| 1. |
- Nicholls, Ian A., et al.
(författare)
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Rational design of biomimetic molecularly imprinted materials : theoretical and computational strategies for guiding nanoscale structured polymer development
- 2011
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Ingår i: Analytical and Bioanalytical Chemistry. - : Springer Science and Business Media LLC. - 1618-2642 .- 1618-2650. ; 400:6, s. 1771-1786
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Forskningsöversikt (refereegranskat)abstract
- In principle, molecularly imprinted polymer science and technology provides a means for ready access to nano-structured polymeric materials of predetermined selectivity. The versatility of the technique has brought it to the attention of many working with the development of nanomaterials with biological or biomimetic properties for use as therapeutics or in medical devices. Nonetheless, the further evolution of the field necessitates the development of robust predictive tools capable of handling the complexity of molecular imprinting systems. The rapid growth in computer power and software over the past decade has opened new possibilities for simulating aspects of the complex molecular imprinting process. We present here a survey of the current status of the use of in silico-based approaches to aspects of molecular imprinting. Finally, we highlight areas where ongoing and future efforts should yield information critical to our understanding of the underlying mechanisms sufficient to permit the rational design of molecularly imprinted polymers.
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| 2. |
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| 3. |
- Nicholls, Ian A., et al.
(författare)
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Theoretical and Computational Strategies in Molecularly Imprinted Polymer Development
- 2018
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Ingår i: Molecularly Imprinted Polymers for Analytical Chemistry Applications. - London : Royal Society of Chemistry. - 9781782626473 - 9781788010474 - 9781788014274 ; , s. 197-226
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Bokkapitel (refereegranskat)abstract
- Theoretical and computational studies of molecular imprinting have helped provide valuable insights concerning the nature of the molecular-level events underlying the recognition characteristics of molecularly imprinted materials. Here, we first present an overview of a thermodynamic treatment of factors governing the behaviour of these functional materials, and then a summary of the development and current status of the use of computational strategies for studying aspects of molecular imprinting and the resulting material properties.
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| 4. |
- Olsson, Gustaf D., et al.
(författare)
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Mechanisms underlying molecularly imprinted polymer molecular memory and the role of crosslinker : resolving debate on the nature of template recognition in phenylalanine anilide imprinted polymers
- 2012
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Ingår i: Journal of Molecular Recognition. - : Wiley. - 0952-3499 .- 1099-1352. ; 25:2, s. 69-73
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Tidskriftsartikel (refereegranskat)abstract
- A series of molecular dynamics simulations of prepolymerization mixtures for phenylalanine anilide imprinted co-(ethylene glycol dimethacrylate-methacrylic acid) molecularly imprinted polymers have been employed to investigate the mechanistic basis for template selective recognition in these systems. This has provided new insights on the mechanisms underlying template recognition, in particular the significant role played by the crosslinking agent. Importantly, the study supports the occurrence of template self-association events that allows us to resolve debate between the two previously proposed models used to explain this system's underlying recognition mechanisms. Moreover, the complexity of the molecular level events underlying template complexation is highlighted by this study, a factor that should be considered in rational molecularly imprinted polymer design, especially with respect to recognition site heterogeneity.
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| 5. |
- Refaat, Doaa, et al.
(författare)
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Strategies for Molecular Imprinting and the Evolution of MIP Nanoparticles as Plastic Antibodies-Synthesis and Applications
- 2019
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Ingår i: International Journal of Molecular Sciences. - : MDPI. - 1661-6596 .- 1422-0067. ; 20:24, s. 1-21
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Forskningsöversikt (refereegranskat)abstract
- Materials that can mimic the molecular recognition-based functions found in biology are a significant goal for science and technology. Molecular imprinting is a technology that addresses this challenge by providing polymeric materials with antibody-like recognition characteristics. Recently, significant progress has been achieved in solving many of the practical problems traditionally associated with molecularly imprinted polymers (MIPs), such as difficulties with imprinting of proteins, poor compatibility with aqueous environments, template leakage, and the presence of heterogeneous populations of binding sites in the polymers that contribute to high levels of non-specific binding. This success is closely related to the technology-driven shift in MIP research from traditional bulk polymer formats into the nanomaterial domain. The aim of this article is to throw light on recent developments in this field and to present a critical discussion of the current state of molecular imprinting and its potential in real world applications.
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| 6. |
- Wiklander, Jesper G., 1974-, et al.
