Metal-organic framework supported single-site nickel catalysts for butene dimerization

Jian Zheng; Laura Löbbert; Saumil Chheda; Navneet Khetrapal; Julian Schmid; Carlo Alberto Gaggioli; Benjamin Yeh; Ricardo Bermejo-Deval; Radha Kishan Motkuri; Mahalingam Balasubramanian; John L. Fulton; Oliver Y. Gutiérrez; J. Ilja Siepmann; Matthew Neurock; Laura Gagliardi; Johannes A. Lercher

doi:10.1016/j.jcat.2022.06.019

Metal-organic framework supported single-site nickel catalysts for butene dimerization

Jian Zheng, Laura Löbbert, Saumil Chheda, Navneet Khetrapal, Julian Schmid, Carlo Alberto Gaggioli, Benjamin Yeh, Ricardo Bermejo-Deval, Radha Kishan Motkuri, Mahalingam Balasubramanian, John L. Fulton, Oliver Y. Gutiérrez, J. Ilja Siepmann, Matthew Neurock, Laura Gagliardi, Johannes A. Lercher

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10 Scopus citations

Abstract

Homotopic sites in a well-controlled environment are not only ideal systems for mechanistic studies, but also allow optimal control of catalytic transformations. Sites having only a single metal cation and sites consisting of metal oxo complexes with few nickel (Ni) cations supported on the nodes of UiO-66 metal–organic framework (Ni-UiO-66) are studied for 1-butene dimerization. Monomeric Ni sites, which bind to the Zr₆ node via two Zr-OH(μ3) linkages, are active and selective for the dimerization of 1-butene to linear and mono-branched C₈ isomers. Ni oxo complexes with few Ni cations show lower activity and promote the oligomerization of transiently formed C8 isomers. Kohn-Sham density function theory calculations combined with spectroscopic measurements and kinetic analyses indicate that dimerization follows a Cossee-Arlman reaction mechanism.

Original language	English (US)
Pages (from-to)	176-183
Number of pages	8
Journal	Journal of Catalysis
Volume	413
DOIs	https://doi.org/10.1016/j.jcat.2022.06.019
State	Published - Sep 2022

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Publisher Copyright:
© 2022

Keywords

Alkene dimerization
Heterogeneous catalysis
Metal–organic framework
Reaction mechanism
Single site catalyst

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Zheng, J., Löbbert, L., Chheda, S., Khetrapal, N., Schmid, J., Gaggioli, C. A., Yeh, B., Bermejo-Deval, R., Motkuri, R. K., Balasubramanian, M., Fulton, J. L., Gutiérrez, O. Y., Siepmann, J. I., Neurock, M., Gagliardi, L., & Lercher, J. A. (2022). Metal-organic framework supported single-site nickel catalysts for butene dimerization. Journal of Catalysis, 413, 176-183. https://doi.org/10.1016/j.jcat.2022.06.019

Zheng, J, Löbbert, L, Chheda, S, Khetrapal, N, Schmid, J, Gaggioli, CA, Yeh, B, Bermejo-Deval, R, Motkuri, RK, Balasubramanian, M, Fulton, JL, Gutiérrez, OY, Siepmann, JI , Neurock, M , Gagliardi, L & Lercher, JA 2022, 'Metal-organic framework supported single-site nickel catalysts for butene dimerization', Journal of Catalysis, vol. 413, pp. 176-183. https://doi.org/10.1016/j.jcat.2022.06.019

