Silicatein and the Translation of its Molecular Mechanism of Biosilicification into Low Temperature Nanomaterial Synthesis

Brutchey, Richard L.; Morse, Daniel E.

doi:10.1021/cr078256b

Cited by 221 publications

(222 citation statements)

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“…Otherwise, silicatein, silaffin and polyamines have been identified as constituents of the axial filaments in sponges and the cell walls in diatoms. 3,8,9 Although this fact strongly suggests that they process silica in the heterogeneous phase, as far as we know, there is no information about in vitro processes carried out under this conditioning (i.e. on the role of solid phase additives).…”

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confidence: 99%

Biomimetic chitosan-mediated synthesis in heterogeneous phase of bulk and mesoporous silica nanoparticles

et al. 2009

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Both bulk and mesoporous silica nanoparticles can be obtained in the form of granular aggregates using chitosan flakes as additive under very soft biomimetic reaction conditions.Biomineralization, that is the formation under extremely soft conditions of complex hierarchical inorganic materials by biological systems, is an exciting research field of increasing interest. 1 Indeed, while technological silica production usually requires vigorous conditions at high pH, 2 certain marine organisms and some higher plants are capable of forming silica skeletons under mild temperature and pressure conditions at circumneutral pH. 1,3,4 Such in vivo processes generating intricate silica nano and macro-scale patterns are speciesspecific, presumably encoded in the genome; 5-7 the possibility of controlling them in the laboratory remains a long-term major challenge. Notwithstanding, there have been different biomolecules identified like silicatein, silaffin and polyamines, which can play key roles in the hydrolysis, condensation and aggregation of the silica species. 3,4,8 Silica is widely used in industry, medicine and nanotechnology in a huge variety of forms. 2,7,9 This, coupled with the insufficiency of natural products of adequate purity and the scientific interest, justifies the search for bioinspired synthesis 8,10 leading to new silica-based materials with simple hierarchical structures or, at least, allowing silica production under soft-conditions (low-cost strategies). Then, inspired by nature, a variety of reagents have been added to check in vitro silicification processes in solution. 11,12 These additives, which intend to mimic the active natural molecules, can play different roles: catalysts, aggregation promoting reagents or structural directing agents. Otherwise, silicatein, silaffin and polyamines have been identified as constituents of the axial filaments in sponges and the cell walls in diatoms. 3,8,9 Although this fact strongly suggests that they process silica in the heterogeneous phase, as far as we know, there is no information about in vitro processes carried out under this conditioning (i.e. on the role of solid phase additives).Here we show how using solid flakes of chitosan (a commercial and low-cost biopolymer present in the shells of crustaceans and the cell walls of fungi and yeast, as well as in squid pens) 13 as additive, it is possible to promote silica polymerization and aggregation in the heterogeneous phase at room temperature, neutral pH and silica concentrations as low as those occurring in sea water or inside the diatom frustules. Our procedural approach leads to bulk biosilica nanoparticles or, alternatively, to similar mesoporous architectures when structural directing agents (SDA) are also added.In order to mimic frustule conditions, 6,14 we have performed the reactions in circulating silica solutions on chitosan flakes blocked in a part of the system in order to favour a certain confining effect (see ESIw). Summarized in Table 1 are the main parameters concerning syntheses of some sel...

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confidence: 99%

Biomimetic chitosan-mediated synthesis in heterogeneous phase of bulk and mesoporous silica nanoparticles

et al. 2009

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“…[18][19][20][21][22] Interested in studying the support structures present within T. aurantia,M orse and his research team discovered that the spicules that the sponge produced to reinforce its biological framework were actually templated on protein filaments (Figure 2). [18] This work demonstrated that, not only did the protein strands act as templates upon which dissolved silicic acid from the surrounding sea water was condensed into silica, but that the protein actually served to catalyze the process.…”

Section: Silicateinmentioning

confidence: 99%

Biocatalysis in Silicon Chemistry

Frampton

Zelisko

2017

Chemistry An Asian Journal

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The application of biocatalytic or chemoenzymatic techniquesi ns ilicon chemistry serves two roles:i tp rovides ag reater understanding of the processing of silicon species by natural systems, such as plants, diatoms, and sponges, as well openingu pa venues to green methodologies in the field. In the latter case, biocatalytic approaches have been applied to the synthesis of small-molecule systems and polymeric materials. Often these biocatalytic approaches allow access to molecular structures under mild conditions and, in some cases, molecular structures that are not accessible throught raditional chemical methodologies. Ar eview of recent advances in the applications of biocatalysis in silicon chemistry is presented.