(författare)
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Towards a synthetic avidin mimic
- 2011
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Ingår i: Analytical and Bioanalytical Chemistry. - : Springer Science and Business Media LLC. - 1618-2642 .- 1618-2650. ; 400:5, s. 1397-1404
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Tidskriftsartikel (refereegranskat)abstract
- A series of streptavidin-mimicking molecularly imprinted polymers has been developed and evaluated for their biotin binding characteristics. A combination of molecular dynamics and NMR spectroscopy was used to examine potential polymer systems, in particular with the functional monomers methacrylic acid and 2-acrylamidopyridine. The synthesis of copolymers of ethylene dimethacrylate and one or both of these functional monomers was performed. A combination of radioligand binding studies and surface area analyses demonstrated the presence of selectivity in polymers prepared using methacrylic acid as the functional monomer. This was predicted by the molecular dynamics studies showing the power of this methodology as a prognostic tool for predicting the behavior of molecularly imprinted polymers.
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| 7. |
- Anaspure, Prasad
(författare)
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Novel strategies for C-C/X bond formation
- 2022
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Doktorsavhandling (övrigt vetenskapligt/konstnärligt)abstract
- The formation of C-C/X bonds is essential for the manufacture of a broad range of chemicals and materials used in areas critical for maintaining quality of life in modern society, e.g. pharmaceuticals, agrochemicals and polymers, and for aspects of research in organic chemistry. The use of catalysts for facilitating these reactions is highly desirable due to the improvements in energy and atom economies that can potentially be achieved.The primary objective of the thesis was to explore novel approaches for catalysis of C-C/X bond-forming reactions, both through C-H activation. In paper I, at unable cobalt catalyzed C-H activation-driven annulation of benzamides with unsymmetrical diynes was developed, where either 3- or 4-substitution of the isoquinolone could be steered by the nature of the diyne used. Anunprecedented iridium catalyzed tandem bis-arylsulfenylation of indoles was described (paper II), where an adamantoyl sacrificial directing group plays a key role in the simultaneous direction of arylsulfenylation to the 2- and 4- positions. In paper III, a flow reactor in a lab-on-a-chip device was developed for the Suzuki cross-coupling reaction. Miniaturization provides the opportunity to reduce material consumption. Polyethyleneimine (PEI)-brushes were used for the immobilization of Pd-nanoparticles, and high efficiencies were observed. Collectively, the research underpinning this thesis provides new strategies forC-C and C-X(S) bond formation.
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| 8. |
- Boventi, Matteo, et al.
(författare)
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Porosity of Molecularly Imprinted Polymers Investigated by 129Xe NMR Spectroscopy
- 2022
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Ingår i: ACS Applied Polymer Materials. - : American Chemical Society (ACS). - 2637-6105. ; 4:12, s. 8740-8749
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Tidskriftsartikel (refereegranskat)abstract
- Molecularly imprinted polymers (MIPs) display intriguing recognition properties and can be used as sensor recognition elements or in separation. In this work, we investigated the formation of hierarchical porosity of compositionally varied MIPs using 129Xe Nuclear Magnetic Resonance (NMR) and 1H Time Domain Nuclear Magnetic Resonance (TD-NMR). Variable temperature 129Xe NMR established the morphological variation with respect to the degree of cross-linking, supported by 1H TDNMR determination of polymer chain mobility. Together, the results indicate that a high degree of cross-linking stabilizes the porous structure: highly cross-linked samples display a significant amount of accessible mesopores that instead collapse in less structured polymers. No significant differences can be detected due to the presence of templated pores in molecularly imprinted polymers: in the dry state, these specific shapes are too small to accommodate xenon atoms, which, instead, probe higher levels in the porous structure, allowing their study in detail. Additional resonances at a high chemical shift are detected in the 129Xe NMR spectra. Even though their chemical shifts are compatible with xenon dissolved in bulk polymers, variable temperature experiments rule out this possibility. The combination of 129Xe and TDNMR data allows attribution of these resonances to softer superficial regions probed by xenon in the NMR time scale. This can contribute to the understanding of the surface dynamics of polymers.
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| 9. |
- Dhillon, Prakriti, et al.
(författare)
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Diyne-steered switchable regioselectivity in cobalt(ii)-catalysed C(sp(2))-H activation of amides with unsymmetrical 1,3-diynes
- 2023
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Ingår i: Organic and biomolecular chemistry. - : Royal Society of Chemistry. - 1477-0520 .- 1477-0539. ; 21:9, s. 1942-1951
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Tidskriftsartikel (refereegranskat)abstract
- The regiochemical outcome of a cobalt(ii) catalysed C-H activation reaction of aminoquinoline benzamides with unsymmetrical 1,3-diynes under relatively mild reaction conditions can be steered through the choice of diyne. The choice of diyne provides access to either 3- or 4-hydroxyalkyl isoquinolinones, paving the way for the synthesis of more highly elaborate isoquinolines.
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| 10. |
- Mahajan, Rashmi, et al.
