Polymer Structure Dependent Hierarchy in PolyMOC Gels

Zhukhovitskiy, Aleksandr V.; Zhao, Julia Xiaojun; Zhong, Mingjiang; Keeler, Eric G.; Alt, Eric A.; Teichen, Paul E.; Griffin, Robert G.; Hore, Michael J. A.; Willard, Adam P.; Johnson, Jeremiah A.

doi:10.1021/acs.macromol.6b01607

Cited by 53 publications

(50 citation statements)

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“…[27][28][29][30][31][32][33][34][35][37][38][39][40] Te ntative compositions for polymeric gelators peciesa re proposed in some cases;f or other cases we have proposed indicative compositions that are, however,h ypothetical. [27][28][29][30][31][32][33][34][35][37][38][39][40] Te ntative compositions for polymeric gelators peciesa re proposed in some cases;f or other cases we have proposed indicative compositions that are, however,h ypothetical.…”

Section: Polymeric Palladium(ii) Complexes As Gelatorsmentioning

confidence: 99%

“…It was noted that the catalytic turnover of the gel phase was greater than that of the xerogel. [37] Interestingly,c omplexation of Pd(NO 3 ) 2 with isomeric ligand L26 resulted in the proposed [Pd 2n (L26) 4n ](NO 3 ) 4n (26)g elator with a[ Pd 2 L 4 ]-type binuclear complex as the junction (Figure 26). Palladium(II)-enriched organic gels were also used in the oxidation of benzyl alcoholt obenzaldehyde.…”

Section: Polymeric Palladium(ii) Complexes With Bi-or Polydentate Ligmentioning

confidence: 99%

“…Gelation promoted by the in situ formation of coordinationpolymer-like speciesi sa lso known. [27][28][29][30][31][32][33][34][35][37][38][39][40] Te ntative compositions for polymeric gelators peciesa re proposed in some cases;f or other cases we have proposed indicative compositions that are, however,h ypothetical. Av ariety of palladium(II)based gelators and their properties is briefly discussed below.…”

Section: Polymeric Palladium(ii) Complexes As Gelatorsmentioning

confidence: 99%

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Discrete and Polymeric Self‐Assembled Palladium(II) Complexes as Supramolecular Gelators

Ganta

Chand

2018

Chemistry An Asian Journal

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Supramolecular gels prepared from low-molecular-weight gelators have been extensively explored. However, the exploitation of discrete or polymeric metal complexes as gelators is a relatively recent trend. The synthesis of self-assembled coordination complexes from palladium(II) and selected ligands is well established, but the potential of these complexes as gelators is a less explored treasure. Herein we focus on the gelation abilities of some self-assembled palladium(II) complexes and the resulting unique properties. First, discrete complexes with PdL, PdL , Pd L, Pd L , Pd L , and Pd L compositions are discussed. Second, gelation behavior promoted by coordination-polymer-like gelators formed in situ is explored. These gel samples have been employed in catalysis and the uptake of organic and dye molecules from the solution and gas phases. It is concluded that untapped unique properties can be realized by further exploration of designer palladium(II) complexes.

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Section: Polymeric Palladium(ii) Complexes As Gelatorsmentioning

confidence: 99%

Section: Polymeric Palladium(ii) Complexes With Bi-or Polydentate Ligmentioning

confidence: 99%

Section: Polymeric Palladium(ii) Complexes As Gelatorsmentioning

confidence: 99%

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Discrete and Polymeric Self‐Assembled Palladium(II) Complexes as Supramolecular Gelators

Ganta

Chand

2018

Chemistry An Asian Journal

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“…The latter two peaks agree well with the form factors of a 3.5 nm nanoparticle; they are assigned to the MOCs embedded within the network. [37] The data suggests that as n increases, the fidelity of MOC formation also increases. The low q SAXS peak for each polyMOC is assigned as the average distance between adjacent MOCs linked by polymer chains (Figure 3, inset).…”

mentioning

confidence: 98%

“…[23][24][25][26][27][28][29] Inspired by this structural versatility and potential applications such as mechanical enhancement, catalysis, encapsulation, sensing, etc., much effort has been recently devoted to installing MOCs into polymer networks to provide 'polyMOC' hybrid materials with tunable viscoelasticity and functionality. [30][31][32][33][34][35][36][37] One [30,[38][39][40][41][42] ; however, there is still a great need to understand how polyMOC microstructure translates to bulk material properties such as modulus and relaxation dynamics. To accomplish this goal, robust, modular polyMOC synthesis strategies that enable access to a wide range of structures and properties are needed.…”

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confidence: 99%

Star PolyMOCs with Diverse Structures, Dynamics, and Functions by Three‐Component Assembly

