Surface plasmon &amp; visible light for polymer functionalization of mesopores and manipulation of ionic permselectivity

Herzog, Nicole; Kind, Jonas; Heß, Christian; Andrieu‐Brunsen, Annette

doi:10.1039/c5cc03507d

Cited by 18 publications

(28 citation statements)

References 26 publications

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“…The authors acknowledge funding from the Hessen State Ministry of Higher Education, Research and the Arts, Germany, in the frame of the Small 2019, 15, 1902710…”

Section: Acknowledgementsmentioning

confidence: 99%

“…The anionic probe molecule [Fe(CN) 6 ] 3−/4− is excluded at basic pH as expected due to electrostatic repulsion resulting from the deprotonated mesopore wall silanol groups together with the pore diameters within the Debye Screening length. After modification with homo oligomers (Figure a for PDMAEMA and Figure b for PMEP) mesoporous silica films show inaccessible pores for the probe molecule being identically charged to the pore wall‐grafted monomers which is in accordance to corresponding literature studies 6c,15. For the homo‐oligomer modification we choose the same polymerization conditions as for the corresponding blocks of the PDMAEMA‐ b ‐PMEP block‐co‐oligomer.…”

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confidence: 91%

“…Comparing the maximum peak current density of PDMAEMAbPMEP block cooligomer functionalized mesopores in the absence of cal cium (Figure 4b spheres, Figure 2d) this is much lower as for purely PDMAEMA functionalized pores under identical condi tions (acidic pH, Figure 2a red). Upon addition of calcium ions to PDMAEMAbPMEP blockcooligomer functionalized mesopores with a pore filling degree of ≈95 vol% (Figure 4b, red star, pH 2) the pore accessibility and thus the measured Small 2019, 15,1902710 maximum peak current density increases by 200 µA cm −2 cor responding to a factor of 1.6-2 and reaches values of ≈535 µA cm −2 comparable to purely PDMAEMA functionalized mesopores with a pore filling degree of ≈80 vol%. This fully inversed transport behavior of the blockcooligomer functional ized mesopores compared to homooligomer functionalized mesopores demonstrates the strong influence of the charge composition and chain architecture.…”

mentioning

confidence: 99%

“…This blockcooligomer chain ratio of 1:1 is important because it allows to generate an identical number of positive and negative charges within the oligomer chain while charging the individual blocks especially up to a pH value of 7.5 referring to monomer solution pKa values. At pH values higher than 7.5, based on the solution Small 2019, 15,1902710 Figure 1. a) Scheme representing block-co-oligomer functionalization of mesoporous silica thin film which are investigated regarding their ionic permselectivity. The mesoporous silica film, displayed in the form of a TEM image, is directly supported on the ITO-coated glass substrate.…”

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confidence: 99%

“…To first validate the ionic permselectivity and gating properties of the PDMAEMAbPMEP blockcooligomer Small 2019, 15,1902710 6 ] 3−/4− is excluded at basic pH as expected due to electrostatic repulsion resulting from the deprotonated mesopore wall silanol groups together with the pore diameters within the Debye Screening length. After modification with homo oligomers (Figure 2a for PDMAEMA and Figure 2b for PMEP) mesoporous silica films show inaccessible pores for the probe molecule being identically charged to the pore wallgrafted monomers which is in accordance to corresponding literature studies.…”

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confidence: 99%

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Influence of Chain Architecture on Nanopore Accessibility in Polyelectrolyte Block‐Co‐Oligomer Functionalized Mesopores

Brilmayer

Heß

Andrieu‐Brunsen

2019

Small

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Functionalized ordered mesoporous silica materials are commonly investigated for applications such as drug release, sensing, and separation processes. Although, various homopolymer functionalized responsive mesopores are reported, little focus has been put on copolymers in mesopores. Mesoporous silica films are functionalized with responsive and orthogonally charged block‐co‐oligomers. Responsive 2‐dimethylamino)ethyl methacrylate)‐block‐2‐(methacryloyloxy)ethyl phosphate (DMAEMA‐b‐MEP) block‐co‐oligomers are introduced into mesoporous films using controlled photoiniferter initiated polymerization. This approach allows a very flexible charge composition design. The obtained block‐co‐oligomer functionalized mesopores show a complex gating behavior indicating a strong interplay between the different blocks emphasizing the strong influence of charge distribution inside mesopores on ionic pore accessibility. For example, in contrast to mesopores functionalized with zwitterionic polymers, DMAEMA‐b‐MEP block‐co‐oligomer functionalized mesopores, containing two oppositely charged blocks, do not show bipolar ion exclusion, demonstrating the influence of the chain architecture on mesopore accessibility. Furthermore, ligand binding–based selective gating is strongly influenced by this chain architecture as demonstrated by an expansion of pore accessibility states for block‐co‐oligomer functionalized mesopores as compared to the individual polyelectrolyte functionalization for calcium induced gating.

