing gas mixture. The structures of carbide catalysts were characterized by high-resolution transmission electron microscopy, X-ray diffraction, and X-ray photoelectron spectroscopy. It was found that molybdenum carbide prepared by the Pechini method predominantly contains a face-centered-cubic MoC1−x phase, while the TPR method yields a hexagonal-close-packed Mo2C phase. By varying the gas hourly space velocity of carburizing gas mixture, the defected phase can be produced. Computer modeling for XRD patterns was used to identify the phase composition of Mo2C catalysts. All the catalysts were found to be active in pairwise hydrogen addition; however the hcp-Mo2C phase exhibits a higher contribution of pairwise H2 addition providing ~ 150-fold proton NMR signal enhancement.

KW - Carbide catalysts

KW - Heterogeneous hydrogenation

KW - Molybdenum

KW - Parahydrogen

KW - Parahydrogen-induced polarization

KW - HYDROGENATION REACTIONS

KW - SURFACE-AREA

KW - MECHANISM

KW - CO HYDROGENATION

KW - PHASE

KW - DEHYDROGENATION

KW - KINETICS

KW - INDUCED POLARIZATION

KW - TRANSITION-METAL CARBIDES

KW - TUNGSTEN

UR - http://www.scopus.com/inward/record.url?scp=85076839543&partnerID=8YFLogxK

U2 - 10.1007/s11244-019-01211-z

DO - 10.1007/s11244-019-01211-z

M3 - Article

AN - SCOPUS:85076839543

VL - 63

SP - 2

EP - 11

JO - Topics in Catalysis

JF - Topics in Catalysis

SN - 1022-5528

IS - 1-2

ER -

ID: 22979141