Standard

Isolated fe sites in metal organic frameworks catalyze the direct conversion of methane to methanol. / Osadchii, Dmitrii Y.; Olivos-Suarez, Alma I.; Szécsényi, Ágnes et al.

In: ACS Catalysis, Vol. 8, No. 6, 01.06.2018, p. 5542-5548.

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

Harvard

Osadchii, DY, Olivos-Suarez, AI, Szécsényi, Á, Li, G, Nasalevich, MA, Dugulan, IA, Crespo, PS, Hensen, EJM, Veber, SL, Fedin, MV, Sankar, G, Pidko, EA & Gascon, J 2018, 'Isolated fe sites in metal organic frameworks catalyze the direct conversion of methane to methanol', ACS Catalysis, vol. 8, no. 6, pp. 5542-5548. https://doi.org/10.1021/acscatal.8b00505

APA

Osadchii, D. Y., Olivos-Suarez, A. I., Szécsényi, Á., Li, G., Nasalevich, M. A., Dugulan, I. A., Crespo, P. S., Hensen, E. J. M., Veber, S. L., Fedin, M. V., Sankar, G., Pidko, E. A., & Gascon, J. (2018). Isolated fe sites in metal organic frameworks catalyze the direct conversion of methane to methanol. ACS Catalysis, 8(6), 5542-5548. https://doi.org/10.1021/acscatal.8b00505

Vancouver

Osadchii DY, Olivos-Suarez AI, Szécsényi Á, Li G, Nasalevich MA, Dugulan IA et al. Isolated fe sites in metal organic frameworks catalyze the direct conversion of methane to methanol. ACS Catalysis. 2018 Jun 1;8(6):5542-5548. doi: 10.1021/acscatal.8b00505

Author

Osadchii, Dmitrii Y. ; Olivos-Suarez, Alma I. ; Szécsényi, Ágnes et al. / Isolated fe sites in metal organic frameworks catalyze the direct conversion of methane to methanol. In: ACS Catalysis. 2018 ; Vol. 8, No. 6. pp. 5542-5548.

BibTeX

@article{df2bec8924ff4657bd09c25e7afb1d58,
title = "Isolated fe sites in metal organic frameworks catalyze the direct conversion of methane to methanol",
abstract = "Hybrid materials bearing organic and inorganic motifs have been extensively discussed as playgrounds for the implementation of atomically resolved inorganic sites within a confined environment, with an exciting similarity to enzymes. Here, we present the successful design of a site-isolated mixed-metal metal organic framework (MOF) that mimics the reactivity of soluble methane monooxygenase enzyme and demonstrates the potential of this strategy to overcome current challenges in selective methane oxidation. We describe the synthesis and characterization of an Fe-containing MOF that comprises the desired antiferromagnetically coupled high-spin species in a coordination environment closely resembling that of the enzyme. An electrochemical synthesis method is used to build the microporous MOF matrix while integrating the atomically dispersed Fe active sites in the crystalline scaffold. The model mimics the catalytic C-H activation behavior of the enzyme to produce methanol and shows that the key to this reactivity is the formation of isolated oxo-bridged Fe units.",
keywords = "MOFs, methane oxidation, isolated metal sites, enzyme-mimicing catalysts, LOW-TEMPERATURE, ACTIVE-SITE, MONOOXYGENASE, OXIDATION, ZEOLITES, HYDROXYLATION, ACTIVATION, ENZYMES, OXYGEN, MODEL",
author = "Osadchii, {Dmitrii Y.} and Olivos-Suarez, {Alma I.} and {\'A}gnes Sz{\'e}cs{\'e}nyi and Guanna Li and Nasalevich, {Maxim A.} and Dugulan, {Iulian A.} and Crespo, {Pablo Serra} and Hensen, {Emiel J.M.} and Veber, {Sergey L.} and Fedin, {Matvey V.} and Gopinathan Sankar and Pidko, {Evgeny A.} and Jorge Gascon",
note = "Publisher Copyright: {\textcopyright} 2018 American Chemical Society.",
year = "2018",
month = jun,
day = "1",
doi = "10.1021/acscatal.8b00505",
language = "English",
volume = "8",
pages = "5542--5548",
journal = "ACS Catalysis",
issn = "2155-5435",
publisher = "American Chemical Society",
number = "6",

}

RIS

TY - JOUR

T1 - Isolated fe sites in metal organic frameworks catalyze the direct conversion of methane to methanol

AU - Osadchii, Dmitrii Y.

AU - Olivos-Suarez, Alma I.

AU - Szécsényi, Ágnes

AU - Li, Guanna

AU - Nasalevich, Maxim A.

AU - Dugulan, Iulian A.

AU - Crespo, Pablo Serra

AU - Hensen, Emiel J.M.

AU - Veber, Sergey L.

AU - Fedin, Matvey V.

AU - Sankar, Gopinathan

AU - Pidko, Evgeny A.

AU - Gascon, Jorge

N1 - Publisher Copyright: © 2018 American Chemical Society.

PY - 2018/6/1

Y1 - 2018/6/1

N2 - Hybrid materials bearing organic and inorganic motifs have been extensively discussed as playgrounds for the implementation of atomically resolved inorganic sites within a confined environment, with an exciting similarity to enzymes. Here, we present the successful design of a site-isolated mixed-metal metal organic framework (MOF) that mimics the reactivity of soluble methane monooxygenase enzyme and demonstrates the potential of this strategy to overcome current challenges in selective methane oxidation. We describe the synthesis and characterization of an Fe-containing MOF that comprises the desired antiferromagnetically coupled high-spin species in a coordination environment closely resembling that of the enzyme. An electrochemical synthesis method is used to build the microporous MOF matrix while integrating the atomically dispersed Fe active sites in the crystalline scaffold. The model mimics the catalytic C-H activation behavior of the enzyme to produce methanol and shows that the key to this reactivity is the formation of isolated oxo-bridged Fe units.

AB - Hybrid materials bearing organic and inorganic motifs have been extensively discussed as playgrounds for the implementation of atomically resolved inorganic sites within a confined environment, with an exciting similarity to enzymes. Here, we present the successful design of a site-isolated mixed-metal metal organic framework (MOF) that mimics the reactivity of soluble methane monooxygenase enzyme and demonstrates the potential of this strategy to overcome current challenges in selective methane oxidation. We describe the synthesis and characterization of an Fe-containing MOF that comprises the desired antiferromagnetically coupled high-spin species in a coordination environment closely resembling that of the enzyme. An electrochemical synthesis method is used to build the microporous MOF matrix while integrating the atomically dispersed Fe active sites in the crystalline scaffold. The model mimics the catalytic C-H activation behavior of the enzyme to produce methanol and shows that the key to this reactivity is the formation of isolated oxo-bridged Fe units.

KW - MOFs

KW - methane oxidation

KW - isolated metal sites

KW - enzyme-mimicing catalysts

KW - LOW-TEMPERATURE

KW - ACTIVE-SITE

KW - MONOOXYGENASE

KW - OXIDATION

KW - ZEOLITES

KW - HYDROXYLATION

KW - ACTIVATION

KW - ENZYMES

KW - OXYGEN

KW - MODEL

UR - http://www.scopus.com/inward/record.url?scp=85046948463&partnerID=8YFLogxK

U2 - 10.1021/acscatal.8b00505

DO - 10.1021/acscatal.8b00505

M3 - Article

AN - SCOPUS:85046948463

VL - 8

SP - 5542

EP - 5548

JO - ACS Catalysis

JF - ACS Catalysis

SN - 2155-5435

IS - 6

ER -

ID: 14102791