Mimicking Biosintering: The Identification of Highly Condensed Surfaces in Bioinspired Silica Materials

Manning, Joseph R. H.; Walkley, Brant; Provis, John L.; Patwardhan, Siddharth V.

doi:10.1021/acs.langmuir.0c03261

Cited by 4 publications

(7 citation statements)

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“…Polyamine-embedded silicas have been used as catalysts and in water remidiation 63 . Furthermore, by posttreatment polyamine-incorporated silicas can be further processed to improve hydrothermal stability of silica 64 . Recently 65 , it has been demonstrated that through the use of cyclams and methylated diamines silica particles can be assembled to produce tuneable hollow structures.…”

Section: Discussionmentioning

confidence: 99%

Chain length of bioinspired polyamines affects size and condensation of monodisperse silica particles

et al. 2021

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Polyamines play a major role in biosilicification reactions in diatoms and sponges. While the effects of polyamines on silicic acid oligomerization and precipitation are well known, the impact of polyamines chain length on silica particle growth is unclear. We studied the effects of polyamine chain length on silica particle growth and condensation in a known, simple, and salt-free biphasic reaction system; with tetraethyl orthosilicate as organic phase and polyamine dissolved in the aqueous phase. The particles at various growth stages were characterized by Cryo- Transmission Electron Microscopy, Scanning Electron Microscopy, Thermogravimetric Analysis, Zeta Potential, and solid-state NMR analysis. Polyamines were found co-localized within silica particles and the particle diameter increased with an increase in polyamine chain length, whereas silica condensation showed the opposite trend. Particle growth is proposed to progress via a coacervate intermediate while the final particles have a core shell structure with an amine-rich core and silica-rich shell. The results presented in this paper would of interest for researchers working in the field of bioinspired materials.

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Section: Discussionmentioning

confidence: 99%

Chain length of bioinspired polyamines affects size and condensation of monodisperse silica particles

et al. 2021

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“… 44 In earlier work, an unproven multistep nonclassical formation pathway was postulated (see Figure 3 b). In terms of understanding the BIS reaction pathways and, more specifically, elucidating the molecular-scale mechanisms that underpin synthesis–property relationships, two avenues of inquiry have been pursued recently: a sequential DoE strategy for systematic and quantitative investigation of the BIS system’s reaction space and 16 a combination of experimental measurements (advanced characterization, including solid state NMR 45 ) and computation (multiscale modeling, including molecular dynamics simulations 46 ) to investigate the additive-silica interface at molecular length-scales. …”

Section: Pathway Understandingmentioning

confidence: 99%

“…a combination of experimental measurements (advanced characterization, including solid state NMR 45 ) and computation (multiscale modeling, including molecular dynamics simulations 46 ) to investigate the additive-silica interface at molecular length-scales.…”

Section: Pathway Understandingmentioning

confidence: 99%

“…48 In a further study, advanced characterization (ssNMR) of BIS identified unexpected, yet significant association between the additives and fully condensed (uncharged) surface silicon species, leading to higher levels of condensation and greater hydrothermal stability than benchmark materials (despite BIS products having a shorter synthesis time). 45 These effects are attributed to the polyfunctional and catalytic nature of the additives. The charge-matching initiates additive-silica interactions at multiple surface sites followed by corresponding catalytic condensation of SiO − moieties at multiple sites.…”

Section: Othersmentioning

confidence: 99%

“…(1) a sequential DoE strategy for systematic and quantitative investigation of the BIS system's reaction space and 16 (2) a combination of experimental measurements (advanced characterization, including solid state NMR 45 ) and computation (multiscale modeling, including molecular dynamics simulations 46 ) to investigate the additive-silica interface at molecular length-scales. The DoE investigation, previously summarized, crucially demonstrated and quantified the pH dependency of the system.…”

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Recent Advances in Enabling Green Manufacture of Functional Nanomaterials: A Case Study of Bioinspired Silica

Pilling

Patwardhan

2022

ACS Sustainable Chem. Eng.

