Molecular recognition between membrane epitopes and nearly free surface silanols explains silica membranolytic activity

Pavan, Cristina; Sydor, Matthew J.; Bellomo, Chiara; Leinardi, Riccardo; Cananà, Stefania; Kendall, Rebekah L.; Rebba, Erica; Corno, Marta; Ugliengo, Piero; Mino, Lorenzo; Holian, Andrij; Turci, Francesco

doi:10.1016/j.colsurfb.2022.112625

Cited by 19 publications

(41 citation statements)

References 63 publications

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“…2758 cm − 1 , represented about 1.6% of total silanols for gQ-n1, 1.5% for gQ-n2, and 0.6% for gQ-n3. In general, the silanol pro les observed for the gQ-n samples were qualitatively similar to the pro les observed for the commercial quartz our (cQ-f) and for pyrogenic amorphous silica particles of similar size 11,12 .…”

Section: Nanoquartz Shows Nfs and Membranolytic Activitysupporting

confidence: 75%

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Preparation of fractured nanoquartz: surface features and cell membrane damage

Bellomo

Pavan

Fiore

et al. 2022

Preprint

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Occupational exposure to quartz dust is associated with fatal diseases. Quartz dusts generated by mechanical fracturing are characterized by a broad range of micrometric to nanometric particles. The contribution of this nanometric fraction to the overall toxicity of quartz is still largely unexplored, primarily because of the strong electrostatic adhesion forces that prevent isolation of the nano-fraction. Furthermore, fractured silica dust exhibits special surface features, namely Nearly Free Silanols (NFS), which impart membranolytic activity to quartz. Nanoquartz can be synthetized via bottom-up methods, but the surface chemistry of those crystals strongly differs from nanoparticles resulting from fracturing. We report here a top-down milling procedure to obtain a nanometric quartz that shares with fractured quartz the key surface properties relevant to toxicity. Ball milling was optimized by coupling dry and wet milling steps, using water as a dispersing agent, and varying milling times and rotational speeds. Nanoquartz with a strong tendency to form submicrometric agglomerates was obtained. Deagglomeration with surfactants or simulated body fluids was negligible. Partial lattice amorphization and bimodal crystallite domain size were observed. A moderate membranolytic activity, which correlated with the amount of NFS, signaled coherence with previous toxicological data. Membranolytic nanoquartz for toxicological investigations was obtained.

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Section: Nanoquartz Shows Nfs and Membranolytic Activitysupporting

confidence: 75%

“…To assess the membranolytic activity of the particles, red blood cells (RBCs) were used as simple model of non-phagocytic cells, using a protocol previously described 12,39 . Samples were dispersed at the initial concentration of 6 mg/ml in 10mM PBS and bath sonicated for 15 minutes (FALC instruments), just before testing.…”

Section: Membranolytic Activitymentioning

confidence: 99%

Preparation of fractured nanoquartz: surface features and cell membrane damage

Bellomo

Pavan

Fiore

et al. 2022

Preprint

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“…[ 15b,35 ] We recently demonstrated on silica that DOPC, but not DOPS, is irreversibly adsorbed, and this interaction specifically masks NFS, which are held responsible for silica membranolytic effect. [ 31 ] For kaolin, the involvement of the exposed outer OH in the interaction with DOPC was further confirmed by FT‐IR spectroscopy (Figure S4, Supporting Information).…”

Section: Resultsmentioning

confidence: 80%

“…DOPC can prevent membranolysis by masking the surface OH species, as it has been shown for silica particles. [ 16c,31 ] The hemolytic activity of K3 and B2, in presence of self‐assembled DOPC and DOPS structures is reported in Figure . DOPC and DOPS were used because they share the same apolar tail (i.e., octadecenoyl) and differentiate for the polar head.…”

Section: Resultsmentioning

confidence: 99%

“…Conversely, negatively‐charged DOPS structures of the same size as DOPC [ 31 ] did not alter the hemolytic activity of K3 and B2, revealing that DOPS likely does not interact with the surface of these two LS. Both K3 and B2 are negatively charged in the physiological milieu used for experiments (Figure 2c), due to deprotonated silanols and aluminols.…”

Section: Resultsmentioning

confidence: 99%

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Interaction of Layered Silicates with Biomembranes: Ion Exchangers and Non‐Exchangers

Cananà

Pavan

Bellomo

et al. 2022

Adv Materials Inter

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Layered silicates (LS, clays) are a composite group of minerals whose industrial interest and technological applications are progressively expanding, spanning from catalysis to biomedicine. However, the compatibility of LS with biological systems is not clear, and mechanistic data about biophysicochemical interactions at the interface of LS and biomembranes are scarce. Here, cell membrane damage, assessed using red blood cells as model membranes, is revealed for kaolin (> 75 wt.% kaolinite, 1:1 layer structure) and bentonite (> 90 wt.% montmorillonite, 1:2 layer structure) particles. The high membranolytic capacity of bentonite (i.e., high ion‐exchanger LS) is the result of the combined contribution of both mineral surface features and sample‐specific cation exchange capacity (CEC). For kaolin (i.e., non‐ion‐exchanger LS), the capacity to damage membranes is primarily due to surface hydroxyl species, that is, silanols and aluminols, exposed at the crystal lattice boundaries. When kaolin is thermally disorganized into amorphous metakaolin, membrane damage is driven by a specific sub‐population of surface hydroxyl species, namely the “nearly free silanols”, previously evidenced on quartz. This study establishes the rationale underlying the interactions between LS particles and membranes and can set the basis for the understanding of interfacial phenomena of LS.

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Key Role of Choline Head Groups in Large Unilamellar Phospholipid Vesicles for the Interaction with and Rupture by Silica Nanoparticles

Leibe

Fritsch‐Decker

Gußmann³

et al. 2023

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For highly abundant silica nanomaterials, detrimental effects on proteins and phospholipids are postulated as critical molecular initiating events that involve hydrogen‐bonding, hydrophobic, and/or hydrophilic interactions. Here, large unilamellar vesicles with various well‐defined phospholipid compositions are used as biomimetic models to recapitulate membranolysis, a process known to be induced by silica nanoparticles in human cells. Differential analysis of the dominant phospholipids determined in membranes of alveolar lung epithelial cells demonstrates that the quaternary ammonium head groups of phosphatidylcholine and sphingomyelin play a critical and dose‐dependent role in vesicle binding and rupture by amorphous colloidal silica nanoparticles. Surface modification by either protein adsorption or by covalent coupling of carboxyl groups suppresses the disintegration of these lipid vesicles, as well as membranolysis in human A549 lung epithelial cells by the silica nanoparticles. Furthermore, molecular modeling suggests a preferential affinity of silanol groups for choline head groups, which is also modulated by the pH value. Biomimetic lipid vesicles can thus be used to better understand specific phospholipid–nanoparticle interactions at the molecular level to support the rational design of safe advanced materials.

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Molecular recognition between membrane epitopes and nearly free surface silanols explains silica membranolytic activity

Cited by 19 publications

References 63 publications

Preparation of fractured nanoquartz: surface features and cell membrane damage

Preparation of fractured nanoquartz: surface features and cell membrane damage

Interaction of Layered Silicates with Biomembranes: Ion Exchangers and Non‐Exchangers

Key Role of Choline Head Groups in Large Unilamellar Phospholipid Vesicles for the Interaction with and Rupture by Silica Nanoparticles

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