Connecting defects and amorphization in UiO-66 and MIL-140 metal-organic frameworks: a combined experimental and computational study

被引：103

作者：

Bennett, Thomas D. ^{[1
]}

Todorova, Tanya K. ^{[2
]}

Baxter, Emma F. ^{[1
]}

Reid, David G. ^{[3
]}

Gervais, Christel ^{[4
]}

Bueken, Bart ^{[5
]}

Van de Voorde, B. ^{[5
]}

De Vos, Dirk ^{[5
]}

Keen, David A. ^{[6
]}

Mellot-Draznieks, Caroline ^{[2
]}

机构：

[1] Univ Cambridge, Dept Mat Sci & Met, Cambridge CB3 0FS, England

[2] Univ Paris 06, Coll France, Lab Chim Proc Biol, CNRS UMR 8229, 11 Pl Marcelin Berthelot,11 Marcelin Berthelot, F-75231 Paris 05, France

[3] Univ Cambridge, Dept Chem, Lensfield Rd, Cambridge CB2 1EW, England

[4] Univ Paris 06, Sorbonne Univ, Coll France,UMR 7574, Chim Mat Condense Paris,CNRS, Paris, France

[5] Katholieke Univ Leuven, Leuven Chem&Tech, Ctr Surface Chem & Catalysis, Celestijnenlaan 200F,POB 2461, B-3001 Heverlee, Belgium

[6] Rutherford Appleton Lab, ISIS Facil, Didcot OX11 0QX, Oxon, England

来源：

PHYSICAL CHEMISTRY CHEMICAL PHYSICS | 2016年 / 18卷 / 03期

关键词：

STATE NMR-SPECTROSCOPY; X-RAY-DIFFRACTION; STABILITY; ZEOLITE;

D O I：

10.1039/c5cp06798g

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：

The mechanism and products of the structural collapse of the metal-organic frameworks (MOFs) UiO-66, MIL-140B and MIL-140C upon ball-milling are investigated through solid state C-13 NMR and pair distribution function (PDF) studies, finding amorphization to proceed by the breaking of a fraction of metal-ligand bonding in each case. The amorphous products contain inorganic-organic bonding motifs reminiscent of the crystalline phases. Whilst the inorganic Zr6O4(OH)(4) clusters of UiO-66 remain intact upon structural collapse, the ZrO backbone of the MIL-140 frameworks undergoes substantial distortion. Density functional theory calculations have been performed to investigate defective models of MIL-140B and show, through comparison of calculated and experimental C-13 NMR spectra, that amorphization and defects in the materials are linked.

引用

页码：2192 / 2201

页数：10

共 59 条

[1] Pair distribution function-derived mechanism of a single-crystal to disordered to single-crystal transformation in a hemilabile metal-organic framework [J].

Allan, Phoebe K. ;

Chapman, Karena W. ;

Chupas, Peter J. ;

Hriljac, Joseph A. ;

Renouf, Catherine L. ;

Lucas, Timothy C. A. ;

Morris, Russell E. .

CHEMICAL SCIENCE, 2012, 3 (08) :2559-2564

[2] Solid state NMR characterisation of encapsulated molecules in mesoporous silica [J].

Babonneau, F ;

Yeung, L ;

Steunou, N ;

Gervais, C ;

Ramila, A ;

Vallet-Regi, M .

JOURNAL OF SOL-GEL SCIENCE AND TECHNOLOGY, 2004, 31 (1-3) :219-223

[3] Superstructure of a Substituted Zeolitic Imidazolate Metal-Organic Framework Determined by Combining Proton Solid-State NMR Spectroscopy and DFT Calculations [J].

Baias, Maria ;

Lesage, Anne ;

Aguado, Sonia ;

Canivet, Jerome ;

Moizan-Basle, Virginie ;

Audebrand, Nathalie ;

Farrusseng, David ;

Emsley, Lyndon .

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2015, 54 (20) :5971-5976

[4] Coordination polymers, metal-organic frameworks and the need for terminology guidelines [J].

Batten, Stuart R. ;

Champness, Neil R. ;

Chen, Xiao-Ming ;

Garcia-Martinez, Javier ;

Kitagawa, Susumu ;

Ohrstrom, Lars ;

O'Keeffe, Michael ;

Suh, Myunghyun Paik ;

Reedijk, Jan .

CRYSTENGCOMM, 2012, 14 (09) :3001-3004

[5] Mechanical properties of zeolitic metal-organic frameworks: mechanically flexible topologies and stabilization against structural collapse [J].

Bennett, T. D. ;

Sotelo, J. ;

Tan, Jin-Chong ;

Moggach, S. A. .

CRYSTENGCOMM, 2015, 17 (02) :286-289

[6] Hybrid glasses from strong and fragile metal-organic framework liquids [J].

Bennett, Thomas D. ;

Tan, Jin-Chong ;

Yue, Yuanzheng ;

Baxter, Emma ;

Ducati, Caterina ;

Terrill, Nick J. ;

Yeung, Hamish H-M ;

Zhou, Zhongfu ;

Chen, Wenlin ;

Henke, Sebastian ;

Cheetham, Anthony K. ;

Greaves, G. Neville .

NATURE COMMUNICATIONS, 2015, 6

[7] Amorphous Metal-Organic Frameworks [J].

Bennett, Thomas D. ;

Cheetham, Anthony K. .

ACCOUNTS OF CHEMICAL RESEARCH, 2014, 47 (05) :1555-1562

[8] Structure and Properties of an Amorphous Metal-Organic Framework [J].

Bennett, Thomas D. ;

Goodwin, Andrew L. ;

Dove, Martin T. ;

Keen, David A. ;

Tucker, Matthew G. ;

Barney, Emma R. ;

Soper, Alan K. ;

Bithell, Erica G. ;

Tan, Jin-Chong ;

Cheetham, Anthony K. .

PHYSICAL REVIEW LETTERS, 2010, 104 (11)

[9] PROJECTOR AUGMENTED-WAVE METHOD [J].

BLOCHL, PE .

PHYSICAL REVIEW B, 1994, 50 (24) :17953-17979

[10] A REFINEMENT OF THE BENZOIC-ACID STRUCTURE AT ROOM-TEMPERATURE [J].

BRUNO, G ;

RANDACCIO, L .

ACTA CRYSTALLOGRAPHICA SECTION B-STRUCTURAL SCIENCE, 1980, 36 (JUL) :1711-1712

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