Models of the Three-Component Bilayer of Stratum Corneum: A Molecular Simulation Study.

The construction of the stratum corneum (SC) is crucial to the problems of transdermal drug delivery. SC consists of the keratinocyte layers and the lipid matrix surrounding it. Among them, the lipid matrix is the barrier for many exogenous molecules, mainly composed of ceramides (CERs), free fatty acids (FFA), and cholesterol (CHOL). In this work, we developed single-component (CERs, CER-NS, and CER-EOS) and six three-component models, and each model was simulated by using the GROMOS-54A7 force field. Short-period phase (SPP) and long-period phase (LPP) systems were established separately, and area per lipid (APL), thickness, order of carbon chain (SCD), and density distribution were analyzed. The transition of CER-NS and CER-EOS in LPP was observed. The results of hydrogen bonds in the lipid systems indicated that a strong hydrogen-bond network was formed between the skin-lipid bilayers. Umbrella sampling method simulations were performed to calculate the free energy change of ethanol moving into the skin-lipid bilayer. The results revealed that ethanol molecules pulled some water molecules into the membrane when they passed through SPP-1. Our findings provided some insights and models of the stratum corneum that could be used for the subsequent mechanism of macromolecule permeation through membranes in drugs, cosmetics, and so on.

Atomistic Insights into the Influence of High Concentration H2O2/H2O on Al Nanoparticles Combustion: ReaxFF Molecules Dynamics Simulation.

The combination of Al nanoparticles (ANPs) as fuel and H2O2 as oxidizer is a potential green space propellant. In this research, reactive force field molecular dynamics (ReaxFF-MD) simulations were used to study the influence of water addition on the combustion of Al/H2O2. The MD results showed that as the percentage of H2O increased from 0 to 30%, the number of Al-O bonds on the ANPs decreased, the number of Al-H bonds increased, and the adiabatic flame temperature of the system decreased from 4612 K to 4380 K. Since the Al-O bond is more stable, as the simulation proceeds, the number of Al-O bonds will be significantly higher than that of Al-H and Al-OH bonds, and the Al oxides (Al[O]x) will be transformed from low to high coordination. Subsequently, the combustion mechanism of the Al/H2O2/H2O system was elaborated from an atomic perspective. Both H2O2 and H2O were adsorbed and chemically activated on the surface of ANPs, resulting in molecular decomposition into free radicals, which were then captured by ANPs. H2 molecules could be released from the ANPs, while O2 could not be released through this pathway. Finally, it was found that the coverage of the oxide layer reduced the rate of H2O2 consumption and H2 production significantly, simultaneously preventing the deformation of the Al clusters' morphology.

"All in One" Strategy for Achieving Superprotonic Conductivity by Incorporating Strong Acids into a Robust Imidazole-Linked Covalent Organic Framework.

The fabrication of solid-state proton-conducting electrolytes possessing both high performance and long-life reusability is significant but challenging. An "all-in-one" composite, H3PO4@PyTFB-1-SO3H, including imidazole, sulfonic acid, and phosphoric acid, which are essential for proton conduction, was successfully prepared by chemical post-modification and physical loading in the rationally pre-synthesized imidazole-based nanoporous covalent organic framework (COF), PyTFB-1. The resultant H3PO4@PyTFB-1-SO3H exhibits superhigh proton conductivity with its value even highly up to 1.15 × 10-1 S cm-1 at 353 K and 98% relative humidity (RH), making it one of the highest COF-based composites reported so far under the same conditions. Experimental studies and theoretical calculations further confirmed that the imidazole and sulfonic acid groups have strong interactions with the H3PO4 molecules and the synergistic effect of these three groups dramatically improves the proton conductivity properties of H3PO4@PyTFB-1-SO3H. This work demonstrated that by aggregating multiple proton carriers into one composite, effective proton-conducting electrolyte can be feasibly achieved.

Molecular insights into the adsorption and penetration of oil droplets on hydrophobic membrane in membrane distillation.

