Structure of DPPC–hyaluronan interfacial layers – effects of molecular weight and ion composition

Wieland, D. C. Florian; Degen, Patrick; Zander, Thomas; Gayer, Sören; Raj, Akanksha; An, Junxue; Dédinaité, Andra; Claesson, Per M.; Willumeit‐Römer, Regine

doi:10.1039/c5sm01708d

Cited by 37 publications

(38 citation statements)

References 44 publications

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“…The HA-PL interactions in SF has been shown to be an important factor in lubrication of AC system [2,[25][26][27][28]. Shorter chains, create more H-bonds with nearest neighbours atoms and this contributes to higher sti®ness in these chains, and in-°u ence its persistence length from its normal value [29,30].…”

Section: Discussionmentioning

confidence: 99%

Hyaluronic Acid Dynamics and its Interaction with Synovial Fluid Components as a Source of the Color Noise

Siódmiak

Bełdowski

2019

Fluct. Noise Lett.

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This work presents the process of physical crosslinking of hyaluronic acid (HA) in the presence of phospholipids (PL) as applied to the lubrication in articular cartilage system. Three time scales of the process have been studied using Molecular Dynamics simulation: 2[Formula: see text]ps, 200[Formula: see text]ps and 20[Formula: see text]ns. The simulations were carried out for long and short chains of HA in the presence and in the absence of PL. We show that in contrast to the macroscopic thermal (white) noise, the short-time noise on the molecular scale has the properties of color noise with the power spectrum distribution proportional to the inverse of frequency, [Formula: see text]. The long-time simulations are characterized by a power spectrum similar to that of white noise.

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Section: Discussionmentioning

confidence: 99%

Hyaluronic Acid Dynamics and its Interaction with Synovial Fluid Components as a Source of the Color Noise

Siódmiak

Bełdowski

2019

Fluct. Noise Lett.

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“…Only large HA chains exhibit the simultaneous capability to crosslink through intra- and inter-chain hydrophobic centers and to absorb to PL head groups that form surface-active complexes. Such hydrophobic and electrostatic phenomena are notable with DPPC [ 25 , 41 ]. An additional consequence of HA globalization secondary to increasing PL concentration is the worsening of synovial fluid viscoelastic properties [ 42 ], further reflecting system dysfunction.…”

Section: Discussionmentioning

confidence: 99%

Molecular Dynamic Analysis of Hyaluronic Acid and Phospholipid Interaction in Tribological Surgical Adjuvant Design for Osteoarthritis

Siódmiak

Bełdowski

Augé³

et al. 2017

Molecules

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Tribological surgical adjuvants constitute a therapeutic discipline made possible by surgical advances in the treatment of damaged articular cartilage beyond palliative care. The purpose of this study is to analyze interactions between hyaluronic acid and phospholipid molecules, and the formation of geometric forms, that play a role in the facilitated lubrication of synovial joint organ systems. The analysis includes an evaluation of the pathologic state to detail conditions that may be encountered by adjuvants during surgical convalescence. The synovial fluid changes in pH, hyaluronic acid polydispersity, and phospholipid concentration associated with osteoarthritis are presented as features that influence the lubricating properties of adjuvant candidates. Molecular dynamic simulation studies are presented, and the Rouse model is deployed, to rationalize low molecular weight hyaluronic acid behavior in an osteoarthritic environment of increased pH and phospholipid concentration. The results indicate that the hyaluronic acid radius of gyration time evolution is both pH- and phospholipid concentration-dependent. Specifically, dipalmitoylphosphatidylcholine induces hydrophobic interactions in the system, causing low molecular weight hyaluronic acid to shrink and at high concentration be absorbed into phospholipid vesicles. Low molecular weight hyaluronic acid appears to be insufficient for use as a tribological surgical adjuvant because an increased pH and phospholipid concentration induces decreased crosslinking that prevents the formation of supramolecular lubricating forms. Dipalmitoylphosphatidylcholine remains an adjuvant candidate for certain clinical situations. The need to reconcile osteoarthritic phenotypes is a prerequisite that should serve as a framework for future adjuvant design and subsequent tribological testing.

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“…9), although the surface is not covered homogenously, as revealed from BAM (Fig. 11) (Wieland et al, 2016).…”

Section: X-ray Reflectometry (Xrr) and Brewster Angle Microscopy (Bam)mentioning

confidence: 92%

New Approach to Structure–Property Correlations of Different Films of Sorbitan Esters and Their Self‐Assembly into Viscoelastic Monolayers

Demand

Egger

Degen

et al. 2019

J Surfact & Detergents

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This publication is focused on the structural origin of viscoelasticity in Langmuir monolayers. To improve the understanding of the structural origin of viscoelasticity of surfactant films, we systematically studied interfacial films of different sorbitan esters with saturated (Span 60 and 65) and unsaturated (Span 80 and 85) paraffin chains by means of surface rheology, Langmuir isotherms, X‐ray reflectometry (XRR), and Brewster angle microscopy (BAM). The results of two‐dimensional shear rheological measurements revealed the existence of temporarily cross‐linked networks. In dynamic BAM experiments, we observed a swinging motion of the monolayers as a result of a sudden externally initiated mechanical perturbation. The viscoelastic film response, which relaxed with time as the external force vanished, could be traced back to the presence of foam‐like supramolecular structures that interlinked solid‐condensed domains. The temperature dependence of the elastic response implied that the solid domains decomposed at temperatures close to the bulk melting point of Span 60 and Span 65. We concluded that insoluble surfactants formed solid domains at the interface, which were linked with each other by nonsolid areas, giving viscoelastic films. These newly discovered insights into coherent film formations could provide new opportunities for designing mechanically stable surfactant interfaces.

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Structure of DPPC–hyaluronan interfacial layers – effects of molecular weight and ion composition

Cited by 37 publications

References 44 publications

Hyaluronic Acid Dynamics and its Interaction with Synovial Fluid Components as a Source of the Color Noise

Hyaluronic Acid Dynamics and its Interaction with Synovial Fluid Components as a Source of the Color Noise

Molecular Dynamic Analysis of Hyaluronic Acid and Phospholipid Interaction in Tribological Surgical Adjuvant Design for Osteoarthritis

New Approach to Structure–Property Correlations of Different Films of Sorbitan Esters and Their Self‐Assembly into Viscoelastic Monolayers

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