Результаты исследований: Научные публикации в периодических изданиях › статья › Рецензирование
Isolated fe sites in metal organic frameworks catalyze the direct conversion of methane to methanol. / Osadchii, Dmitrii Y.; Olivos-Suarez, Alma I.; Szécsényi, Ágnes и др.
в: ACS Catalysis, Том 8, № 6, 01.06.2018, стр. 5542-5548.Результаты исследований: Научные публикации в периодических изданиях › статья › Рецензирование
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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