Membrane fouling induced by oily substances significantly constrains membrane distillation performance in treating hypersaline oily wastewater. Overcoming this challenge necessitates a heightened fundamental understanding of the oil fouling phenomenon. Herein, the adsorption and penetration mechanism of oil droplets on hydrophobic membranes in membrane distillation process was investigated at the molecular level. Our results demonstrated that the adsorption and penetration of oil droplets were divided into four stages, including the free stage, contact stage, spreading stage, and equilibrium stage. Due to the extensive non-polar surface distribution of the polytetrafluoroethylene (PTFE) membrane (comprising 95.41 %), the interaction between oil molecules and PTFE was primarily governed by van der Waals interaction. Continuous oil droplet membrane fouling model revealed that the new oil droplet molecules preferred to penetrate into membrane pores where oil droplets already existed. The penetration of resin (a component of medium-quality oil droplets) onto PTFE membrane pores required the "pre-paving" of light crude oil. Finally, the ΔE quantitative structure-activity relationships (QSAR) models were developed to evaluate the penetration mechanism of pollutant molecules on the PTFE membrane. This research provides new insights for improving sustainable membrane distillation technologies in treating saline oily wastewater.

Insights into the pH-dependent interactions of sulfadiazine antibiotic with soil particle models.

Sulfonamide antibiotics (SAs) are widely used as a broad-spectrum antibiotic, leading to global concerns due to their potential soil accumulation and subsequent effects on ecosystems. SAs often exhibit remarkable environmental persistence, necessitating further investigation to uncover the ultimate destiny of these molecules. In this work, molecular dynamics simulations combined with complementary quantum chemistry calculations were employed to investigate the influence of pH on the behavior of sulfadiazine (SDZ, a typical SAs) in soil particle models (silica, one of the main components of soil). Meanwhile, the quantification of SDZ molecules aggregation potential onto silica was further extended. SDZ molecules tend to form a monolayer on the soil surface under acidic conditions while forming aggregated adsorption on the surface under neutral conditions. Due to the hydrophilicity of the silica, multiple hydration layers would form on its surface, hindering the further adsorption of SDZ molecules on its surface. The calculated soil-water partition coefficient (Psoil/water) of SDZ+ and SDZ were 9.01 and 7.02, respectively. The adsorption evaluation and mechanisms are useful in controlling the migration and transformation of SAs in the soil environment. These findings provide valuable insights into the interactions between SDZ and soil components, shedding light on its fate and transport in the environment.

Molecular Dynamics Study on the Effect of Polyacrylamide on Electric Field Demulsification of Oil-in-Water Emulsion.

The effect of the water-soluble polymer (partially hydrolyzed polyacrylamide, HPAM) in produced water on the demulsification process of the electric field was studied by molecular dynamics simulations. By comparing the coalescence process of oil droplets in the electric field environment with or without HPAM, we find that HPAM in the water phase can promote the coalescence of nearly oil droplets but hinder the deformation and migration of oil droplets. By analyzing the radial distribution function and interaction energy between molecules, we conclude that the existence of HPAM molecules can reduce the hydrophilicity of other molecules through their strong interaction with water, and sodium ions (Na+) have strong interaction with bound water in the process of breaking away from HPAM, thus leading the movement of water molecules. At the same time, the influence of HPAM molecules located between the two oil droplets on the demulsification process was also studied. The HPAM molecules and sodium ions located between the two oil droplets also affected the coalescence process of oil droplets under an electric field by interacting with water.

Molecular Dynamics Simulations of Supramolecular Polymers within Nanoconfinements for Enhanced Oil Recovery.

Supramolecular polymers offer promising potential for enhanced oil recovery (EOR) advancing techniques. Current instrumental analyses face limitations in capturing instantaneous intracomplex motions due to temporal and spatial constraints. The molecular mechanism of supramolecular polymer transport behavior within nanoconfinement is not yet fully understood. Therefore, the self-assembly mechanism of ß-cyclodextrin (ß-CD) and adamantane (ADA)-modified supramolecular polymers (p-AA-ß-CD-ADA) was delved into in this work. Further exploration focuses on the translocation dynamics of p-AA-ß-CD-ADA within nanoconfinement under external driving forces. Results suggest that ß-CD and ADA in p-AA-ß-CD-ADA were assembled into nodes in the form of a host and a guest, combining with a "node-rebar-cement" interaction model encapsulating the formation mechanism of these supramolecular polymers. The heightened density of the hydrate layers at the nanoscale pore throats acts as a constraining factor, resulting in restricted mobility and altered dynamics of the supramolecular polymers. During passage through nanopore throats, host-guest molecules within the supramolecular polymer experience noncovalent dissociation. Notably, these supramolecular polymers exhibit remarkable self-healing capabilities, reinstating their assembly state upon traversing pore throats. This work provides a molecular-level comprehension of the potential utility of supramolecular polymers in EOR processes, offering valuable information for the molecular design of polymers employed for EOR in low-permeability reservoirs.