Wang

Keeler

et al. 2016

Angewandte Chemie

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We report star polymer metal-organic cage (polyMOC) materials whose structures, mechanical properties, functionalities, and dynamics can all be precisely tailored through a simple threecomponent assembly strategy. The star polyMOC network is composed of tetra-arm star polymers functionalized with ligands on the chain ends, small molecule ligands, and palladium ions; polyMOCs are formed via metal-ligand coordination and thermal annealing. The ratio of small molecule ligands to polymer-bound ligands determines the connectivity of the MOC junctions and the network structure. The use of large M 12 L 24 MOCs enables great flexibility in tuning this ratio, which provides access to a rich spectrum of material properties including tunable moduli and relaxation dynamics. HHS Public Access Author Manuscript Author ManuscriptAuthor Manuscript Author ManuscriptA three-component assembly strategy is reported that enables the creation of a versatile class of polymer metal-organic cage (polyMOC) networks with tailored microstructures, mechanical properties, functionalities, and network dynamics. KeywordsMetal-organic cage; Metal-organic polyhedra; Polymer network; Metallosupramolecular assembly; Gel; PolyMOC Polymer networks are versatile materials with a wide range of structures and properties suitable for industrial and academic applications. [1][2][3] In a typical network, macromolecules of choice are connected to branched junctions of a particular type; the nature of these components determines the material's properties such as stiffness, toughness, responsiveness, etc. [2] Several strategies have been developed to tune polymer network structure in order to realize desirable properties. For example, interpenetrating networks, [4][5] nanocomposites, [6] and reversible and/or dynamic covalent bonds [7] are employed to yield materials with self-healing, stimuli-responsive, and other valuable behaviors. [7][8] In all of these cases, control over network structure and dynamics is critical. In this communication, we describe a versatile and simple strategy for controlling structure, function, and dynamics in a relatively new class of polymer networks that is based on the use of large metal-organic cages/polyhedra (MOCs).MOCs are discrete 3D structures assembled from x metal ions and y organic ligands via coordination bonds. [9][10][11][12][13][14][15][16][17][18][19][20][21][22] By rational design of the ligands and proper choice of the metal ions, MOCs of different M x L y stoichiometries, sizes, and geometries can be synthesized. [23][24][25][26][27][28][29] Inspired by this structural versatility and potential applications such as mechanical enhancement, catalysis, encapsulation, sensing, etc., much effort has been recently devoted to installing MOCs into polymer networks to provide 'polyMOC' hybrid materials with tunable viscoelasticity and functionality. [30][31][32][33][34][35][36][37] One [30,[38][39][40][41][42] ; however, there is still a great need to understand how polyMOC microstructure translates to bulk ...

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Metallogels: Availability, Applicability, and Advanceability

et al. 2019

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amount of cross-linked solid. According to the nature of solvents, gels are categorized into hydrogel and organogel to indicate whether the solvent is water or organic solvent(s), respectively. As to the gelation driving forces, gels can be classified into physical gels in which intermolecular interactions are responsible for gel formation, and chemical gels in which the gel skeleton is cross-linked by covalent bonds.Incorporation of metal components (metal ions, metal-organic molecules, and metal nanoparticles) is an effective way to locally establish extra interactions among the building blocks and consequently trigger gel formation, [2][3][4] weaken [5] or enhance [6] gel strength, and modify gel morphology. [7,8] Moreover, addition of metal components is a straightforward way to integrate the specific properties of metals with the properties of organic matrix, therefore to tune properties like conductivity, [9] color, [10,11] rheological behavior, [12] adsorption, [13] emission, [14] photophysical properties, [15] magnetism, [16,17] antibacterial activities, [18,19] catalytic activities, [20][21][22][23] redox activities, [24,25] and selfhealing properties. [26][27][28] Therefore, a broad response range to physical and chemical stimuli can be achieved. For instance, the incorporation of multivalence ions such as Fe 2+ /Fe 3+ , [25,29] Co 2+ / Co 3+ , [30] Cu + /Cu 2+ , [31] results in redox reactive hydrogels; the incorporation of magnetic nanoparticles like Fe 3 O 4[17] causes the gel to respond to external magnetic fields. In addition to the abovementioned intrinsically functional superiorities, metallogels can also serve as ideal templates to generate new materials, [13,22,23,32,33] such as 3D networks, [34] porous structures, [35] chiral materials, [36][37][38] quantum dots, [39] and nanorods. [40] Following the rapid advancement of exploration on the knowledge acquisition toward the major roles that metallogels are playing in catalysis, sensing, biomedicine, electronics, and optical devices, the focus of research has been transferred to the design principles of metallogels in the last decade. Owing to the advancements in the instrumental characterizations and theoretical calculations, [41] a number of pioneering efforts on metallogel design have been made and several innovative reviews have summarized these inspiring contributions. [32,[42][43][44] Despite their extensively acknowledged application advantages in many fields, the discovery of new metallogels with expected functionalities is still highly dependent on experimental screening and serendipity. The challenge stems from the susceptible balance among those complicated intermolecular interactions and the elaborate structure requirements of metallogels.Another research niche that needs to be clarified before discussing recent development of metallogels is: how to sort Introducing metal components into gel matrices provides an effective strategy to develop soft materials with advantageous properties such as: optical activity, conductivity, magn...

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Polymer Structure Dependent Hierarchy in PolyMOC Gels

Cited by 53 publications

References 53 publications

Discrete and Polymeric Self‐Assembled Palladium(II) Complexes as Supramolecular Gelators

Discrete and Polymeric Self‐Assembled Palladium(II) Complexes as Supramolecular Gelators

Star PolyMOCs with Diverse Structures, Dynamics, and Functions by Three‐Component Assembly

Metallogels: Availability, Applicability, and Advanceability

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