Supramolecular Construction of an Aldehyde–Cyclobutane via the Solid State: Combining Reversible Imine Formation and Metal–Organic Self-Assembly

2017 ◽  
Vol 139 (25) ◽  
pp. 8452-8454 ◽  
Author(s):  
Shalisa M. Oburn ◽  
Dale C. Swenson ◽  
S. V. Santhana Mariappan ◽  
Leonard R. MacGillivray
Keyword(s):  
Solid State ◽  
Self Assembly ◽  
Metal Organic

scholarly journals Mechanochemical and solvent-free assembly of zirconium-based metal–organic frameworks

2016 ◽  
Vol 52 (10) ◽  
pp. 2133-2136 ◽  
Author(s):  
Krunoslav Užarević ◽  
Timothy C. Wang ◽  
Su-Young Moon ◽  
Athena M. Fidelli ◽  
Joseph T. Hupp ◽  
...  
Keyword(s):  
Solid State ◽  
High Temperatures ◽  
Self Assembly ◽  
Metal Organic Frameworks ◽  
Accelerated Aging ◽  
Solvent Free ◽  
Catalytically Active ◽  
Metal Organic ◽  
Strong Acids ◽  
Zirconium Metal

Mechanochemistry and accelerated aging are new routes to zirconium metal–organic frameworks, yielding UiO-66 and catalytically active UiO-66-NH2 accessible on the gram scale through mild solid-state self-assembly, without strong acids, high temperatures or excess reactants.

scholarly journals Redox-promoted associative assembly of metal–organic materials

2016 ◽  
Vol 7 (1) ◽  
pp. 707-712 ◽  
Author(s):  
Martin Glavinović ◽  
Feng Qi ◽  
Athanassios D. Katsenis ◽  
Tomislav Friščić ◽  
Jean-Philip Lumb
Keyword(s):  
Solid State ◽  
Self Assembly ◽  
Organic Materials ◽  
Metal Oxidation ◽  
Metal Organic ◽  
One Step

We develop an associative synthesis of metal–organic materials that combines solid-state metal oxidation and coordination-driven self-assembly into a one-step, waste-free transformation.

Kinetic Control of Interpenetration in Fe-Biphenyl-4,4′-dicarboxylate MOFs by Coordination and Oxidation Modulation

2018 ◽  
Author(s):  
Dominic Bara ◽  
Claire Wilson ◽  
Max Mörtel ◽  
Marat M. Khusniyarov ◽  
ben slater ◽  
...  
Keyword(s):  
Self Assembly ◽  
Surface Areas ◽  
Metal Precursors ◽  
Additional Coordination ◽  
Fine Control ◽  
Multiple Alternative ◽  
Metal Organic ◽  
Dft Simulations ◽  
High Valent ◽  
And Control

Phase control in the self-assembly of metal-organic frameworks (MOFs) – materials wherein organic ligands connect metal ions or clusters into network solids with potential porosity – is often a case of trial and error. Judicious control over a number of synthetic variables is required to select for the desired topology and control features such as interpenetration and defectivity, which have significant impact on physical properties and application. Herein, we present a comprehensive investigation of self-assembly in the Fe-biphenyl-4,4'-dicarboxylate system, demonstrating that coordination modulation, the addition of competing ligands into solvothermal syntheses, can reliably tune between the kinetic product, non-interpenetrated MIL-88D(Fe), and the thermodynamic product, two-fold interpenetrated MIL-126(Fe). DFT simulations reveal that correlated disorder of the terminal anions on the metal clusters in the interpentrated phase results in H-bonding between adjacent nets and is the thermodynamic driving force for its formation. Coordination modulation slows self-assembly and therefore selects the thermodynamic product MIL-126(Fe), while offering fine control over defectivity, inducing mesoporosity, but electron microscopy shows the MIL-88D(Fe) phase persists in many samples despite not being evident in diffraction experiments, suggesting its presence accounts for the lower than predicted surface areas reported for samples to date. Interpenetration control is also demonstrated by utilizing the 2,2'-bipyridine-5,5'-dicarboxylate linker; DFT simulations show that it is energetically prohibitive for it to adopt the twisted conformation required to form the interpenetrated phase, and are confirmed by experimental data, although multiple alternative phases are identified due to additional coordination of the Fe cations to the N-donors of the ligand. Finally, we introduce oxidation modulation – the concept of using metal precursors in a different oxidation state to that found in the final MOF – as a further protocol to kinetically control self-assembly. Combining coordination and oxidation modulation allows the synthesis of pristine MIL-126(Fe) with BET surface areas close to the predicted maximum capacity for the first time, suggesting that combining the two may be a powerful methodology for the controlled self-assembly of high-valent MOFs.<br><br>

