Multivalent non-covalent interactions lead to strongest polymer adhesion

Lallemang, Max; Yu, Leixiao; Cai, Wanhao; Rischka, Klaus; Hartwig, Andreas; Haag, Rainer; Hugel, Thorsten; Balzer, Bizan N.

doi:10.1039/d1nr08338d

Cited by 16 publications

(14 citation statements)

References 66 publications

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“…Here, synergistic combinations of several cooperative binding events allow one to compensate for weak individual noncovalent interactions . Multivalent binding is thus significantly more resilient than individual bonds between the equivalent number of monovalent ligands and can drastically enhance the binding affinity between interacting species. , Unlike covalent bonds, multivalent noncovalent interactions are also fully reversible through the sequential dissociation of individual bonds, rendering the respective physiological interactions highly dynamic . Consequently, multivalency plays a key role in many biological processes involving interactions between biomacromolecules, between cells, or between cells and bacteria or viruses, including Sars-CoV-2. − Likewise, lectins, as carbohydrate-binding proteins that mediate attachment and binding of the latter, have been successfully targeted by multivalent oligosaccharides or dendrimeric models thereof. ,,− However, all these proteins possess well-defined tightly folded surfaces; addressing flexibles loops or conformationally ill-defined protein substructures and dynamic domains poses a much greater challenge.…”

Section: Introductionmentioning

confidence: 99%

“…30 Multivalent binding is thus significantly more resilient than individual bonds between the equivalent number of monovalent ligands and can drastically enhance the binding affinity between interacting species. 31,32 Unlike covalent bonds, multivalent noncovalent interactions are also fully reversible through the sequential dissociation of individual bonds, rendering the respective physiological interactions highly dynamic. 33 Consequently, multivalency plays a key role in many biological processes involving interactions between biomacromolecules, between cells, or between cells and bacteria or viruses, including Sars-CoV-2.…”

Section: ■ Introductionmentioning

confidence: 99%

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Recognition of a Flexible Protein Loop in Taspase 1 by Multivalent Supramolecular Tweezers

et al. 2022

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Many natural proteins contain flexible loops utilizing well-defined complementary surface regions of their interacting partners and usually undergo major structural rearrangements to allow perfect binding. The molecular recognition of such flexible structures is still highly challenging due to the inherent conformational dynamics. Notably, protein–protein interactions are on the other hand characterized by a multivalent display of complementary binding partners to enhance molecular affinity and specificity. Imitating this natural concept, we here report the rational design of advanced multivalent supramolecular tweezers that allow addressing two lysine and arginine clusters on a flexible protein surface loop. The protease Taspase 1, which is involved in cancer development, carries a basic bipartite nuclear localization signal (NLS) and thus interacts with Importin α, a prerequisite for proteolytic activation. Newly established synthesis routes enabled us to covalently fuse several tweezer molecules into multivalent NLS ligands. The resulting bi- up to pentavalent constructs were then systematically compared in comprehensive biochemical assays. In this series, the stepwise increase in valency was robustly reflected by the ligands’ gradually enhanced potency to disrupt the interaction of Taspase 1 with Importin α, correlated with both higher binding affinity and inhibition of proteolytic activity.

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Section: Introductionmentioning

confidence: 99%

Section: ■ Introductionmentioning

confidence: 99%

Recognition of a Flexible Protein Loop in Taspase 1 by Multivalent Supramolecular Tweezers

et al. 2022

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“…The increased stability and adhesive strength of molecules tethered via multiple noncovalent bonds has been shown by several studies. 68,69 One of the first macroinitiators for surface-initiated radical polymerization was developed by Stoḧr and Ruḧe. 70 The macroinitiator was a monolayer of poly(ε-caprolactone) with covalently bound azo groups that were incorporated in the polymer backbone.…”

Section: Macroinitiatorsmentioning

confidence: 99%

Supramolecular Polymer Brushes

Metze

Klok

2023

ACS Polym. Au

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Polymer brushes are thin polymer films that consist of densely grafted, chain-end tethered polymers. These thin polymer films can be produced either by anchoring presynthesized chain-end functional polymers to the surface of interest (“grafting to”), or by using appropriately modified surfaces to facilitate growth of polymer chains from the substrate (“grafting from”). The vast majority of polymer brushes that have been prepared and studied so far involved chain-end tethered polymer assemblies that are anchored to the surface via covalent bonds. In contrast, the use of noncovalent interactions to prepare chain-end tethered polymer thin films is much less explored. Anchoring or growing polymer chains using noncovalent interactions results in supramolecular polymer brushes. Supramolecular polymer brushes may possess unique chain dynamics as opposed to their covalently tethered counterparts, which could provide avenues to, for example, renewable or (self-)healable surface coatings. This Perspective article provides an overview of the various approaches that have been used so far to prepare supramolecular polymer brushes. After presenting an overview of the various approaches that have been used to prepare supramolecular brushes via the “grafting to” strategy, examples will be presented of strategies that have been successfully applied to produce supramolecular polymer brushes via “grafting from” methods.

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“…TiO 2 substrate is prepared as reported in the literature. 46 The glass substrates are cleaned as follows: rstly, they are cleaned ultrasonically for 10 min with H 2 O and methanol and respectively. Secondly, they are immersed in RCA solution at 60 C for 1 hour.…”

Section: Materials and Sample Preparationmentioning

confidence: 99%

Angle-dependent strength of a single chemical bond by stereographic force spectroscopy

et al. 2022

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Multivalent non-covalent interactions lead to strongest polymer adhesion

Abstract: Multivalent interactions are quantified using AFM-based single molecule force spectroscopy showing that non-covalent interactions are ideal candidates to mediate robust adhesion.

Cited by 16 publications

References 66 publications

Recognition of a Flexible Protein Loop in Taspase 1 by Multivalent Supramolecular Tweezers

Recognition of a Flexible Protein Loop in Taspase 1 by Multivalent Supramolecular Tweezers

Supramolecular Polymer Brushes

Angle-dependent strength of a single chemical bond by stereographic force spectroscopy

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