Controlled biomimetic silica formation using star-shaped poly(l-lysine)

Wang, Qinrong; Yu, Jun; Yan, Yunsong; Xu, Shaoqiang; Wang, Fangfang; Li, Qingnan; Wang, Jinzhi; Zhang, Xin; Liu, Daojun

doi:10.1039/c2py20070h

Cited by 13 publications

(16 citation statements)

References 48 publications

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“…137 Specifically, a PEI core (MW ≈ 10 kDa) with ca. 60 primary amine groups was employed as an initiator to generate star polymers with PLL arms (ca.…”

Section: Chemical Reviewsmentioning

confidence: 99%

Star Polymers

et al. 2016

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Recent advances in controlled/living polymerization techniques and highly efficient coupling chemistries have enabled the facile synthesis of complex polymer architectures with controlled dimensions and functionality. As an example, star polymers consist of many linear polymers fused at a central point with a large number of chain end functionalities. Owing to this exclusive structure, star polymers exhibit some remarkable characteristics and properties unattainable by simple linear polymers. Hence, they constitute a unique class of technologically important nanomaterials that have been utilized or are currently under audition for many applications in life sciences and nanotechnologies. This article first provides a comprehensive summary of synthetic strategies towards star polymers, then reviews the latest developments in the synthesis and characterization methods of star macromolecules, and lastly outlines emerging applications and current commercial use of star-shaped polymers. The aim of this work is to promote star polymer research, generate new avenues of scientific investigation, and provide contemporary perspectives on chemical innovation that may expedite the commercialization of new star nanomaterials. We envision in the not-too-distant future star polymers will play an increasingly important role in materials science and nanotechnology in both academic and industrial settings.

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“…137 Specifically, a PEI core (MW ≈ 10 kDa) with ca. 60 primary amine groups was employed as an initiator to generate star polymers with PLL arms (ca.…”

Section: Chemical Reviewsmentioning

confidence: 99%

Star Polymers

et al. 2016

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“…[4] These features modifythe nucleationf ree energy barriera nd nucleation kinetics of silica, which ultimately governt he growth into well-defineds tructures. [5][6][7][8][9][10] Building upon the lessons learned from insightful work on biomineralization, numerouss ilica production strategies have used amine-bearing polymers such as poly(ethyleneimine), [11][12][13] polylysine, [14][15][16][17][18][19] peptides, [20][21][22] and block copolymers [23][24][25][26] to obtainh ighlyi ntricate structures. This methodi sa dvantageous because the amine-rich polymers not only serve as as caffold but also act as acatalysttopromote the condensation of silicic acid.…”

Section: Introductionmentioning

confidence: 99%

“…Building upon the lessons learned from insightful work on biomineralization, numerous silica production strategies have used amine‐bearing polymers such as poly(ethyleneimine), [11–13] polylysine, [14–19] peptides, [20–22] and block copolymers [23–26] to obtain highly intricate structures. This method is advantageous because the amine‐rich polymers not only serve as a scaffold but also act as a catalyst to promote the condensation of silicic acid.…”

Section: Introductionmentioning

confidence: 99%

Bioinspired Scaffolding by Supramolecular Amines Allows the Formation of One‐ and Two‐Dimensional Silica Superstructures

Magana

Gumí-Audenis

Tas

et al. 2020

Chemistry A European J

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Silica materials attract an increasing amount of interest in (fundamental) research, and find applications in, for example, sensing, catalysis, and drug delivery.A st he properties of these (nano)materials not only depend on their chemistry but also their size, shape,a nd surface area, the controllable synthesis of silica is essential for tailoringt he materials to specific applications. Advantageously,b ioinspired routes for silica production are environmentally friendly ands traightforward since the formation process is spontaneousa nd proceeds under mild conditions. These strategies mostly employ amine-bearing phosphorylated (bio)polymers. In this work, we expand this principle to supramolecular polymers based on the water-soluble cationic cyanine dye Pinacyanol acetate. Upon assembly in water, these dye molecules form large, polyaminated, supramolecular fibers.T he surfaces of these fibers can be used as ascaffold for the condensation of silicic acid. Controlo ver the ionic strength, dye concentration, and silicic acid saturation yielded silica fibers with ad iameter of 25 nm and as ingle, 4nmp ore. Unexpectedly,o ther unusual superstructures, namely,n ummulites and spherulites, are also observed depending on the ionic strength and dye concentration.T ransmission and scanning electronm icroscopy (TEM and SEM) showedt hat these superstructures are formed by aligned silica fibers. Close examination of the dye scaffold prior silicification using small-angle X-ray scattering (SAXS), and UV/Vis spectroscopy revealed minor influence of the ionic strength and dye concentration on the morphologyo ft he supramolecular scaffold.T otal internal reflection fluorescence (TIRF) during silicification unraveledt hat if the reaction is kept under static conditions, only silica fibers are obtained. Experiments performed on the dye scaffold and silica superstructures evidenced that the marked structurald iversity originates from the arrangemento fs ilica/dye fibers. Under these mild conditions, external force fields can profoundly influence the morphologyo ft he produced silica.

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“…15−19 The bathochromic shift in the minimum or maximum wavelength is reasonably ascribed to the specific branched structure. 29−31 In comparison, BPL-4 predominantly adopts a β-sheet conformation, as evidenced by a negative band at 203 nm and a positive band at 240 nm. Generally, the positive peak at 210 31 or 218 nm 29 could be a characteristic of type II β-turns.…”

Section: Results and Discussionmentioning

confidence: 99%

Synthesis of Polylysine/Silica Hybrids through Branched-Polylysine-Mediated Biosilicification

Min

Liu

et al. 2018

ACS Omega

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Although many biosilicification methods based on cationic linear α-poly - l - lysine for synthesis of polylysine/silica hybrids have been investigated, these methods tend to rely on the counteranions, added catalysts, and complex synthesis process. To explore a simple and efficient biosilicification method, in this work, branched poly- l -lysine (BPL) is used as both a catalyst to hydrolyze tetraethoxysilane (TEOS) and an in situ template to direct silicic acids forming polylysine/silica hybrids in one-pot mode. The catalysis of BPL to hydrolyze TEOS results from the abundant hydrogen bonding (as the active site) to increase the nucleophilicity of BPL. Meanwhile, the hydrogen bonding is also found to be the key factor determining the self-assembly of BPL. During biosilicification, owing to self-assembly of BPL molecules, BPL would form spherical particles by keeping a random-coil conformation or form lamellar structures by undergoing a conformational transition from a random-coil to β-sheet construction. As a result, polylysine/silica hybrids with tunable topological structures are synthesized using aggregated BPLs as templates after the hydrolysis of TEOS. This finding of applying BPL to fulfill the biosilicification procedure without counteranions and added catalysts would enable a better understanding of the polypeptide-governed biosilicification process and pave a way for fabricating complex inorganic architectures applicable to silica transformational chemistry.

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Controlled biomimetic silica formation using star-shaped poly(l-lysine)

Cited by 13 publications

References 48 publications

Star Polymers

Star Polymers

Bioinspired Scaffolding by Supramolecular Amines Allows the Formation of One‐ and Two‐Dimensional Silica Superstructures

Synthesis of Polylysine/Silica Hybrids through Branched-Polylysine-Mediated Biosilicification

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