Spatially resolved NMR spectroscopy of heterogeneous gas phase hydrogenation of 1,3-butadiene with

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Spatially resolved NMR spectroscopy of heterogeneous gas phase hydrogenation of 1,3-butadiene with : Para hydrogen. / Svyatova, Alexandra; Kononenko, Elizaveta S.; Kovtunov, Kirill V. et al.

In: Catalysis Science and Technology, Vol. 10, No. 1, 07.01.2020, p. 99-104.

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

Author

Svyatova, Alexandra ; Kononenko, Elizaveta S. ; Kovtunov, Kirill V. et al. / Spatially resolved NMR spectroscopy of heterogeneous gas phase hydrogenation of 1,3-butadiene with : Para hydrogen. In: Catalysis Science and Technology. 2020 ; Vol. 10, No. 1. pp. 99-104.

BibTeX

@article{127cdff41d3d47c78826e340fcdcae4f,

title = "Spatially resolved NMR spectroscopy of heterogeneous gas phase hydrogenation of 1,3-butadiene with: Para hydrogen",

abstract = "Magnetic resonance-based methods such as nuclear magnetic resonance (NMR) and magnetic resonance imaging (MRI) are widely used to provide in situ/operando information of chemical reactions. However, the low spin density and magnetic field inhomogeneities associated with heterogeneous catalytic systems containing gaseous reactants complicate such studies. Hyperpolarization techniques, in particular parahydrogen-induced polarization (PHIP), increase significantly the NMR signal intensity. In this study, we test 16 glass tube reactors containing Pd, Pt, Rh or Ir nanoparticles dispersed on a thin layer of TiO2, CeO2, SiO2 or Al2O3 for the hydrogenation of 1,3-butadiene using parahydrogen. The catalytic coatings of Ir and Rh gave hydrogenation products with the highest nuclear spin polarization while the coatings of Pd are the most selective ones for the semihydrogenation of 1,3-butadiene to 1- and 2-butenes. Spatially resolved NMR spectroscopy of the reagent and the product distribution along the reactor axis provided further mechanistic insight into the catalytic function of these reactive coatings under operando conditions.",

keywords = "INDUCED POLARIZATION, MASS-TRANSPORT, SPIN-EXCHANGE, MRI, CATALYSTS, REACTORS, HYPERPOLARIZATION, FLOW",

author = "Alexandra Svyatova and Kononenko, {Elizaveta S.} and Kovtunov, {Kirill V.} and Dmitry Lebedev and Gerasimov, {Evgeniy Yu} and Bukhtiyarov, {Andrey V.} and Prosvirin, {Igor P.} and Bukhtiyarov, {Valerii I.} and M{\"u}ller, {Christoph R.} and Alexey Fedorov and Koptyug, {Igor V.}",

year = "2020",

month = jan,

day = "7",

doi = "10.1039/c9cy02100k",

language = "English",

volume = "10",

pages = "99--104",

journal = "Catalysis Science and Technology",

issn = "2044-4753",

publisher = "Royal Society of Chemistry",

number = "1",

}

RIS

TY - JOUR

T1 - Spatially resolved NMR spectroscopy of heterogeneous gas phase hydrogenation of 1,3-butadiene with

T2 - Para hydrogen

AU - Svyatova, Alexandra

AU - Kononenko, Elizaveta S.

AU - Kovtunov, Kirill V.

AU - Lebedev, Dmitry

AU - Gerasimov, Evgeniy Yu

AU - Bukhtiyarov, Andrey V.

AU - Prosvirin, Igor P.

AU - Bukhtiyarov, Valerii I.

AU - Müller, Christoph R.

AU - Fedorov, Alexey

AU - Koptyug, Igor V.

PY - 2020/1/7

Y1 - 2020/1/7

N2 - Magnetic resonance-based methods such as nuclear magnetic resonance (NMR) and magnetic resonance imaging (MRI) are widely used to provide in situ/operando information of chemical reactions. However, the low spin density and magnetic field inhomogeneities associated with heterogeneous catalytic systems containing gaseous reactants complicate such studies. Hyperpolarization techniques, in particular parahydrogen-induced polarization (PHIP), increase significantly the NMR signal intensity. In this study, we test 16 glass tube reactors containing Pd, Pt, Rh or Ir nanoparticles dispersed on a thin layer of TiO2, CeO2, SiO2 or Al2O3 for the hydrogenation of 1,3-butadiene using parahydrogen. The catalytic coatings of Ir and Rh gave hydrogenation products with the highest nuclear spin polarization while the coatings of Pd are the most selective ones for the semihydrogenation of 1,3-butadiene to 1- and 2-butenes. Spatially resolved NMR spectroscopy of the reagent and the product distribution along the reactor axis provided further mechanistic insight into the catalytic function of these reactive coatings under operando conditions.

AB - Magnetic resonance-based methods such as nuclear magnetic resonance (NMR) and magnetic resonance imaging (MRI) are widely used to provide in situ/operando information of chemical reactions. However, the low spin density and magnetic field inhomogeneities associated with heterogeneous catalytic systems containing gaseous reactants complicate such studies. Hyperpolarization techniques, in particular parahydrogen-induced polarization (PHIP), increase significantly the NMR signal intensity. In this study, we test 16 glass tube reactors containing Pd, Pt, Rh or Ir nanoparticles dispersed on a thin layer of TiO2, CeO2, SiO2 or Al2O3 for the hydrogenation of 1,3-butadiene using parahydrogen. The catalytic coatings of Ir and Rh gave hydrogenation products with the highest nuclear spin polarization while the coatings of Pd are the most selective ones for the semihydrogenation of 1,3-butadiene to 1- and 2-butenes. Spatially resolved NMR spectroscopy of the reagent and the product distribution along the reactor axis provided further mechanistic insight into the catalytic function of these reactive coatings under operando conditions.

KW - INDUCED POLARIZATION

KW - MASS-TRANSPORT

KW - SPIN-EXCHANGE

KW - MRI

KW - CATALYSTS

KW - REACTORS

KW - HYPERPOLARIZATION

KW - FLOW

UR - http://www.scopus.com/inward/record.url?scp=85077515136&partnerID=8YFLogxK

U2 - 10.1039/c9cy02100k

DO - 10.1039/c9cy02100k

M3 - Article

AN - SCOPUS:85077515136

VL - 10

SP - 99

EP - 104

JO - Catalysis Science and Technology

JF - Catalysis Science and Technology

SN - 2044-4753

IS - 1

ER -

ID: 23121061