Effect of Membrane Curvature Nanoarchitectonics on Membrane-Disruptive Interactions of Antimicrobial Lipids and Surfactants

Abstract

Single-chain lipid amphiphiles such as fatty acids and monoglycerides along with structurally related surfactants have received significant attention as membranedisrupting antimicrobials to inhibit bacteria and viruses. Such promise has motivated deeper exploration of how these compounds disrupt phospholipid membranes, and the membrane-mimicking, supported lipid bilayer (SLB) platform has provided a useful model system to evaluate corresponding mechanisms of action and potency levels. Even so, it remains largely unknown how biologically relevant membrane properties, such as sub-100 nm membrane curvature, might affect these membrane-disruptive interactions, especially from a nanoarchitectonics perspective. Herein, using the quartz crystal microbalancedissipation (QCM-D) technique, we fabricated intact vesicle adlayers composed of different-size vesicles (70 or 120 nm diameter) with varying degrees of membrane curvature on a titanium oxide surface and tracked changes in vesicle adlayer properties upon adding lauric acid (LA), glycerol monolaurate (GML), or sodium dodecyl sulfate (SDS). Above their critical micelle concentration (CMC) values, LA and GML caused QCM-D measurement shifts associated with tubule-and bud-like formation, respectively, and both compounds interacted similarly with small (high curvature) and large (low curvature) vesicles. In marked contrast, SDS exhibited distinct interactions with small and large vesicles. For large vesicles, SDS caused nearly complete membrane solubilization in a CMC-independent manner, whereas SDS was largely ineffective at solubilizing small vesicles at all tested concentrations. We rationalize these experimental observations by taking into account the interplay of the headgroup properties of LA, GML, and SDS and curvature-induced membrane geometry, and our findings demonstrate that membrane curvature nanoarchitectonics can strongly influence the membrane interaction profiles of antimicrobial lipids and surfactants.

Mechanistic Evaluation of Antimicrobial Lipid Interactions with Tethered Lipid Bilayers by Electrochemical Impedance Spectroscopy

“…Moreover, the tBLM platform has a higher degree of structural flexibility (i.e., less confined geometry) compared to previously used confined SLB platforms, which allowed us to distinguish the irreversible and reversible membrane damaging effects caused by GML and LA micelles, respectively. Moreover, SDS was observed to cause distinct types of membrane-disruptive behavior above and below its CMC, which is also in line with recent findings that the membrane-disruptive properties of SDS depend on the membrane nanoarchitecture [ 52 ]. Together, these findings demonstrate that the EIS technique is useful for evaluating the mechanistic details of how antimicrobial lipids and surfactants interact with the tBLM platform and such capabilities can be utilized to further screen and optimize the membrane-disruptive performance of candidate lipids and surfactants in future work.…”

Porous carbon nanoarchitectonics for the environment: detection and adsorption

“…[61][62][63][64] The environmental field is one of the promising applications. Sensing hazardous substances, 65,66 their removal, 67,68 and bio-related care 69,70 are also targets of nanoarchitectonics.…”

“…[189][190][191] Among a variety of sources, i.e., urea, glucose, ethylene glycol, glycerol, xylitol, melamine, and FA, they found glucose as the most promising secondary source because of its capability of reducing the loss of N-species from the ZIFs by pre-melting and in situ polymerization during the carbonization. 69 Although metal-free porous carbons could be obtained by the carbonization of a simple mixture of MOF and secondary component (Fig. 5a), the porosity, homogeneity, and coherency in the morphology was rather inferior than the wet-impregnation method.…”

Molecular Machines and Microrobots: Nanoarchitectonics Developments and On-Water Performances

“…It can be likened to the Theory of Everything in the world of physics [ 63 ], and can be called the Method for Everything in materials science [ 64 ]. In fact, the concept of nanoarchitectonics is used in fundamental areas such as fabrication and control of materials [ 65 , 66 , 67 ], micro/nano-structure organization [ 68 , 69 , 70 ], understanding of physical phenomena [ 71 , 72 , 73 ], and pursuit of basic biological and biochemical functions [ 74 , 75 , 76 ], as well as application-oriented fields such as catalysis [ 77 , 78 , 79 ], sensors [ 80 , 81 , 82 ], devices [ 83 , 84 , 85 ], energy-related applications [ 86 , 87 , 88 ], environment-related applications [ 89 , 90 , 91 ], and biomedical applications [ 92 , 93 , 94 ].…”