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Global specialty silica production is over 3 million tonnes per annum with diverse applications across sectors and an increasing demand for more complex material structures and surface chemistries. Commercial manufacturing of high-value silica nanomaterials is energy and resource intensive. In order to meet market needs and mitigate environmental impacts, new synthesis methods for these porous materials are required. The development of the bioinspired silica (BIS) product system, which is the focus of this review, provides a potential solution to this challenge. BIS is a versatile and greener route with the prospect of good scalability, attractive process economics and well controlled product materials. The potential of the system lies not only in its provision of specific lead materials but also, as itself, a rich design-space for the flexible and potentially predictive design of diverse sustainable silica nanomaterials. Realizing the potential of this design space, requires an integrative mind-set, which enables parallel and responsive progression of multiple and dependent research strands, according to need, opportunities, and emergent knowledge. Specifically, this requires development of detailed understanding of (i) the pathways and extent of material diversity and control, (ii) the influences and mechanisms of scale-up, and (iii) performance, economic and environmental characteristics and sensitivities. Crucially, these need to be developed for the system overall, which sits in contrast to a more traditional research approach, which focuses initially on the discovery of specific material leads at the laboratory scale, leaving scale-up, commercialization, and, potentially, pathway understanding to be considered as distinctly separate concerns. The intention of this review is to present important recent advances made in the field of BIS. Specifically, advances made along three research themes will be discussed: (a) particle formation pathways, (b) product design, and (c) scale-up and manufacture. These advances include first quantitative investigation of synthesis-product relationships, first structured investigation of mixing effects, preparation of a broad range of functionalized and encapsulated silica materials and continued industrial engagement and market research. We identify future challenges and provide an important foundation for the development of new research avenues. These include the need to develop comprehensive and predictive product design models, to understand markets in terms of product cost, performance and environmental considerations, and to develop capabilities enabling rapid prototyping and scale-up of desired nanomaterials.

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Silica-Coated Micrometer-Sized Latex Particles

et al. 2023

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A series of silica-coated micrometer-sized poly(methyl methacrylate) latex particles are prepared using a Stöber silica deposition protocol that employs tetraethyl orthosilicate (TEOS) as a soluble silica precursor. Given the relatively low specific surface area of the latex particles, silica deposition is best conducted at relatively high solids to ensure a sufficiently high surface area. Such conditions aid process intensification. Importantly, physical adsorption of chitosan onto the latex particles prior to silica deposition minimizes secondary nucleation and promotes the formation of silica shells: in the absence of chitosan, well-defined silica overlayers cannot be obtained. Thermogravimetry studies indicate that silica formation is complete within a few hours at 20 °C regardless of the presence or absence of chitosan. Kinetic data obtained using this technique suggest that the adsorbed chitosan chains promote surface deposition of silica onto the latex particles but do not catalyze its formation. Systematic variation of the TEOS/latex mass ratio enables the mean silica shell thickness to be tuned from 45 to 144 nm. Scanning electron microscopy (SEM) studies of silica-coated latex particles after calcination at 400 °C confirm the presence of hollow silica particles, which indicates the formation of relatively smooth (albeit brittle) silica shells under optimized conditions. Aqueous electrophoresis and X-ray photoelectron spectroscopy studies are also consistent with latex particles coated in a uniform silica overlayer. The silica deposition formulation reported herein is expected to be a useful generic strategy for the efficient coating of micrometer-sized particles at relatively high solids.

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Mimicking Biosintering: The Identification of Highly Condensed Surfaces in Bioinspired Silica Materials

Cited by 4 publications

References 54 publications

Chain length of bioinspired polyamines affects size and condensation of monodisperse silica particles

Chain length of bioinspired polyamines affects size and condensation of monodisperse silica particles

Recent Advances in Enabling Green Manufacture of Functional Nanomaterials: A Case Study of Bioinspired Silica

Silica-Coated Micrometer-Sized Latex Particles

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