Multivalent counterions diminish the lubricity of polyelectrolyte brushes

Yu, Jing; Jackson, Nicholas E.; Xu, Xin; Morgenstern, Yakov; Kaufman, Yair; Ruths, Marina; Pablo, Juan; Tirrell, Matthew

doi:10.1126/science.aar5877

Cited by 161 publications

(147 citation statements)

References 39 publications

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“…[19] To delve into how H 2 O molecule coordinates via Hbonding with PIL in SPPMs, we conducted proton nuclear magnetic resonance ( 1 H NMR) experiments for SPPM samples in different solvent environments. Taking SPPM-1 for example, the blue line in Figure 2 e displays its 1…”

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confidence: 99%

Crosslinking of a Single Poly(ionic liquid) by Water into Porous Supramolecular Membranes

Shao

Wang

et al. 2020

Angew Chem Int Ed

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Reversible regulation of membrane microstructures via non‐covalent interactions is of considerable interest yet remains a challenge. Herein, we discover a general one‐step approach to fabricate supramolecular porous polyelectrolyte membranes (SPPMs) from a single poly(ionic liquid) (PIL). The experimental results and theoretical simulation suggested that SPPMs were formed by a hydrogen‐bond‐induced phase separation of a PIL between its polar and apolar domains, which were linked together by water molecules. This unique feature was capable of modulating microscopic porous architectures and thus the global mechanical property of SPPMs by a rational design of the molecular structure of PILs. Such SPPMs could switch porosity upon thermal stimuli, as exemplified by dynamically adaptive transparency to thermal fluctuation. This finding provides fascinating opportunities for creating multifunctional SPPMs.

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confidence: 99%

Crosslinking of a Single Poly(ionic liquid) by Water into Porous Supramolecular Membranes

Shao

Wang

et al. 2020

Angew Chem Int Ed

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“…An interesting system to investigate with respect to their sensitivity to charges are polyelectrolyte brushes due to their intriguing surface geometry. Yu et al [30] studied the effect of multivalent ions on the lubricity of polystyrene sulfonate brushes. Even small concentrations of multivalent cations such as Y 3 + , Ba 2 + and Ca 2 + were found to strongly increase the friction between layers of the brush polyelectrolyte due to cation bridging effects.…”

Section: Other Interfacesmentioning

confidence: 99%

“…Even small concentrations of multivalent cations such as Y 3 + , Ba 2 + and Ca 2 + were found to strongly increase the friction between layers of the brush polyelectrolyte due to cation bridging effects. Yu et al [30] underline the significant effect of multivalent counterions on the lubricating properties of polyelectrolyte brushes, stressing the importance of this effect for applications such as biomedical devices.…”

Section: Other Interfacesmentioning

confidence: 99%

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Multivalent ions and biomolecules: Attempting a comprehensive perspective

2020

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Ions are ubiquitous in nature. They play a key role for many biological processes on the molecular scale, from molecular interactions, to mechanical properties, to folding, to self‐organisation and assembly, to reaction equilibria, to signalling, to energy and material transport, to recognition etc. Going beyond monovalent ions to multivalent ions, the effects of the ions are frequently not only stronger (due to the obviously higher charge), but qualitatively different. A typical example is the process of binding of multivalent ions, such as Ca2+, to a macromolecule and the consequences of this ion binding such as compaction, collapse, potential charge inversion and precipitation of the macromolecule. Here we review these effects and phenomena induced by multivalent ions for biological (macro)molecules, from the “atomistic/molecular” local picture of (potentially specific) interactions to the more global picture of phase behaviour including, e. g., crystallisation, phase separation, oligomerisation etc. Rather than attempting an encyclopedic list of systems, we rather aim for an embracing discussion using typical case studies. We try to cover predominantly three main classes: proteins, nucleic acids, and amphiphilic molecules including interface effects. We do not cover in detail, but make some comparisons to, ion channels, colloidal systems, and synthetic polymers. While there are obvious differences in the behaviour of, and the relevance of multivalent ions for, the three main classes of systems, we also point out analogies. Our attempt of a comprehensive discussion is guided by the idea that there are not only important differences and specific phenomena with regard to the effects of multivalent ions on the main systems, but also important similarities. We hope to bridge physico‐chemical mechanisms, concepts of soft matter, and biological observations and connect the different communities further.

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“…For planar polyelectrolyte brushes of poly(styrenesulfonate) in contact with solutions containing trivalent ions, the observed structures (both from the MD simulations and AFM) strongly resemble those predicted for polymer and polyelectrolyte brushes in poor solvents, and were rationalized by the ability of multivalent ions to form intrachain and interchain bridges as well as nearest neighbor condensation [ 143 ]. Multivalent ions were also found to have a strong impact on the lubricating properties of opposing polyelectrolyte brushes sliding against each other [ 144 ].…”

Section: Applicationsmentioning

confidence: 99%

Theoretical Modeling of Chemical Equilibrium in Weak Polyelectrolyte Layers on Curved Nanosystems

et al. 2020

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Surface functionalization with end-tethered weak polyelectrolytes (PE) is a versatile way to modify and control surface properties, given their ability to alter their degree of charge depending on external cues like pH and salt concentration. Weak PEs find usage in a wide range of applications, from colloidal stabilization, lubrication, adhesion, wetting to biomedical applications such as drug delivery and theranostics applications. They are also ubiquitous in many biological systems. Here, we present an overview of some of the main theoretical methods that we consider key in the field of weak PE at interfaces. Several applications involving engineered nanoparticles, synthetic and biological nanopores, as well as biological macromolecules are discussed to illustrate the salient features of systems involving weak PE near an interface or under (nano)confinement. The key feature is that by confining weak PEs near an interface the degree of charge is different from what would be expected in solution. This is the result of the strong coupling between structural organization of weak PE and its chemical state. The responsiveness of engineered and biological nanomaterials comprising weak PE combined with an adequate level of modeling can provide the keys to a rational design of smart nanosystems.

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Multivalent counterions diminish the lubricity of polyelectrolyte brushes

Cited by 161 publications

References 39 publications

Crosslinking of a Single Poly(ionic liquid) by Water into Porous Supramolecular Membranes

Crosslinking of a Single Poly(ionic liquid) by Water into Porous Supramolecular Membranes

Multivalent ions and biomolecules: Attempting a comprehensive perspective

Theoretical Modeling of Chemical Equilibrium in Weak Polyelectrolyte Layers on Curved Nanosystems

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