Ion-Specific Modulation of Interfacial Interaction Potentials between Solid Substrates and Cell-Sized Particles Mediated via Zwitterionic, Super-Hydrophilic Poly(sulfobetaine) Brushes

Higaki, Yasuki; Fröhlich, Benjamin; Yamamoto, Akihisa; Murakami, Ryo; Kaneko, Makoto; Takahara, Atsushi; Tanaka, Motomu

doi:10.1021/acs.jpcb.6b11540

Cited by 19 publications

(23 citation statements)

References 37 publications

(64 reference statements)

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“…71−73 However, timeresolved in situ NR measurements, using the time-of-flight method with a powerful wide-wavelength band pulsed neutron beam, are valid for the tracking of structure evolution of soft interfaces in response to the environment. 74,75 Some timeresolved NR measurements have already been applied for the investigation of the structure evolution process of polymer films. 74,76 We foresee that the insights obtained by our research are valuable in the design of materials covered with polyzwitterion brushes tailored to medical products.…”

Section: ■ Conclusion and Perspectivementioning

confidence: 99%

Hydration State Variation of Polyzwitterion Brushes through Interplay with Ions

Higaki

Kobayashi

Takahara³

2020

Langmuir

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Polyzwitterions have emerged as a new class of antifouling materials alternating poly(ethylene glycol). The exemplary biopassivation and lubrication behaviors are often attributed to the particular chemical structure of zwitterions, which involve a large dipole moment of the charged groups and a neutral net charge, while the hydration state and dynamics also associate with these characteristics. Polymer brushes composed of surface-tethered polyzwitterion chains produced by surface-initiated controlled radical polymerization have been developed as thin films which exhibit excellent antifouling and lubrication properties. In past decades, numerous studies have been devoted to examining the structure and dynamics of polyzwitterion brush chains in aqueous solutions. This feature article provides an overview of recent studies exploring the hydration state of polyzwitterion brushes with specular neutron reflectivity, highlights some newly published work on the nonuniform equilibrium structure, ion concentration dependence, ion specificity, and the effects of charge spacer length in the zwitterions, and discusses future perspective in this field.

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Section: ■ Conclusion and Perspectivementioning

confidence: 99%

Hydration State Variation of Polyzwitterion Brushes through Interplay with Ions

Higaki

Kobayashi

Takahara³

2020

Langmuir

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“…Polyzwitterionic brushes contain both positive and negative charges, and as with polyanionic or polycationic brushes, the strong affinity of these charged groups for water leads to superhydrophilic films that are attractive as antifouling coatings. − Nevertheless, the strong inter- and intramolecular associations between opposite charges in polyzwitterionic brushes lead to unusual trends in swelling. For example, in contrast to polyanionic or polycationic films, poly(sulfobetaine methacrylate) (PSBMA) brushes show enhanced swelling in aqueous solutions with increasing ionic strength. − …”

Section: Introductionmentioning

confidence: 99%

Aqueous Swelling of Zwitterionic Poly(sulfobetaine methacrylate) Brushes in the Presence of Ionic Surfactants

Yang

Zhang

Tarabara³

et al. 2018

Macromolecules

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Superhydrophilic polyzwitterionic brushes resist fouling, but free ions may screen zwitterion charges and alter brush hydration. This work examines the effect of ionic surfactants on polyzwitterionic brush swelling. In situ ellipsometry shows that the swelling of poly[2-(methacryloyloxy)ethyldimethyl-(3-sulfopropyl)ammonium hydroxide] (PMEDSAH) brushes depends on surfactant charge and concentration as well as film thickness. Solutions containing ≥6 mM sodium dodecyl sulfate (SDS) increase the swollen thicknesses of PMEDSAH brushes 2-to 9-fold with respect to thicknesses in water, and increases in swelling are especially high (6-to 9-fold) for thin films. Surfactant adsorption likely breaks ionic cross-links in brushes to enhance swelling, and immersion of brushes in 500 mM NaCl also leads to extensive swelling. Fitting of in situ ellipsometry data suggests that highly swollen films consist of a relatively dense, collapsed base layer covered by dilute brushes that contain about 98% water. At 10 or 20 mM surfactant concentrations, dodecyltrimethylammonium bromide (DTAB) yields much smaller increases in swelling than SDS, presumably because of the hydrophobicity of DTAB. Fluxes through PMEDSAH-modified microfiltration membranes are higher with 2 mM DTAB than with 6 mM SDS, consistent with the higher swelling of thin PMEDSAH brushes in the SDS solution.

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“…As described the previous section, it is still challanging to deal with ion specific interactions of charged polymers. For example, Wang et al reported the anion-specific changes in conformation and protein repellency for poly-sulfobetaine follow Hofmeister series (Wang et al, 2013), while Higaki et al suggested that the dependence of effective interaction potentials on cations cannot be explained by this framework (Higaki et al, 2017). It also seems plausible that the conformational fluctuation of molecules entropically repells proteins and cells from the surface.…”

Section: Toward Rational Design Of New Materials: Bioinertnessmentioning

confidence: 99%

Interplays of Interfacial Forces Modulate Structure and Function of Soft and Biological Matters in Aquatic Environments

Tanaka

2020

Front. Chem.

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Water had been considered as a passive matrix that merely fills up the space, supporting the diffusion of solute molecules. In the past several decades, a number of studies have demonstrated that water play vital roles in regulating structural orders of biological systems over several orders of magnitude. Water molecules take versatile structures, many of which are transient. Water molecules act as hydrogen bond donors as well as acceptors and biochemical reactions utilize water molecules as nucleophiles. Needless to say, the same principle holds for the synthetic materials that function under water: the conformation, dynamics and functions of molecules are significantly influenced by the surrounding water. This review sheds light on how the structure and function of soft and biological matter in aquatic environments are modulated by the orchestration of various interfacial forces.

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Ion-Specific Modulation of Interfacial Interaction Potentials between Solid Substrates and Cell-Sized Particles Mediated via Zwitterionic, Super-Hydrophilic Poly(sulfobetaine) Brushes

Cited by 19 publications

References 37 publications

Hydration State Variation of Polyzwitterion Brushes through Interplay with Ions

Hydration State Variation of Polyzwitterion Brushes through Interplay with Ions

Aqueous Swelling of Zwitterionic Poly(sulfobetaine methacrylate) Brushes in the Presence of Ionic Surfactants

Interplays of Interfacial Forces Modulate Structure and Function of Soft and Biological Matters in Aquatic Environments

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