Kinetics and Thermodynamics of Constitutional Dynamic Coordination Systems Based on FeII, CoII, NiII, CuII, and ZnII

Neranon, Kitjanit; Ramström, Olof

doi:10.1002/ejic.201600331

Cited by 7 publications

(5 citation statements)

References 54 publications

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“…These ligands were then complexed with Zn(II) salts to afford the model complexes (Figure b). ESI-MS spectra showed that the metal-to-ligand molar ration in the model complexes is 1:2, which is typical for Zn(II) complexes with tridentate ligands. , …”

Section: Resultsmentioning

confidence: 87%

“…ESI-MS spectra showed that the metal-to-ligand molar ration in the model complexes is 1:2, which is typical for Zn(II) complexes with tridentate ligands. 47,48 To directly observe the dynamic ligand exchange behavior in solution, we mixed complexes [Zn(L 1 ) 2 ](OTf) 2 and [Zn(L 2 ) 2 ]-(OTf) 2 in acetonitrile, and the formation of [Zn(L 1 L 2 )](OTf) 2 was monitored by ESI-MS spectra over time at 25 °C (Figure 1c). 49−51 Figure S6 shows the time-dependent ESI-MS spectrometry of the mixture solution.…”

Section: Resultsmentioning

confidence: 99%

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Distinct Mechanical and Self-Healing Properties in Two Polydimethylsiloxane Coordination Polymers with Fine-Tuned Bond Strength

Wang

Lai

et al. 2018

Inorg. Chem.

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Coordination bonds are effective for constructing highly efficient self-healing materials as their strength is highly tunable. To design self-healing polymers with better performance, it is important to get a profound understanding of the structure-property relationships. However, this is challenging for self-healing polymers based on coordination bonds, because many parameters, such as bond energy, bond dynamics, and coordination number will have an essential effect on the mechanical and self-healing properties of the polymer. In this work, we synthesized two poly(dimethylsiloxane) (PDMS) polymers cross-linked by different Zn(II)-diiminopyridine coordination complexes (denoted as PDMS-NNN-Zn, PDMS-MeNNN-Zn respectively). The two cross-linking Zn(II)-diiminopyridine complexes are similar in coordination modes, but differ in coordination dynamics. As manifested by ITC, rheology, and tensile experiments, we confirm that the coordination bond in PDMS-MeNNN-Zn polymer films is weaker but more dynamic. Consequently, the PDMS-MeNNN-Zn polymer has poorer mechanical strength but higher stretchability and better self-healing properties. The inflicted cracks on PDMS-MeNNN-Zn polymer films can be completely healed after healing at room temperature for only 30 min with healing efficiencies higher than 90%. Such fast self-healing properties have never been achieved in self-healing polymers based on coordination bonds. Our results also demonstrate the important impact of the thermodynamic stability and kinetic lability of coordination complexes on the mechanical and self-healing properties of polymers. Such a comprehensive understanding is helpful for further design of novel synthetic polymers, which can achieve an optimal balance between the mechanical strength and self-healing performance.

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Section: Resultsmentioning

confidence: 87%

Section: Resultsmentioning

confidence: 99%

Distinct Mechanical and Self-Healing Properties in Two Polydimethylsiloxane Coordination Polymers with Fine-Tuned Bond Strength

Wang

Lai

et al. 2018

Inorg. Chem.

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“…The proportion of broken spheres is also very low, suggesting that the dendrimeric spheres are robust and difficult to break. This indicates that aggregation of the dendritic structures is dynamically reversible, resulting in the formation of spheres in aqueous solution prior to vacuum treatment during SEM analysis …”

Section: Resultsmentioning

confidence: 97%

Design, Synthesis and Self‐Assembly of Functional Amphiphilic Metallodendrimers

2020

Self Cite

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A new family of alkynylated, amphiphilic dendrimers consisting of amidoamine linkers connected to 5,5′‐functionalized 2,2′‐bipyridine cores has been developed and evaluated in the formation of metallodendrimers of different generations and in self‐assembly protocols. A convergent synthetic strategy was applied to provide dumbbell‐shaped amphiphilic dendrimers, where the 2,2′‐bipyridine cores could be coordinated to FeII centers to afford corresponding metallodendrimers. The ability of the metallic‐ and non‐metallic dendritic structures to self‐assemble into functional supramolecular aggregates were furthermore evaluated in aqueous solution. Spherical aggregates with sizes of a few hundred nanometers were generally produced, where controlled disassembly of the metallodendrimers through decomplexation could be achieved.

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“…At the +2 oxidation degree, these neighbors in the periodic table were previously reported to reversibly bind polyamine-based ligands thereby yielding dynamic combinatorial libraries of octahedral complexes. 29 While rare earth metals collectively display the same behavior, 21 nickel and cobalt afforded soluble systems along the full CO2 loading range in the presence of 12 eq. of DETA.…”

Section: Micro-and Macroscopic Perturbing Effects Of Metal Salts: Towmentioning

confidence: 99%

Simultaneous CO2 Capture and Metal Purification from Waste Streams

Leclaire

Septavaux²,

Tosi³

et al. 2018

Preprint

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The process of carbon capture, which is one of the most mature yet cost-intensive technology proposed to mitigate global warming has herein been explored as a potential strategy to generate dynamic ligands for metal separation and recovery. Spontaneous CO2 fixation by industrial amines such as diethylenetriamine affords dynamic arrays of interconverting species, from which tailored subsets can be selected yielding organometallic adducts of contrasted solubility. Quantitative compositional analyses of the phases produced with varying CO2 loadings allow to elucidate the underpining self-sorting scenario induced by each metal, and to identify the conditions affording optimal individual separation by precipitation. To illustrate the potentiality of this approach, which could bring substantial added value to the CO2 capture and utilization chain value, bimetallic separation was conducted directly from exhaust gas of an internal combustrion engine vehicle, and the three constituents of the alloys used to produce the cathodes of electric vehicles were separated and recovered by successive CO2-induced selective precipitations. This study provides a potential framework to integrated CO2 capture and utilization and paves the way toward the design of CO2-sourced sustainable processes.

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Kinetics and Thermodynamics of Constitutional Dynamic Coordination Systems Based on Fe^II, Co^II, Ni^II, Cu^II, and Zn^II

Cited by 7 publications

References 54 publications

Distinct Mechanical and Self-Healing Properties in Two Polydimethylsiloxane Coordination Polymers with Fine-Tuned Bond Strength

Distinct Mechanical and Self-Healing Properties in Two Polydimethylsiloxane Coordination Polymers with Fine-Tuned Bond Strength

Design, Synthesis and Self‐Assembly of Functional Amphiphilic Metallodendrimers

Simultaneous CO2 Capture and Metal Purification from Waste Streams

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