2H Solid-State NMR Spectroscopy Reveals the Dynamics of a Pyridine Probe Interacting with Coordinatively Unsaturated Metal Sites of MIL-100(Al) Metal

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²H Solid-State NMR Spectroscopy Reveals the Dynamics of a Pyridine Probe Interacting with Coordinatively Unsaturated Metal Sites of MIL-100(Al) Metal–Organic Frameworks. / Khudozhitkov, Alexander E.; Toktarev, Alexander V.; Arzumanov, Sergei S. et al.

In: Chemistry - A European Journal, Vol. 25, No. 46, 14.08.2019, p. 10808-10812.

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

BibTeX

@article{d9c1d9258d77478cb5e916c1fde61b22,

title = "2H Solid-State NMR Spectroscopy Reveals the Dynamics of a Pyridine Probe Interacting with Coordinatively Unsaturated Metal Sites of MIL-100(Al) Metal–Organic Frameworks",

abstract = "Coordinatively unsaturated metal sites (CUS) play an important role in catalysis by metal-organic frameworks (MOF). Being an intrinsic part of the framework the CUS take the role of acidic sites active in industrially relevant processes such as condensation or oxidation reactions. The key step of such reactions represents the coordination of the reagents to CUS. In MOFs the mechanism of the reagent interaction with CUS is poorly understood. Herein, we characterize the interaction of a widely used acidity probe pyridine with CUS of MIL-100(Al) MOF by means of the 2H solid-state NMR spectroscopy. 2H NMR reveals that pyridine species, which are interacting with CUS and the ones which are coordinated to the Al−OH site, exhibit different motional behavior. 2H NMR line shape as well as T1, T2 relaxation analyses for [D5]pyridine adsorbed in MIL-100(Al) allowed us to perform a detailed characterization of pyridine dynamics in both states including the kinetics of the exchange process between these adsorption states.",

keywords = "adsorption, coordinatively unsaturated metal sites, metal–organic frameworks, molecular mobility, NMR spectroscopy, OXIDATION, DEFECTS, LEWIS-ACID, CATALYSTS, metal-organic frameworks, CR, FE",

author = "Khudozhitkov, {Alexander E.} and Toktarev, {Alexander V.} and Arzumanov, {Sergei S.} and Gabrienko, {Anton A.} and Kolokolov, {Daniil I.} and Stepanov, {Alexander G.}",

note = "{\textcopyright} 2019 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.",

year = "2019",

month = aug,

day = "14",

doi = "10.1002/chem.201901956",

language = "English",

volume = "25",

pages = "10808--10812",

journal = "Chemistry - A European Journal",

issn = "0947-6539",

publisher = "Wiley-VCH Verlag",

number = "46",

}

RIS

TY - JOUR

T1 - 2H Solid-State NMR Spectroscopy Reveals the Dynamics of a Pyridine Probe Interacting with Coordinatively Unsaturated Metal Sites of MIL-100(Al) Metal–Organic Frameworks

AU - Khudozhitkov, Alexander E.

AU - Toktarev, Alexander V.

AU - Arzumanov, Sergei S.

AU - Gabrienko, Anton A.

AU - Kolokolov, Daniil I.

AU - Stepanov, Alexander G.

PY - 2019/8/14

Y1 - 2019/8/14

N2 - Coordinatively unsaturated metal sites (CUS) play an important role in catalysis by metal-organic frameworks (MOF). Being an intrinsic part of the framework the CUS take the role of acidic sites active in industrially relevant processes such as condensation or oxidation reactions. The key step of such reactions represents the coordination of the reagents to CUS. In MOFs the mechanism of the reagent interaction with CUS is poorly understood. Herein, we characterize the interaction of a widely used acidity probe pyridine with CUS of MIL-100(Al) MOF by means of the 2H solid-state NMR spectroscopy. 2H NMR reveals that pyridine species, which are interacting with CUS and the ones which are coordinated to the Al−OH site, exhibit different motional behavior. 2H NMR line shape as well as T1, T2 relaxation analyses for [D5]pyridine adsorbed in MIL-100(Al) allowed us to perform a detailed characterization of pyridine dynamics in both states including the kinetics of the exchange process between these adsorption states.

AB - Coordinatively unsaturated metal sites (CUS) play an important role in catalysis by metal-organic frameworks (MOF). Being an intrinsic part of the framework the CUS take the role of acidic sites active in industrially relevant processes such as condensation or oxidation reactions. The key step of such reactions represents the coordination of the reagents to CUS. In MOFs the mechanism of the reagent interaction with CUS is poorly understood. Herein, we characterize the interaction of a widely used acidity probe pyridine with CUS of MIL-100(Al) MOF by means of the 2H solid-state NMR spectroscopy. 2H NMR reveals that pyridine species, which are interacting with CUS and the ones which are coordinated to the Al−OH site, exhibit different motional behavior. 2H NMR line shape as well as T1, T2 relaxation analyses for [D5]pyridine adsorbed in MIL-100(Al) allowed us to perform a detailed characterization of pyridine dynamics in both states including the kinetics of the exchange process between these adsorption states.

KW - adsorption

KW - coordinatively unsaturated metal sites

KW - metal–organic frameworks

KW - molecular mobility

KW - NMR spectroscopy

KW - OXIDATION

KW - DEFECTS

KW - LEWIS-ACID

KW - CATALYSTS

KW - metal-organic frameworks

KW - CR

KW - FE

UR - http://www.scopus.com/inward/record.url?scp=85069726186&partnerID=8YFLogxK

U2 - 10.1002/chem.201901956

DO - 10.1002/chem.201901956

M3 - Article

C2 - 31241210

AN - SCOPUS:85069726186

VL - 25

SP - 10808

EP - 10812

JO - Chemistry - A European Journal

JF - Chemistry - A European Journal

SN - 0947-6539

IS - 46

ER -

ID: 21046016

2H Solid-State NMR Spectroscopy Reveals the Dynamics of a Pyridine Probe Interacting with Coordinatively Unsaturated Metal Sites of MIL-100(Al) Metal–Organic Frameworks

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²H Solid-State NMR Spectroscopy Reveals the Dynamics of a Pyridine Probe Interacting with Coordinatively Unsaturated Metal Sites of MIL-100(Al) Metal–Organic Frameworks