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title = "Metal-organic framework supported single-site nickel catalysts for butene dimerization",

abstract = "Homotopic sites in a well-controlled environment are not only ideal systems for mechanistic studies, but also allow optimal control of catalytic transformations. Sites having only a single metal cation and sites consisting of metal oxo complexes with few nickel (Ni) cations supported on the nodes of UiO-66 metal–organic framework (Ni-UiO-66) are studied for 1-butene dimerization. Monomeric Ni sites, which bind to the Zr6 node via two Zr-OH(μ3) linkages, are active and selective for the dimerization of 1-butene to linear and mono-branched C8 isomers. Ni oxo complexes with few Ni cations show lower activity and promote the oligomerization of transiently formed C8 isomers. Kohn-Sham density function theory calculations combined with spectroscopic measurements and kinetic analyses indicate that dimerization follows a Cossee-Arlman reaction mechanism.",

keywords = "Alkene dimerization, Heterogeneous catalysis, Metal–organic framework, Reaction mechanism, Single site catalyst",

author = "Jian Zheng and Laura L{\"o}bbert and Saumil Chheda and Navneet Khetrapal and Julian Schmid and Gaggioli, {Carlo Alberto} and Benjamin Yeh and Ricardo Bermejo-Deval and Motkuri, {Radha Kishan} and Mahalingam Balasubramanian and Fulton, {John L.} and Guti{\'e}rrez, {Oliver Y.} and Siepmann, {J. Ilja} and Matthew Neurock and Laura Gagliardi and Lercher, {Johannes A.}",

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year = "2022",

month = sep,

doi = "10.1016/j.jcat.2022.06.019",

language = "English (US)",

volume = "413",

pages = "176--183",

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T1 - Metal-organic framework supported single-site nickel catalysts for butene dimerization

AU - Zheng, Jian

AU - Löbbert, Laura

AU - Chheda, Saumil

AU - Khetrapal, Navneet

AU - Schmid, Julian

AU - Gaggioli, Carlo Alberto

AU - Yeh, Benjamin

AU - Bermejo-Deval, Ricardo

AU - Motkuri, Radha Kishan

AU - Balasubramanian, Mahalingam

AU - Fulton, John L.

AU - Gutiérrez, Oliver Y.

AU - Siepmann, J. Ilja

AU - Neurock, Matthew

AU - Gagliardi, Laura

AU - Lercher, Johannes A.

PY - 2022/9

Y1 - 2022/9

N2 - Homotopic sites in a well-controlled environment are not only ideal systems for mechanistic studies, but also allow optimal control of catalytic transformations. Sites having only a single metal cation and sites consisting of metal oxo complexes with few nickel (Ni) cations supported on the nodes of UiO-66 metal–organic framework (Ni-UiO-66) are studied for 1-butene dimerization. Monomeric Ni sites, which bind to the Zr6 node via two Zr-OH(μ3) linkages, are active and selective for the dimerization of 1-butene to linear and mono-branched C8 isomers. Ni oxo complexes with few Ni cations show lower activity and promote the oligomerization of transiently formed C8 isomers. Kohn-Sham density function theory calculations combined with spectroscopic measurements and kinetic analyses indicate that dimerization follows a Cossee-Arlman reaction mechanism.

AB - Homotopic sites in a well-controlled environment are not only ideal systems for mechanistic studies, but also allow optimal control of catalytic transformations. Sites having only a single metal cation and sites consisting of metal oxo complexes with few nickel (Ni) cations supported on the nodes of UiO-66 metal–organic framework (Ni-UiO-66) are studied for 1-butene dimerization. Monomeric Ni sites, which bind to the Zr6 node via two Zr-OH(μ3) linkages, are active and selective for the dimerization of 1-butene to linear and mono-branched C8 isomers. Ni oxo complexes with few Ni cations show lower activity and promote the oligomerization of transiently formed C8 isomers. Kohn-Sham density function theory calculations combined with spectroscopic measurements and kinetic analyses indicate that dimerization follows a Cossee-Arlman reaction mechanism.

KW - Alkene dimerization

KW - Heterogeneous catalysis

KW - Metal–organic framework

KW - Reaction mechanism

KW - Single site catalyst

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DO - 10.1016/j.jcat.2022.06.019

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AN - SCOPUS:85132855469

SN - 0021-9517

VL - 413

SP - 176

EP - 183

JO - Journal of Catalysis

JF - Journal of Catalysis

ER -

Metal-organic framework supported single-site nickel catalysts for butene dimerization

Abstract

Bibliographical note

Keywords

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