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Author Gonzalez-Nelson, A.; Mula, S.; Simenas, M.; Balciunas, S.; Altenhof, A.R.; Vojvodin, C.S.; Canossa, S.; Banys, J.; Schurko, R.W.; Coudert, F.-X.; van der Veen, M.A.
Title Emergence of coupled rotor dynamics in metal-organic frameworks via tuned steric interactions Type A1 Journal article
Year (down) 2021 Publication Journal Of The American Chemical Society Abbreviated Journal J Am Chem Soc
Volume 143 Issue 31 Pages 12053-12062
Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
Abstract The organic components in metal-organic frameworks (MOFs) are unique: they are embedded in a crystalline lattice, yet, as they are separated from each other by tunable free space, a large variety of dynamic behavior can emerge. These rotational dynamics of the organic linkers are especially important due to their influence over properties such as gas adsorption and kinetics of guest release. To fully exploit linker rotation, such as in the form of molecular machines, it is necessary to engineer correlated linker dynamics to achieve their cooperative functional motion. Here, we show that for MIL-53, a topology with closely spaced rotors, the phenylene functionalization allows researchers to tune the rotors' steric environment, shifting linker rotation from completely static to rapid motions at frequencies above 100 MHz. For steric interactions that start to inhibit independent rotor motion, we identify for the first time the emergence of coupled rotation modes in linker dynamics. These findings pave the way for function-specific engineering of gear-like cooperative motion in MOFs.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000684581100022 Publication Date 2021-07-29
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 0002-7863 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 13.858 Times cited Open Access OpenAccess
Notes Approved Most recent IF: 13.858
Call Number UA @ admin @ c:irua:180504 Serial 6867
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Author Canossa, S.; Gonzalez-Nelson, A.; Shupletsov, L.; Carmen Martin, M.; Van der Veen, M.A.
Title Overcoming Crystallinity Limitations of Aluminium Metal-Organic Frameworks by Oxalic Acid Modulated Synthesis Type A1 Journal article
Year (down) 2020 Publication Chemistry-A European Journal Abbreviated Journal Chem-Eur J
Volume 26 Issue 16 Pages 3564-3570
Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
Abstract A modulated synthesis approach based on the chelating properties of oxalic acid (H2C2O4) is presented as a robust and versatile method to achieve highly crystalline Al‐based metal‐organic frameworks. A comparative study on this method and the already established modulation by hydrofluoric acid was conducted using MIL‐53 as test system. The superior performance of oxalic acid modulation in terms of crystallinity and absence of undesired impurities is explained by assessing the coordination modes of the two modulators and the structural features of the product. The validity of our approach was confirmed for a diverse set of Al‐MOFs, namely X‐MIL‐53 (X=OH, CH3O, Br, NO2), CAU‐10, MIL‐69, and Al(OH)ndc (ndc=1,4‐naphtalenedicarboxylate), highlighting the potential benefits of extending the use of this modulator to other coordination materials.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000517650300001 Publication Date 2020-03-18
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 0947-6539 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 4.3 Times cited Open Access OpenAccess
Notes The Elettra Synchrotron facility (CNR Trieste, Basovizza, Italy) is acknowledged for granting beamtime at the single-crystal diffraction beamline XRD1 (Proposal ID 20185483) and the beamline staff is gratefully thanked for the precious assistance. This work was funded by the European Research Council (grant number 759 212) within the Horizon 2020 Framework Programme (H2020-EU.1.1). The work by A.G.-N. forms part of the research programme of DPI, NEWPOL project 731.015.506. Approved Most recent IF: 4.3; 2020 IF: 5.317
Call Number EMAT @ emat @c:irua:167706 Serial 6388
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