Molecular design principles of Lysine-DOPA wet adhesion

Abstract

The mussel byssus has long been a source of inspiration for the adhesion community. Recently, adhesive synergy between flanking lysine (Lys, K) and 3,4-Dihydroxyphenylalanine (DOPA, Y) residues in the mussel foot proteins (Mfps) has been highlighted. However, the complex topological relationship of DOPA and Lys as well as the interfacial adhesive roles of other amino acids have been understudied. Herein, we study adhesion of Lys and DOPAcontaining peptides to organic and inorganic substrates using single-molecule force spectroscopy (SMFS). We show that a modest increase in peptide length, from KY to (KY) 3 , increases adhesion strength to TiO 2. Surprisingly, further increase in peptide length offers no additional benefit. Additionally, comparison of adhesion of dipeptides containing Lys and either DOPA (KY) or phenylalanine (KF) shows that DOPA is stronger and more versatile. We furthermore demonstrate that incorporating a nonadhesive spacer between (KY) repeats can mimic the hidden length in the Mfp and act as an effective strategy to dissipate energy.

Genetically Engineered Polypeptide Adhesive Coacervates for Surgical Applications

“…[35,37] We speculate that the robust adhesion performance of K-NAT glues might be related to the presence of strong π-π stacking and cation-π interactions. [13,29,30,38] We also investigated photo-modulation of the adhesion performance by switching the azobenzene moiety from trans-to cis configuration. However, it turned out that the light irradiation with different wavelength didn't change the adhesion performance of the K-NAT adhesive.…”

Ultrahigh Adhesion Force Between Silica-Binding Peptide SB7 and Glass Substrate Studied by Single-Molecule Force Spectroscopy and Molecular Dynamic Simulation

“…Recently, a SMFS study on the dipeptide of lysine (Lys, K) and 3,4-Dihydroxyphenylalanine (DOPA, Y) residue, KY, also showed two distributions of adhesion force on TiO 2 at ∼100 pN and ∼ 600 pN, which is similar to our results of adhesion force of SB7 on silica. Substitution of DOPA with phenylalanine showed no detectable adhesion force on TiO 2 , suggesting that DOPA is responsible for the binding on TiO 2 (Li et al, 2020).…”

“…Traditional methods such as surface plasma resonance (SPR) and quartz crystal microbalance (QCM) have been used to study the binding strength and molecular mechanism of the adhesion of peptides and proteins on different substrates (Hellner et al, 2020). Atomic force microscope (AFM) based single-molecule force spectroscopy (SMFS) has been widely used as a powerful tool to study the protein dynamics (Ott et al, 2017b), nano-mechanics of polymers (Cai et al, 2019;Song et al, 2019;Bao et al, 2020), the mechanical strength of single chemical bonds (Xue et al, 2014;Huang et al, 2019), the interaction of ligandreceptor (Lei et al, 2017a;Ott et al, 2017b;Li and Zheng, 2018) and single-molecule adhesions (Li et al, 2014(Li et al, , 2020Maity et al, 2015;Pyles et al, 2019) with high force resolution. SMFS provides detailed information about peptidessurface interactions such as singe-molecule adhesion force that is not available with other techniques (Li et al, 2014(Li et al, , 2020Maity et al, 2015).…”

Perspective for a New Bioinspired Permanent Adhesive for dry Conditions - Insights in the Glue Producing Japanese art of Defence System of the Oita Salamander Hynobius dunni

“…3,4-dihydroxypheny-L-alanine (L-DOPA) is probably the bestcharacterized compound in the field of bioadhesion and it is prominent in the literature for its numerous novel biomimetic and adhesive-inspired applications (Hofman et al, 2018;Li et al, 2020;Kang et al, 2021). Thus far, L-DOPA has been confirmed in the glue of a few species, including bacteria (Alteromonas spp.)…”