Defect Engineering: Tuning the Porosity and Composition of the Metal-Organic Framework UiO-66 via Modulated Synthesis

被引：1090

作者：

Shearer, Greig C. ^{[1
]}

Chavan, Sachin ^{[1
]}

Bordiga, Silvia ^{[1
,2
]}

Svelle, Stian ^{[1
]}

Olsbye, Unni ^{[1
]}

Lillerud, Karl Petter ^{[1
]}

机构：

[1] Univ Oslo, Dept Chem, POB 1033, N-0315 Oslo, Norway

[2] Univ Torino, Dept Chem, NIS & INSTM Reference Ctr, Via G Quarello 15, I-10135 Turin, Italy

来源：

CHEMISTRY OF MATERIALS | 2016年 / 28卷 / 11期

关键词：

MICROWAVE-ASSISTED SYNTHESIS; STRUCTURAL STABILITY; HYDROGEN STORAGE; WATER-ADSORPTION; FACILE SYNTHESIS; CO2; ADSORPTION; SURFACE-AREA; ZR; ACID; VAPOR;

D O I：

10.1021/acs.chemmater.6b00602

中图分类号：

O64 [物理化学（理论化学）、化学物理学];

学科分类号：

070304 ; 081704 ;

摘要：

Presented in this paper is a deep investigation into the defect chemistry of UiO-66 when synthesized in the presence of monocarboxylic acid modulators under the most commonly employed conditions. We unequivocally demonstrate that missing cluster defects are the predominant defect and that their concentration (and thus the porosity and composition of the material) can be tuned to a remarkable extent by altering the concentration and/or acidity of the modulator. Finally, we attempt to rationalize these observations by speculating on the underlying solution chemistry.

引用

页码：3749 / 3761

页数：13

共 91 条

[1] Modulated UiO-66-Based Mixed-Matrix Membranes for CO2 Separation [J].

Anjum, M. Waqas ;

Vermoortele, Frederik ;

Khan, Asim Laeeq ;

Bueken, Bart ;

De Vos, Dirk E. ;

Vankelecom, Ivo F. J. .

ACS APPLIED MATERIALS & INTERFACES, 2015, 7 (45) :25193-25201

[2] A General Strategy for the Synthesis of Functionalised UiO-66 Frameworks: Characterisation, Stability and CO2 Adsorption Properties [J].

Biswas, Shyam ;

Van der Voort, Pascal .

EUROPEAN JOURNAL OF INORGANIC CHEMISTRY, 2013, (12) :2154-2160

[3] Enhanced selectivity of CO2 over CH4 in sulphonate-, carboxylate- and iodo-functionalized UiO-66 frameworks [J].

Biswas, Shyam ;

Zhang, Jian ;

Li, Zhibao ;

Liu, Ying-Ya ;

Grzywa, Maciej ;

Sun, Lixian ;

Volkmer, Dirk ;

Van der Voort, Pascal .

DALTON TRANSACTIONS, 2013, 42 (13) :4730-4737

[4] Tailoring of network dimensionality and porosity adjustment in Zr- and Hf-based MOFs [J].

Bon, Volodymyr ;

Senkovska, Irena ;

Weiss, Manfred S. ;

Kaskel, Stefan .

CRYSTENGCOMM, 2013, 15 (45) :9572-9577

[5] Zr- and Hf-Based Metal-Organic Frameworks: Tracking Down the Polymorphism [J].

Bon, Volodymyr ;

Senkovska, Irena ;

Baburin, Igor A. ;

Kaskel, Stefan .

CRYSTAL GROWTH & DESIGN, 2013, 13 (03) :1231-1237

[6] Zr(IV) and Hf(IV) based metal-organic frameworks with reo-topology [J].

Bon, Volodymyr ;

Senkovskyy, Volodymyr ;

Senkovska, Irena ;

Kaskel, Stefan .

CHEMICAL COMMUNICATIONS, 2012, 48 (67) :8407-8409

[7]

Bosch M., 2014, Advances in Chemistry, V2014, P8, DOI DOI 10.1155/2014/182327

[8] Free Energy of Ligand Removal in the Metal-Organic Framework UiO-66 [J].

Bristow, Jessica K. ;

Svane, Katrine L. ;

Tiana, Davide ;

Skelton, Jonathan M. ;

Gale, Julian D. ;

Walsh, Aron .

JOURNAL OF PHYSICAL CHEMISTRY C, 2016, 120 (17) :9276-9281

[9] A zirconium squarate metal-organic framework with modulator-dependent molecular sieving properties [J].

Bueken, Bart ;

Reinsch, Helge ;

Reimer, Nele ;

Stassen, Ivo ;

Vermoortele, Frederik ;

Ameloot, Rob ;

Stock, Norbert ;

Kirschhock, Christine E. A. ;

De Vos, Dirk .

CHEMICAL COMMUNICATIONS, 2014, 50 (70) :10055-10058

[10] Origin of highly active metal-organic framework catalysts: defects? Defects! [J].

Canivet, J. ;

Vandichel, M. ;

Farrusseng, D. .

DALTON TRANSACTIONS, 2016, 45 (10) :4090-4099

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