Nucleation-Controlled Polymerization of Nanoparticles into Supramolecular Structures

Wang, Jing; Xia, Hongwei; Zhang, Yanfeng; Lu, Hua; Kamat, Ranjan K.; Dobrynin, Andrey V.; Cheng, Jianjun; Lin, Yao

doi:10.1021/ja402757e

Cited by 50 publications

(48 citation statements)

References 36 publications

(13 reference statements)

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“…cooperative self-assembly). Cooperative self-assembly processes have been reported in numerous systems including proteins 49 , peptide-based molecules 50 , small molecules 49,51 , and nanoparticles 52 and are characterized by a bimodal distribution of small oligomers and larger aggregates. In our system, the small micelles may fuse to form metastable intermediates, which then rapidly fuse with additional smaller micelles to produce a bimodal size distribution.…”

Section: Discussionmentioning

confidence: 99%

Size evolution of highly amphiphilic macromolecular solution assemblies via a distinct bimodal pathway

et al. 2014

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The solution self-assembly of macromolecular amphiphiles offers an efficient, bottom-up strategy for producing well--defined nanocarriers, with applications ranging from drug delivery to nanoreactors. Typically, the generation of uniform nanocarrier architecturesis controlled by processing methods that rely upon cosolvent mixtures. These preparation strategies hinge on the assumption that macromolecular solution nanostructures are kinetically stable following transfer from an organic/aqueous cosolvent into aqueous solution. Herein we demonstrate that unequivocal step-change shifts in micelle populations occur over several weeks following transfer into a highly selective solvent. The unexpected micelle growth evolves through a distinct bimodal distribution separated by multiple fusion events and critically depends on solution agitation. Notably, these results underscore fundamental similarities between assembly processes in amphiphilic polymer, small molecule, and protein systems. Moreover, the non-equilibrium micelle size increase can have a major impact on the assumed stability of solution assemblies, for which performance is dictated by nanocarrier size and structure.

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Section: Discussionmentioning

confidence: 99%

Size evolution of highly amphiphilic macromolecular solution assemblies via a distinct bimodal pathway

et al. 2014

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“…Although a variety of gold nanoparticle (Au NP) supraspheres have been prepared [14][15][16][17] , the hydrophobically driven formation of analogous assemblies in pure water remains elusive [18][19][20][21] . The main obstacle is that precipitation rapidly results from a lack of control over the aggregation processes 19 .…”

Section: Hydrophobically Driven Assembly In Watermentioning

confidence: 99%

Host–guest chemistry with water-soluble gold nanoparticle supraspheres

et al. 2016

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The uptake of molecular guests, a hallmark of the supramolecular chemistry of cages and containers, has yet to be documented for soluble assemblies of metal nanoparticles. Here we demonstrate that gold nanoparticle-based supraspheres serve as a host for the hydrophobic uptake, transport and subsequent release of over two million organic guests, exceeding by five orders of magnitude the capacities of individual supramolecular cages or containers and rivalling those of zeolites and metal-organic frameworks on a mass-per-volume basis. The supraspheres are prepared in water by adding hexanethiol to polyoxometalate-protected 4 nm gold nanoparticles. Each 200 nm assembly contains hydrophobic cavities between the estimated 27,400 gold building blocks that are connected to one another by nanometre-sized pores. This gives a percolated network that effectively absorbs large numbers of molecules from water, including 600,000, 2,100,000 and 2,600,000 molecules (35, 190 and 234 g l ) of para-dichorobenzene, bisphenol A and trinitrotoluene, respectively.H ost-guest phenomena that involve the uptake of gases and small molecules are associated with the supramolecular chemistry of soluble capsules, cages and containers [1][2][3][4][5] or, alternatively, with heterogeneous reactions of porous solid-state materials such as zeolites 6 and metal-organic frameworks 7 . Only now, however, are organized assemblies of metal nanoparticles beginning to serve in a similar capacity as hosts for molecular guests. In organic solvents, for example, light-induced dipoledipole interactions between gold nanoparticles with azobenzenefunctionalized thiolate ligands were recently used to entrap and catalyse the reactions of polar and alkylaromatic substrates 8 . By design, substrates were entrapped during nanoparticle aggregation to overcome the poor uptake and diffusion of molecular guests into colloidal nanocrystal assemblies. However, the uptake of molecular guests, a trait of supramolecular and solid-state chemistry, has so far not been achieved for colloidal nanoparticle assemblies.For that to occur, a thermodynamically favourable driving force must be combined with a porous structure whose interior architecture features host cavities, along with pathways for the effective diffusion of molecular guests from the exterior (bulk solution) to host domains deeply buried in the assembly's interior. If this were achieved, colloidal metal-nanoparticle assemblies could emerge as a new class of functional nano-engineered structures that are uniquely positioned between supramolecular containers and porous solid-state materials.We report a new class of functional assemblies, wherein the hydrophobic effect 9,10 drives the spontaneous uptake of alkyl and alkylaromatic guests 11 by porous 200 nm diameter supraspheres whose host capacities are orders of magnitude larger than those of individual cages or containers. On a mass-per-volume basis, the level of uptake rivals those of zeolites and metal-organic frameworks, which, for methane at elevated pressures, r...

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“…The most common geometry is (possibly branched) chains that are called “plasmonic polymers” because they give rise to a shift in the plasmon resonance of the nanocrystals . The spontaneous assembly of particles into chains has been achieved by chemical cross‐linking, physical attraction between ligands, or oriented attachment of nanocrystals . The aggregation number of these polymeric assemblies is usually between 5 and 20.…”

Section: Figurementioning

confidence: 99%

CdSe Nanoplatelets: Living Polymers

Jana

Abécassis

2016

Angewandte Chemie

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Colloidal CdSe nanoplatelets are considered to be excellent candidates for many applications in nanotechnology. One of the current challenges is to self‐assemble these colloidal quantum wells into large ordered structures to control their collective optical properties. We describe a simple and robust procedure to achieve controlled face‐to‐face self‐assembly of CdSe nanoplatelets into micron‐long polymer‐like threads made of up to ∼1000 particles. These structures are formed by addition of oleic acid to a stable colloidal dispersion of platelets, followed by slow drying and re‐dispersion. We could control the average length of the CdSe nanoplatelet threads by varying the amount of added oleic acid. These 1‐dimensional structures are flexible and feature a “living polymer” character because threads of a given length can be further grown through the addition of supplementary nanoplatelets at their reactive ends.

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Nucleation-Controlled Polymerization of Nanoparticles into Supramolecular Structures

Cited by 50 publications

References 36 publications

Size evolution of highly amphiphilic macromolecular solution assemblies via a distinct bimodal pathway

Size evolution of highly amphiphilic macromolecular solution assemblies via a distinct bimodal pathway

Host–guest chemistry with water-soluble gold nanoparticle supraspheres

CdSe Nanoplatelets: Living Polymers

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