Unraveling the reversible formation of defective Ce3+sites in the UiO-66(Ce) material: a multi-technique study

被引：10

作者：

Rojas-Buzo, S. ^{[1
]}

Salusso, D. ^{[1
]}

Bonino, F. ^{[1
]}

Paganini, M. C. ^{[1
]}

Bordiga, S. ^{[1
]}

机构：

[1] Univ Torino, NIS & INSTM Reference Ctr, Dept Chem, I-10125 Turin, Italy

来源：

MATERIALS TODAY CHEMISTRY | 2023年 / 27卷

关键词：

Metal -organic framework; Ce-MOF; Ce reduction; Laboratory techniques; NEXAFS; METAL-ORGANIC FRAMEWORKS; OXYGEN VACANCY; CE3+; CEO2; STABILITY; CHEMISTRY; SURFACE; PERFORMANCE; ADSORPTION; INTERFACE;

D O I：

10.1016/j.mtchem.2022.101337

中图分类号：

O6 [化学];

学科分类号：

0703 ;

摘要：

Ce3+ presence and formation in Ce-based UiO-66 Metal-Organic Framework (MOF) still presents a debated evaluation between the employed characterization techniques. In this work, we have prepared a defective UiO-66(Ce) and investigated the nature of Ce3+ sites on the CeOx clusters. Laboratory tech-niques (EPR, XPS, UV-Vis and FTIR spectroscopy) were compared with operando Ce M5-edge NEXAFS to study Ce3+ accessibility. All the employed techniques presented different degrees of accessibility or reliability (e.g., sample damage or not sufficient sensitivity). Among the obtained results, EPR, UV-Vis and NEXAFS spectroscopies unraveled Ce4+/Ce3+ conversion during the sample dehydration. The MOF structure was not damaged by neither water loss nor the beam, directly relating Ce oxidation state to the water content, opening a new route to both synthesis of stable and active MOFs and non-invasive characterization strategies. Finally, laboratory measurements considerations were exploited for studying Ce3+ formation in Zr-doped UiO-66(Ce) samples. (c) 2022 Elsevier Ltd. All rights reserved.

引用

页数：7

共 56 条

[1] Disclosing the Properties of a New Ce(III)-Based MOF:Ce2(NDC)3(DMF)2 [J].

Atzori, Cesare ;

Lomachenko, Kirill A. ;

Oien-Odegaard, Sigurd ;

Lamberti, Carlo ;

Stock, Norbert ;

Barolo, Claudia ;

Bonino, Francesca .

CRYSTAL GROWTH & DESIGN, 2019, 19 (02) :787-796

[2] IR study of polycrystalline ceria properties in oxidised and reduced states [J].

Binet, C ;

Daturi, M ;

Lavalley, JC .

CATALYSIS TODAY, 1999, 50 (02) :207-225

[3] Coordinatively Unsaturated Hf-MOF-808 Prepared via Hydrothermal Synthesis as a Bifunctional Catalyst for the Tandem N-Alkylation of Amines with Benzyl Alcohol [J].

Bohigues, Benjamin ;

Rojas-Buzo, Sergio ;

Moliner, Manuel ;

Corma, Avelino .

ACS SUSTAINABLE CHEMISTRY & ENGINEERING, 2021, 9 (47) :15793-15806

[4] Understanding Solid-Gas Reaction Mechanisms by Operando Soft X-Ray Absorption Spectroscopy at Ambient Pressure [J].

Braglia, Luca ;

Fracchia, Martina ;

Ghigna, Paolo ;

Minguzzi, Alessandro ;

Meroni, Daniela ;

Edla, Raju ;

Vandichel, Matthias ;

Ahlberg, Elisabet ;

Cerrato, Giuseppina ;

Torelli, Piero .

JOURNAL OF PHYSICAL CHEMISTRY C, 2020, 124 (26) :14202-14212

[5] A reaction cell for ambient pressure soft x-ray absorption spectroscopy [J].

Castan-Guerrero, C. ;

Krizmancic, D. ;

Bonanni, V. ;

Edla, R. ;

Deluisa, A. ;

Salvador, F. ;

Rossi, G. ;

Panaccione, G. ;

Torelli, P. .

REVIEW OF SCIENTIFIC INSTRUMENTS, 2018, 89 (05)

[6] A new zirconium inorganic building brick forming metal organic frameworks with exceptional stability [J].

Cavka, Jasmina Hafizovic ;

Jakobsen, Soren ;

Olsbye, Unni ;

Guillou, Nathalie ;

Lamberti, Carlo ;

Bordiga, Silvia ;

Lillerud, Karl Petter .

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2008, 130 (42) :13850-13851

[7] Origin of Visible Light Photoactivity of the CeO2/ZnO Heterojunction [J].

Cerrato, Erik ;

Gionco, Chiara ;

Paganini, Maria Cristina ;

Giamello, Elio ;

Albanese, Elisa ;

Pacchioni, Gianfranco .

ACS APPLIED ENERGY MATERIALS, 2018, 1 (08) :4247-4260

[8] Ce3+ and oxygen vacancy mediated tuning of structural and optical properties of CeO2 nanoparticles [J].

Choudhury, Biswajit ;

Choudhury, Amarjyoti .

MATERIALS CHEMISTRY AND PHYSICS, 2012, 131 (03) :666-671

[9] Design of Hierarchical Architectures in Metal-Oganic Frameworks for Catalysis and Adsorption [J].

Cirujano, Francisco G. ;

Martin, Nuria ;

Wee, Lik H. .

CHEMISTRY OF MATERIALS, 2020, 32 (24) :10268-10295

[10] Correlated defect nanoregions in a metal-organic framework [J].

Cliffe, Matthew J. ;

Wan, Wei ;

Zou, Xiaodong ;

Chater, Philip A. ;

Kleppe, Annette K. ;

Tucker, Matthew G. ;

Wilhelm, Heribert ;

Funnell, Nicholas P. ;

Coudert, Francois-Xavier ;

Goodwin, Andrew L. .

NATURE COMMUNICATIONS, 2014, 5

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