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“…The authors acknowledge funding from the Hessen State Ministry of Higher Education, Research and the Arts, Germany, in the frame of the Small 2019, 15, 1902710…”

Section: Acknowledgementsmentioning

confidence: 99%

mentioning

confidence: 91%

mentioning

confidence: 99%

mentioning

confidence: 99%

mentioning

confidence: 99%

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Influence of Chain Architecture on Nanopore Accessibility in Polyelectrolyte Block‐Co‐Oligomer Functionalized Mesopores

Brilmayer

Heß

Andrieu‐Brunsen

2019

Small

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Surface Plasmons and Visible Light Iniferter Initiated Polymerization for Nanolocal Functionalization of Mesoporous Separation Layers

John

Stanzel

Andrieu‐Brunsen

2021

Adv Funct Materials

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Although the technological relevance of mesoporous ceramic polymer hybrid materials is well accepted, missing functionalization concepts enabling 3D nanoscale local control of polymer placement into mesoporous materials, including thin films, and ideally using controlled polymerization techniques limit the application potential. Here, nanolocal functionalization of mesoporous separation layers using controlled, visible light iniferter initiated polymerization allowing responsive polymer functionalization locally limited to the irradiated spot is introduced. Thereby, two visible light sensitive iniferters, s-p-trimethoxysilylbenzyl-S´-dodecyltrithiocarbonate and 4-cyano-4-((dodecylsulfanylthiocarbonyl)sulfanyl)pentanoic acid, are developed for polymer functionalization of mesoporous films in a grafting from and a grafting through approach. 3D nanolocal polymer placement close to the proximity of the plasmonic field source is demonstrated by combining these visible light iniferter initiated polymerizations with optical near field modes, such as localized surface plasmon resonance (LSPR). As the location of the LSPR in mesoporous films can be controlled by placing metal alloy nanoparticles into these films and film thicknesses can be adjusted, this strategy is applied for precise positioning of polymers into mesoporous films with nanolocal control in three dimensions and thus reduces the gap in precision of functional group positioning between technological and biological nanopores.

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The Beginner's Guide to Chiral Plasmonics: Mostly Harmless Theory and the Design of Large‐Area Substrates

Goerlitzer

Puri

Moses

et al. 2021

Advanced Optical Materials

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Plasmonic effects in noble metal nanostructures are probably one of the most widely recognized forms of nanotechnology. The tremendous success and interdisciplinary use of plasmonic Chiral plasmonics is a fascinating research field that is attractive to scientists from diverse backgrounds. Physicists study light-matter interactions, chemists seek ways to analyze enantiomeric molecules, biologists study living objects, and material engineers focus on scalable production processes. Successful access to this emergent field for an interdisciplinary community depends on overcoming three main issues. First, understanding the physical background of chiral plasmonics requires proper introduction in easy language. Second, pitfalls in the characterization of chiroplasmonic features can prevent accurate interpretation. Third, simple and robust methods capable of covering macroscopic substrate areas must be available. This tutorial-style review addresses these issues with the goal to provide a comprehensive introduction into chiral plasmonic nanostructures. It starts with a brief introduction of the relevant physics involved in chiral light−matter interactions. A brief guide about how to adequately characterize samples follows. Subsequently, an overview of fabrication techniques that produce chiral substrates over large areas is given, and the strengths and weaknesses of the different approaches are discussed. The focus is on simple and robust processes that do not require clean room facilities and can be implemented by a much larger scientific audience.

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Surface plasmon & visible light for polymer functionalization of mesopores and manipulation of ionic permselectivity

Cited by 18 publications

References 26 publications

Influence of Chain Architecture on Nanopore Accessibility in Polyelectrolyte Block‐Co‐Oligomer Functionalized Mesopores

Influence of Chain Architecture on Nanopore Accessibility in Polyelectrolyte Block‐Co‐Oligomer Functionalized Mesopores

Surface Plasmons and Visible Light Iniferter Initiated Polymerization for Nanolocal Functionalization of Mesoporous Separation Layers

The Beginner's Guide to Chiral Plasmonics: Mostly Harmless Theory and the Design of Large‐Area Substrates

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