Self-Assembled Aggregates of Rod-Coil Block Copolymers and Their Solubilization and Encapsulation of Fullerenes

Jenekhe, Samson A.; Chen, X. Linda

doi:10.1126/science.279.5358.1903

Cited by 868 publications

(580 citation statements)

References 43 publications

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“…In the past, a great deal of theoretical 1-10 and experimental efforts [11][12][13][14][15][16] have been made in understanding their characteristics in solutions with concentrations ranging from dilute to concentrated. One of the remarkable discoveries in the last century is the theory of simple electrolytes made by Debye and Hückel, 17 where electrostatic interactions get screened ͑colloquially referred to as the Debye screening͒.…”

Section: Introductionmentioning

confidence: 99%

Confinement free energy of flexible polyelectrolytes in spherical cavities

Kumar

Muthukumar

2008

The Journal of Chemical Physics

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A weakly charged flexible polyelectrolyte chain in a neutral spherical cavity is analyzed by using self-consistent field theory within an explicit solvent model. Assuming the radial symmetry for the system, it is found that the confinement of the chain leads to creation of a charge density wave along with the development of a potential difference across the center of cavity and the surface. We show that the solvent entropy plays an important role in the free energy of the confined system. For a given radius of the spherical cavity and fixed charge density along the backbone of the chain, solvent and small ion entropies dominate over all other contributions when chain lengths are small. However, with the increase in chain length, chain conformational entropy and polymer-solvent interaction energy also become important. Our calculations reveal that energy due to electrostatic interactions plays a minor role in the free energy. Furthermore, we show that the total free energy under spherical confinement is not extensive in the number of monomers. Results for the osmotic pressure and mean activity coefficient for monovalent salt are presented. We demonstrate that fluctuations at one-loop level lower the free energy and corrections to the osmotic pressure and mean activity coefficient of the salt are discussed. Finite size corrections are shown to widen the range of validity of the fluctuation analysis.

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Section: Introductionmentioning

confidence: 99%

Confinement free energy of flexible polyelectrolytes in spherical cavities

Kumar

Muthukumar

2008

The Journal of Chemical Physics

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“…They typically reveal unique self-assembly nanostructures and semiconducting characteristics [32][33][34][35][36]. Various kinds of copolymers were designed, synthesized and incorporated into BHJ with remarkable PCE improvements and/or PCE preservation.…”

Section: Copolymermentioning

confidence: 99%

Morphological Control Agent in Ternary Blend Bulk Heterojunction Solar Cells

et al. 2014

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Bulk heterojunction (BHJ) organic photovoltaic (OPV) promise low cost solar energy and have caused an explosive increase in investigations during the last decade. Control over the 3D morphology of BHJ blend films in various length scales is one of the pillars accounting for the significant advance of OPV performance recently. In this contribution, we focus on the strategy of incorporating an additive into BHJ blend films as a morphological control agent, i.e., ternary blend system. This strategy has shown to be effective in tailoring the morphology of BHJ through different inter-and intra-molecular interactions. We systematically review the morphological observations and associated mechanisms with respect to various kinds of additives, i.e., polymers, small molecules and inorganic nanoparticles. We organize the effects of morphological control (compatibilization, stabilization, etc.) and provide general guidelines for rational molecular design for additives toward high efficiency and high stability organic solar cells.

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“…Jenekhe et al found that rod−coil copolymers could selfassemble to form hollow nanospheres directly in their selective solvent (a solvent only dissolve one block of the copolymers). 21 Over the past 10 years, this convenient method has aroused many researcher's interest. 22−24 Recently, we developed a novel approach to prepare rod−coil complexes using the selective inclusion complexation between CD and copolymers.…”

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confidence: 99%

Cyclodextrin-Based Microcapsules as Bioreactors for ATP Biosynthesis

Jian-hu

Wang

et al. 2013

Biomacromolecules

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A biomimetic energy converter was fabricated via the assembly of CF 0 F 1 -ATPase on lipid-coated hollow nanocapsules composed of α-cyclodextrins/ chitosan-graf t-poly(ethylene glycol) methacrylate. Upon entrapped GOD into these capsules, the addition of glucose could trigger proton-motive force and then drive the rotation of ATPase to synthesize ATP.L iving organisms make a series of metabolisms every moment. An organism that wants to maintain activities needs a continuous supply of energy: adenosine triphosphate (ATP). As the energy currency, ATP induces large conformational changes in molecules such as myosin, kinesin, and chaperonin. With inspiration from biology, biological and biomimetic devices that supply ATP as energy, such as molecular motors and artificial cell bioreactors, have been developed. 1−4 However, in motility and functionality assays reported on these devices, the issue of ATP regulation is usually sidestepped by supplying ATP externally into the buffer solution. Complications can occur as high concentrations of ATP, and the devices stop operation when all the ATP runs out. For the long-term operation of more complex molecular devices, continual supply of the right amount of ATP is required.The enzyme primarily responsible for the production of ATP is the F 1 F 0 -type ATPase, which synthesizes ATP from adenosine diphosphate (ADP) and inorganic phosphate (Pi) by utilizing proton gradients. 5 Several groups have been working on the reconstitution of ATPase in liposomes as biomimetic systems to carry out ATP biosynthesis. 6−8 Although they have excellent assay characteristics, the future applicability of liposomes is intrinsically limited due to chemical and mechanical weaknesses. In order to get more stable and robust biomimetic membranes, polymersome and lipid bilayercoated microcapsules have been developed replacing traditional liposomes very recently. 9−12 For instance, Choi et al. demonstrated that synthesized amphiphilic polymersomes can replace liposomes for ATP synthesis. However, the synthesis needs strict control, and the assembled vesicles were not sufficiently stable. Li et al. introduced microcapsules fabricated by the layer-by-layer (LBL) assembly technique into the biomimetic system design and fabricated a series of biomimetic energy converters via the assembly of ATPase on lipid-coated hollow microcapsules. However, this strategy requires a procedure to remove the core in order to create a hollow interior and needs multiple steps to produce the wall of the microcapsules.In our previous study, we reported that polymeric hollow spheres with semipermeability could be obtained directly by self-assembly of rod−coil copolymers/cyclodextrin (CD) complexes in analogy to the cell membrane. 13−18 In the present work, we utilized this self-assembly approach to design a new type of biomimetic capsules for ATP synthesis. This capsule comprised a self-assembled hollow sphere as the inner support and its absorbed lipid as the out layer. Furthermore, glucose oxidases (GODs) were ent...

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Self-Assembled Aggregates of Rod-Coil Block Copolymers and Their Solubilization and Encapsulation of Fullerenes

Cited by 868 publications

References 43 publications

Confinement free energy of flexible polyelectrolytes in spherical cavities

Confinement free energy of flexible polyelectrolytes in spherical cavities

Morphological Control Agent in Ternary Blend Bulk Heterojunction Solar Cells

Cyclodextrin-Based Microcapsules as Bioreactors for ATP Biosynthesis

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