(författare)
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Oxytocin-Selective Nanogel Antibody Mimics
- 2022
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Ingår i: International Journal of Molecular Sciences. - : MDPI. - 1661-6596 .- 1422-0067. ; 23:5
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Tidskriftsartikel (refereegranskat)abstract
- Oxytocin imprinted polymer nanoparticles were synthesized by glass bead supported solid phase synthesis, with NMR and molecular dynamics studies used to investigate monomer-template interactions. The nanoparticles were characterized by dynamic light scattering, scanning- and transmission electron microscopy and X-ray photoelectron spectroscopy. Investigation of nanoparticle-template recognition using quartz crystal microbalance-based studies revealed sub-nanomolar affinity, k(d) approximate to 0.3 +/- 0.02 nM (standard error of the mean), comparable to that of commercial polyclonal antibodies, k(d) approximate to 0.02-0.2 nM.
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| 11. |
- Mavliutova, Liliia, et al.
(författare)
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Discrimination between sialic acid linkage modes using sialyllactose-imprinted polymers
- 2021
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Ingår i: RSC Advances. - : Royal Society of Chemistry. - 2046-2069. ; 11:36, s. 22409-22418
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Tidskriftsartikel (refereegranskat)abstract
- Glycosylation plays an important role in various pathological processes such as cancer. One key alteration in the glycosylation pattern correlated with cancer progression is an increased level as well as changes in the type of sialylation. Developing molecularly-imprinted polymers (MIPs) with high affinity for sialic acid able to distinguish different glycoforms such as sialic acid linkages is an important task which can help in early cancer diagnosis. Sialyllactose with alpha 2,6 ' vs. alpha 2,3 ' sialic acid linkage served as a model trisaccharide template. Boronate chemistry was employed in combination with a library of imidazolium-based monomers targeting the carboxylate group of sialic acid. The influence of counterions of the cationic monomers and template on their interactions was investigated by means of H-1 NMR titration studies. The highest affinities were afforded using a combination of Br- and Na+ counterions of the monomers and template, respectively. The boronate ester formation was confirmed by MS and H-1/B-11 NMR, indicating 1 : 2 stoichiometries between sialyllactoses and boronic acid monomer. Polymers were synthesized in the form of microparticles using boronate and imidazolium monomers. This combinatorial approach afforded MIPs selective for the sialic acid linkages and compatible with an aqueous environment. The molecular recognition properties with respect to saccharide templates and glycosylated targets were reported.
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| 12. |
- Nicholls, Ian A., et al.
(författare)
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The Use of Computational Methods for the Development of Molecularly Imprinted Polymers
- 2021
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Ingår i: Polymers. - : MDPI. - 2073-4360. ; 13:17
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Forskningsöversikt (refereegranskat)abstract
- Recent years have witnessed a dramatic increase in the use of theoretical and computational approaches in the study and development of molecular imprinting systems. These tools are being used to either improve understanding of the mechanisms underlying the function of molecular imprinting systems or for the design of new systems. Here, we present an overview of the literature describing the application of theoretical and computational techniques to the different stages of the molecular imprinting process (pre-polymerization mixture, polymerization process and ligand-molecularly imprinted polymer rebinding), along with an analysis of trends within and the current status of this aspect of the molecular imprinting field.
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| 13. |
- Nicholls, Ian A., et al.
(författare)
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Towards Peptide and Protein Recognition by Antibody Mimicking Synthetic Polymers – Background, State of the Art, and Future Outlook
- 2020
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Ingår i: Australian journal of chemistry (Print). - : CSIRO Publishing. - 0004-9425 .- 1445-0038. ; 73:4, s. 300-306
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Forskningsöversikt (refereegranskat)abstract
- Antibody–peptide/protein interactions are instrumental for many processes in the pharmaceutical and biotechnology industries and as tools for biomedical and biochemical research. The recent development of molecularly imprinted polymer nanoparticles displaying antibody-like recognition of peptides and proteins offers the possibility for substituting antibodies with these robust materials for applications where the structural integrity and function of antibodies is compromised by temperature, pH, solvent, etc. The background to the development of this class of antibody-mimicking material and the state-of-the-art in their synthesis and application is presented in this review.
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| 14. |
- Olsson, Gustaf D., et al.
(författare)
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Using Molecular Dynamics in the Study of Molecularly Imprinted Polymers
- 2021
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Ingår i: Molecularly Imprinted Polymers. - New York, NY : Humana Press. - 9781071616284 - 9781071616291 ; , s. 241-268
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Bokkapitel (refereegranskat)abstract
- Molecular dynamics (MD) simulations of prepolymerization mixtures can provide detailed insights concerning the molecular-level mechanisms underlying the performance of molecularly imprinted polymers (MIPs) and can be used for the in silico screening of candidate polymer systems. Here, we describe the use of MD simulations of all-atom, all-component MIP prepolymerization mixtures and procedures for the evaluation of the simulation data using the Amber simulation software suite.
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| 16. |
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