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“…Central to biogenic control over mineralization is the use of soluble organic additives, where these can even guide the assembly of composite materials [4][5][6][7][8][9] with superior mechanical properties. [ 3,4,10 ] Many bioinspired mineralization strategies therefore utilize either naturally extracted biomacromolecules or their synthetic analogues, [ 1,2,5,7,9,10 ] and even small organic species such as amino acids and surfactants can exert considerable control over mineralization, sometimes supporting the formation of complex particle assemblies. [ 5,6,8,[11][12][13] While attractive, however, this approach is still hampered by the diffi culty in selecting appropriate organic additives-and in particular combinations of additives-to give materials with target structures and properties.…”

Section: Doi: 101002/adma201403185mentioning

confidence: 99%

“…[1][2][3] These bioinspired methods are characterized by mild reaction conditions and promise the ability to generate structures comparable to those found in nature. Central to biogenic control over mineralization is the use of soluble organic additives, where these can even guide the assembly of composite materials [4][5][6][7][8][9] with superior mechanical properties. [ 3,4,10 ] Many bioinspired mineralization strategies therefore utilize either naturally extracted biomacromolecules or their synthetic analogues, [ 1,2,5,7,9,10 ] and even small organic species such as amino acids and surfactants can exert considerable control over mineralization, sometimes supporting the formation of complex particle assemblies.…”

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Genetic Algorithm‐Guided Discovery of Additive Combinations That Direct Quantum Dot Assembly

et al. 2014

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these techniques are limited by the requirement for complex enzymatic reactions. As an alternative strategy that bypasses the need for genetic engineering, combinatorial methods can be employed. These can be used to explore tens to hundreds of reaction conditions, where the most promising or "lead" conditions may be selected based on the structures or properties of the resultant material. [ 17,18 ] Lead conditions can then be used to narrow the reaction landscape in successive screening rounds. Surprisingly, although combinatorial methods are often used in solid-state chemistry to explore, for example, different reagent compositions, [ 18 ] we are not aware of their use in identifying soluble additives capable of directing mineralization.In this article we demonstrate how combinatorial methods can be used in conjunction with effi cient screening processes to rapidly identify combinations of small organic molecules that are capable of directing the formation of photoluminescent quantum dot minerals in aqueous solution and at room temperature. Indeed, a key feature of biomineralization processes is that control over mineral formation is achieved using many soluble additives that operate in concert. That this feature has seldom been addressed in bioinspired methods is almost certainly due to the vast number of potential variables, which renders a full, systematic exploration intractable. As a solution to this challenge, we here utilize a genetic algorithm as a bioinspired heuristic that mimics natural evolution. Genetic algorithms use selection, recombination, and mutation strategies to rapidly identify and optimize the combination of conditions (here, soluble additives), which gives rise to materials with target properties. [ 19 ] Using a pipetting robot to prepare reaction sets and a UV-light table to rapidly assess the reactions for the formation of photoluminescent minerals, we are able to rapidly identify the key additives that promote the formation of quantum dot superstructures from one-pot aqueous reactions.Our initial library of organic mediators included 23 components, of which 17 were amino acids and 6 were surfactants. Stock solutions of the amino acids were prepared to initial concentrations of 100 × 10 −3 M , and explored at concentrations ranging from 0.01 to 50 × 10 −3 M , while surfactants were prepared to near their solubility limits in water. Surfactants were included as potential structure-directing agents to drive hierarchical assembly in aqueous solution. The overall screening approach used to identify the key additive set is summarized in Figure 1 . First, library amino acids and surfactants were randomly mixed in 48 wells of a multi-well plate, such that each well contained between 1-6 amino acids and 1-3 surfactants (Figure 1 A). Cadmium chloride and thioacetic acid (as a sulfur source) [ 20 ] were then added to a concentration of 1 × 10 −3 M in all wells, as precursors for CdS. After 3 d the plate was viewed under UV illumination (Figure 1 A) and with a fl uorimetric Biomineralization, whi...

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Silicatein and the Translation of its Molecular Mechanism of Biosilicification into Low Temperature Nanomaterial Synthesis

Cited by 221 publications

References 134 publications

Biomimetic chitosan-mediated synthesis in heterogeneous phase of bulk and mesoporous silica nanoparticles

Biomimetic chitosan-mediated synthesis in heterogeneous phase of bulk and mesoporous silica nanoparticles

Biocatalysis in Silicon Chemistry

Genetic Algorithm‐Guided Discovery of Additive Combinations That Direct Quantum Dot Assembly

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