Theoretical investigation of asphaltene molecules in crude oil viscoelasticity enhancement.

Understanding the mechanisms of viscosity enhancement in crude oil phases is crucial for optimizing extraction and transportation processes. The enhanced viscosity mechanism of crude oil phase can be attributed to the intricate intermolecular interactions between asphaltene molecules. However, the molecular mechanism of the viscosification of asphaltene molecules in crude oil is not yet to be fully understood. In this work, molecular dynamics simulations were employed to investigate the dynamic behavior and viscosification mechanism of asphaltene molecules in complex oil phases. Research suggests that the neutral surface of asphaltenes features abundant positive and negative electrostatic potential regions, facilitating complementary pairing between these areas. This significantly augments electrostatic interactions among asphaltene molecules. Besides, the expansive nonpolar expanse on the normal asphaltene surface facilitates interactions between asphaltenes and crude oil molecules. This leads the crude oil viscosity of the system containing normal asphaltene is higher than that of the system containing acidic asphaltene under the same mass fraction (382 µ Pa·s for AAsp and 416 µ Pa·s for NAsp). This work provides insight into the viscosity enhancement mechanisms in crude oil phases and is helpful in improving the efficiency of crude oil extraction and transportation.

Comparison of H2O Adsorption and Dissociation Behaviors on Rutile (110) and Anatase (101) Surfaces Based on ReaxFF Molecular Dynamics Simulation.

The relationship between structure and reactivity plays a dominant role in water dissociation on the various TiO2 crystallines. To observe the adsorption and dissociation behavior of H2O, the reaction force field (ReaxFF) is used to investigate the dynamic behavior of H2O on rutile (110) and anatase (101) surfaces in an aqueous environment. Simulation results show that there is a direct proton transfer between the adsorbed H2O (H2Oad) and the bridging oxygen (Obr) on the rutile (110) surface. Compared with that on the rutile (110) surface, an indirect proton transfer occurs on the anatase (101) surface along the H-bond network from the second layer of water. This different mechanism of water dissociation is determined by the distance between the 5-fold coordinated Ti (Ti5c) and Obr of the rutile and anatase TiO2 surfaces, resulting in the direct or indirect proton transfer. Additionally, the hydrogen bond (H-bond) network plays a crucial role in the adsorption and dissociation of H2O on the TiO2 surface. To describe interfacial water structures between TiO2 and bulk water, the double-layer model is proposed. The first layer is the dissociated H2O on the rutile (110) and anatase (101) surfaces. The second layer forms an ordered water structure adsorbed to the surface Obr or terminal OH group through strong hydrogen bonding (H-bonding). Affected by the H-bond network, the H2O dissociation on the rutile (110) surface is inhibited but that on the anatase (101) surface is promoted.

Harmonic Vibrational Frequency Simulation of Pharmaceutical Molecules via a Novel Multi-Molecular Fragment Interception Method.

By means of a computational method based on Density Functional Theory (DFT), using commercially available software, a novel method for simulating equilibrium geometry harmonic vibrational frequencies is proposed. Finasteride, Lamivudine, and Repaglinide were selected as model molecules to study the adaptability of the new method. Three molecular models, namely the single-molecular, central-molecular, and multi-molecular fragment models, were constructed and calculated by Generalized Gradient Approximations (GGAs) with the PBE functional via the Material Studio 8.0 program. Theoretical vibrational frequencies were assigned and compared to the corresponding experimental data. The results indicated that the traditional single-molecular calculation and scaled spectra with scale factor exhibited the worst similarity for all three pharmaceutical molecules among the three models. Furthermore, the central-molecular model with a configuration closer to the empirical structure resulted in a reduction of mean absolute error (MAE) and root mean squared error (RMSE) in all three pharmaceutics, including the hydrogen-bonded functional groups. However, the improvement in computational accuracy for different drug molecules using the central-molecular model for vibrational frequency calculation was unstable. Whereas, the new multi-molecular fragment interception method showed the best agreement with experimental results, exhibiting MAE and RMSE values of 8.21 cm-1 and 18.35 cm-1 for Finasteride, 15.95 cm-1 and 26.46 cm-1 for Lamivudine, and 12.10 cm-1 and 25.82 cm-1 for Repaglinide. Additionally, this work provides comprehensive vibrational frequency calculations and assignments for Finasteride, Lamivudine, and Repaglinide, which have never been thoroughly investigated in previous research.

