Improved Molecular Imprinting Based on Colloidal Particles Made from Miniemulsion: A Case Study on Testosterone and Its Structural Analogues

Kellens, Evelien; Bové, Hannelore; Conradi, Matthias; D’Olieslaeger, Lien; Wagner, Patrick; Landfester, Katharina; Junkers, Thomas; Ethirajan, Anitha

doi:10.1021/acs.macromol.6b00130

Cited by 23 publications

(25 citation statements)

References 62 publications

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“…This templating could be considered a corona phase analog of molecular imprinting, except that the template remains bound to the backbone and no cross-linking is required. [48][49][50][51][52][53][54] An advantage is that the newly created binding site has direct access to the transducer, which can remain nanometer in scale. The bound appendage should be reversibly displaced upon addition of a more strongly adsorbing analyte.…”

Section: Polymer Library Designmentioning

confidence: 99%

Implantable Nanosensors for Human Steroid Hormone Sensing In Vivo Using a Self‐Templating Corona Phase Molecular Recognition

Lee

Wang

Jin

et al. 2020

Adv Healthcare Materials

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Dynamic measurements of steroid hormones in vivo are critical, but steroid sensing is currently limited by the availability of specific molecular recognition elements due to the chemical similarity of these hormones. In this work, a new, self-templating synthetic approach is applied using corona phase molecular recognition (CoPhMoRe) targeting the steroid family of molecules to produce near infrared fluorescent, implantable sensors. A key limitation of CoPhMoRe has been its reliance on library generation for sensor screening. This problem is addressed with a self-templating strategy of polymer design, using the examples of progesterone and cortisol sensing based on a styrene and acrylic acid copolymer library augmented with an acrylated steroid. The pendant steroid attached to the corona backbone is shown to self-template the phase, providing a unique CoPhMoRE design strategy with high efficacy. The resulting sensors exhibit excellent stability and reversibility upon repeated analyte cycling. It is shown that molecular recognition using such constructs is viable even in vivo after sensor implantation into a murine model by employing a poly (ethylene glycol) diacrylate (PEGDA) hydrogel and porous cellulose interface to limit nonspecific absorption. The results demonstrate that CoPhMoRe templating is sufficiently robust to enable a new class of continuous, in vivo biosensors.

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Section: Polymer Library Designmentioning

confidence: 99%

Implantable Nanosensors for Human Steroid Hormone Sensing In Vivo Using a Self‐Templating Corona Phase Molecular Recognition

Lee

Wang

Jin

et al. 2020

Adv Healthcare Materials

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“…No report has yet been made for brush formation of acidic monomers, which may have interesting biomedical application due to their polyelectrolyte character. Also the employment of amine carrying functional monomers is via such route enabled due to absence of ligand competition.…”

Section: Introductionmentioning

confidence: 99%

Organocatalyzed Photo‐Atom Transfer Radical Polymerization of Methacrylic Acid in Continuous Flow and Surface Grafting

Ramakers

Krivcov

Trouillet

et al. 2017

Macromol. Rapid Commun.

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The organocatalyzed photo-atom transfer radical polymerization (photoATRP) using 10-phenylphenothiazine as catalyst is studied toward its use in methacrylic acid (MAA) polymerization and surface grafting. The organocatalyzed photoATRP of methyl methacrylate (MMA) is first optimized for continuous flow synthesis in order to assess the livingness of the polymerization. MMA can be polymerized in batch and in flow; however, conversions are limited by the loss of bromine functionality and hence high conversions have to be traded in with increasing dispersities. Also, MAA is polymerized successfully in continuous flow with similar limitations. Flow conditions are transferred to surface grafting from silanized silicon wafers. The presence of ATRP initiators after silanization is confirmed by secondary ion mass spectrometry and X-ray photoelectron spectroscopy. Dense polymethacrylic acid brush films are successfully produced, which is not directly accessible via classical copper-mediated ATRP techniques.

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“…As a result of the EDL formation, properties of the liquid such as viscosity, diffusion coefficient, structuring at the interface differ significantly from bulk values. A detailed understanding of the molecular structure of EDLs is essential for many chemical and engineering processes, such as adsorption, adhesion, catalysis, electrochemical processes, clay swelling, colloidal dispersions, or the biomedical sciences …”

Section: Introductionmentioning

confidence: 99%

Anion Layering and Steric Hydration Repulsion on Positively Charged Surfaces in Aqueous Electrolytes

Weber

Cheng

et al. 2017

ChemPhysChem

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The molecular structure at charged solid/liquid interfaces is vital for many chemical or electrochemical processes, such as adhesion, catalysis, or the stability of colloidal dispersions. How cations influence structural hydration forces and interactions across negatively charged surfaces has been studied in great detail. However, how anions influence structural hydration forces on positively charged surfaces is much less understood. Herein we report force versus distance profiles on freshly cleaved mica using atomic force microscopy with silicon tips. We characterize steric anion hydration forces for a set of common anions (Cl , ClO , NO , SO and PO ) in pure acids at pH ≈1, where protons are the co-ions. Solutions containing anions with low hydration energies exhibit repulsive structural hydration forces, indicating significant ion and/or water structuring within the first 1-2 nm on a positively charged surface. We attribute this to specific adsorption effects within the Stern layer. In contrast, ions with high hydration energies show exponentially repulsive hydration forces, indicating a lower degree of structuring within the Stern layer. The presented data demonstrates that anion hydration forces in the inner double layer are comparable to cation hydration forces, and that they qualitatively correlate with hydration free energies. This work contributes to understanding interaction processes in which positive charge is screened by anions within an electrolyte.

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Improved Molecular Imprinting Based on Colloidal Particles Made from Miniemulsion: A Case Study on Testosterone and Its Structural Analogues

Cited by 23 publications

References 62 publications

Implantable Nanosensors for Human Steroid Hormone Sensing In Vivo Using a Self‐Templating Corona Phase Molecular Recognition

Implantable Nanosensors for Human Steroid Hormone Sensing In Vivo Using a Self‐Templating Corona Phase Molecular Recognition

Organocatalyzed Photo‐Atom Transfer Radical Polymerization of Methacrylic Acid in Continuous Flow and Surface Grafting

Anion Layering and Steric Hydration Repulsion on Positively Charged Surfaces in Aqueous Electrolytes

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