scholarly journals A Cavity‐Tailored Metal‐Organic Cage Entraps Gases Selectively in Solution and the Amorphous Solid State

2021 ◽  
Author(s):  
Jun-Long Zhu ◽  
Dawei Zhang ◽  
Tanya Ronson ◽  
Wenjing Wang ◽  
Lin Xu ◽  
...  
Keyword(s):  
Solid State ◽  
Amorphous Solid ◽  
Metal Organic

scholarly journals HKUST-1@IL-Li Solid-state Electrolyte with 3D Ionic Channels and Enhanced Fast Li+ Transport for Lithium Metal Batteries at High Temperature

Nanomaterials ◽  
2021 ◽  
Vol 11 (3) ◽  
pp. 736
Author(s):  
Man Li ◽  
Tao Chen ◽  
Seunghyun Song ◽  
Yang Li ◽  
Joonho Bae
Keyword(s):  
High Temperature ◽  
Solid State ◽  
Solid Electrolyte ◽  
Metal Organic Framework ◽  
Ionic Channels ◽  
Transference Numbers ◽  
Lithium Metal ◽  
Lithium Metal Batteries ◽  
Metal Organic ◽  
Organic Framework

The challenge of safety problems in lithium batteries caused by conventional electrolytes at high temperatures is addressed in this study. A novel solid electrolyte (HKUST-1@IL-Li) was fabricated by immobilizing ionic liquid ([EMIM][TFSI]) in the nanopores of a HKUST-1 metal–organic framework. 3D angstrom-level ionic channels of the metal–organic framework (MOF) host were used to restrict electrolyte anions and acted as “highways” for fast Li+ transport. In addition, lower interfacial resistance between HKUST-1@IL-Li and electrodes was achieved by a wetted contact through open tunnels at the atomic scale. Excellent high thermal stability up to 300 °C and electrochemical properties are observed, including ionic conductivities and Li+ transference numbers of 0.68 × 10-4 S·cm-1 and 0.46, respectively, at 25 °C, and 6.85 × 10-4 S·cm-1 and 0.68, respectively, at 100 °C. A stable Li metal plating/stripping process was observed at 100 °C, suggesting an effectively suppressed growth of Li dendrites. The as-fabricated LiFePO4/HKUST-1@IL-Li/Li solid-state battery exhibits remarkable performance at high temperature with an initial discharge capacity of 144 mAh g-1 at 0.5 C and a high capacity retention of 92% after 100 cycles. Thus, the solid electrolyte in this study demonstrates promising applicability in lithium metal batteries with high performance under extreme thermal environmental conditions.

Porous Colloidal Hydrogels Formed by Coordination‐Driven Self‐Assembly of Charged Metal‐Organic Polyhedra

2021 ◽  
Author(s):  
Zaoming Wang ◽  
Gavin A. Craig ◽  
Alexandre Legrand ◽  
Frederik Haase ◽  
Saori Minami ◽  
...  
Keyword(s):  
Self Assembly ◽  
Metal Organic

Azoimidazole gold(III) complexes: Synthesis, structural characterization and self-assembly in the solid state

2021 ◽  
Vol 522 ◽  
pp. 120373
Author(s):  
Alexander G. Tskhovrebov ◽  
Alexander S. Novikov ◽  
Boris S. Tupertsev ◽  
Alexey A. Nazarov ◽  
Anastasia A. Antonets ◽  
...  
Keyword(s):  
Solid State ◽  
Structural Characterization ◽  
Self Assembly
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