Contribution of air-water interface in removing PFAS from drinking water: Adsorption, stability, interaction and machine learning studies.

As a class of synthetic persistent organic pollutants, contamination of Per-and poly-fluoroalkyl substances (PFAS) in drinking water has attracted widespread concern. Aeration has been confirmed to enhance the removal of PFAS in drinking water by activated carbon (AC). However, the contribution of the air-water interface in removing PFAS is not yet to be fully understood at the molecular level. In this work, molecular dynamics (MD) simulations were employed to investigate the role of nanobubble in removing PFAS in the aqueous environment. The result suggests that the free energies of the air-water interface are about 3-7 kcal mol-1 lower than that of the bulk water region, indicating that the transformation of PFAS from the water phase into the air-water interface is favorable from the viewpoint of thermodynamics. The interface-water partition coefficients (Psur/wat) of PFAS are in the order of PFOS > PFOA > PFHxS > PFBS. On the air-water-AC three-phase interface, PFBS can not only move along the interface region but also leave the interface region into water phase, while PFOS tended to move along the interface region until it was captured by AC. Finally, the ΔGwater-interface quantitative structure-activity relationships (QSAR) models were developed to predict the removal efficiencies of PFAS enhanced by aeration in aquatic systems. The proposed mechanism promotes the understanding of the contribution of air-water interface in removing PFAS from drinking water by activated carbon.

Molecular Insights into Cyclodextrin-Adamantane-Modified Copolymer Host-Guest Interactions.

Supramolecular polymer flooding has great potential in solving the problems of difficult injection and low recovery in low-permeability polymer reservoirs. However, the self-assembly mechanism of supramolecular polymers is not yet to be fully understood at the molecular level. In this work, molecular dynamics simulations were used to explore the formation of cyclodextrin and adamantane-modified supramolecular polymer hydrogels; the self-assembly mechanism was summarized; and the effect of concentration on the oil displacement index was evaluated. The assembly mechanism of supramolecular polymers can be attributed to the "node-rebar-cement" mode of action. At the same time, Na+ can form intermolecular and intramolecular salt bridges with supramolecular polymers, and together with the "node-rebar-cement" mode of action, the supramolecular polymers can form a more compact 3D network structure. When the polymer concentration was increased, especially up to its critical association concentration (CAC), the association increased significantly. Besides, the construction of a 3D network was promoted, which results in a higher viscosity. This work investigated the assembly process of supramolecular polymers from the molecular scale and explained its mechanism of action, which makes up for the deficiencies of other research methods and provides a theoretical basis for screening out functional units that can be used for the supramolecular polymer assembly.

Understanding the transformations of nanoplastic onto phospholipid bilayers: Mechanism, microscopic interaction and cytotoxicity assessment.

The ubiquitous nanoplastics are now considered emergent pollutants in environments. Bioaccumulation of nanoplastics is an important indicator of their hazard. In this work, molecular dynamics were used to study the uptake of five nanoplastics (polyvinyl chloride (PVC), polystyrene (PS), polylactic acid (PLA), polypropylene (PP), and polyethylene terephthalate (PET)) onto DPPC (dipalmitoylphosphatidylcholine) bilayers. Results suggest that nanoplastics became compact after they were deposited in the human body. For PET, PLA, and PS nanoplastics, a free energy barrier of 4-22 kcal mol-1 needed to be overcome to transfer these polymers from the interface region to the center of the DPPC bilayer. Besides, the free energy difference of PVC and PP from the bulk H2O to the surface of DPPC was -18.67 kcal mol-1 and -25.94 kcal mol-1, respectively. After uptake, the interaction between nanoplastics and lipid bilayer was dominated by the van der Waals rather than electrostatic interaction. Furthermore, the cytotoxicity of nanoplastics was also evaluated and it is reflected in their ability to decrease the thickness of the lipid bilayer. Overall, this work provides implications for understanding the bioaccumulation and toxicity of nanoplastic at the molecular level.

Hydrophilic Silica Nanoparticles in O/W Emulsion: Insights from Molecular Dynamics Simulation.

Previous studies have been carried out on the effect of silica nanoparticles (SNPs) on the stability of oil-water emulsions. However, the combining configuration of SNPs and oil droplets at the molecular level and the effect of SNP content on the coalescence behavior of oil droplets cannot be obtained through experiments. In this paper, molecular dynamics (MD) simulation was performed to investigate the adsorption configuration of hydrophilic SNPs in an O/W emulsion system, and the effect of adsorption of SNPs on coalescence of oil droplets. The simulation results showed: (i) SNPs adsorbed on the surface of oil droplets, and excessive SNPs self-aggregated and connected by hydrogen bonds. (ii) Partially hydrophilic asphaltene and resin molecules formed adsorption configurations with SNPs, which changed the distribution of oil droplet components. Furthermore, compared with hydrophobic asphaltene, the hydrophilic asphaltene was easier to combine with SNPs. (iii) SNPs would extend the oil droplet coalescence time, and the π-π stacking structures were formed between asphaltene and asphaltene or resin molecules to enhance the connection between oil droplets during the oil droplet contact process. (iv) Enough SNPs tightly wrapped around the oil droplet, similar to the formation of a rigid film on the surface of an oil droplet, which hindered the contact and coalescence of components between oil droplets.

Theoretical insights into the uptake of sulfonamides onto phospholipid bilayers: Mechanisms, interaction and toxicity evaluation.

Sulfonamides (SAs) are now recognized as the main emerging environmental pollutants in aquatic environments. Although the bioaccumulation capacities of SAs have been confirmed, the pathway for the penetration of the SAs into lipid bilayer has been not fully understood. In this study, the bioaccumulation mechanism of four typical SAs onto the dipalmitoyl phosphatidylcholine (DPPC) lipid bilayer and their effects on the properties of DPPC bilayer were employed and evaluated respectively by using molecular dynamics simulations. Results show that from the viewpoint of thermodynamics, it is favorable for these SAs partitioning to DPPC bilayer. The accommodation of four SAs onto the lipid membrane needs to undergo several processes, which include the contact stage, transformation stage, and absorption stage. Besides, the sulfamethoxazole (SMX) and sulfamethazine (SMZ) show a strong preference for the DPPC phase rather than the interface region while the sulfadiazine (SDZ) and sulfametoxydiazine (SMD) have similar tendencies in the interface region and DPPC phase. Furthermore, the cytotoxicity of SAs is reflected in their ability to affect the electrostatic potential of the membrane and to reduce the thickness of phospholipid bilayers. This molecular-level study provided an insightful understanding of the toxicity and bioaccumulation of SAs.

Molecular Dynamics Study on Properties of Hydration Layers above Polymer Antifouling Membranes.

Zwitterionic polymers as crucial antifouling materials exhibit excellent antifouling performance due to their strong hydration ability. The structure−property relationship at the molecular level still remains to be elucidated. In this work, the surface hydration ability of three antifouling polymer membranes grafting on polysiloxane membranes Poly(sulfobetaine methacrylate) (T4-SB), poly(3-(methacryloyloxy)propane-1-sulfonate) (T4-SP), and poly(2-(dimethylamino)ethyl methacrylate) (T4-DM) was investigated. An orderly packed, and tightly bound surface hydration layer above T4-SP and T4-SB antifouling membranes was found by means of analyzing the dipole orientation distribution, diffusion coefficient, and average residence time. To further understand the surface hydration ability of three antifouling membranes, the surface structure, density profile, roughness, and area percentage of hydrophilic surface combining electrostatic potential, RDFs, SDFs, and noncovalent interactions of three polymers' monomers were studied. It was concluded that the broadest distribution of electrostatic potential on the surface and the nature of anionic SO3- groups led to the following antifouling order of T4-SB > T4-SP > T4-DM. We hope that this work will gain some insight for the rational design and optimization of ecofriendly antifouling materials.

Molecular Dynamics Simulation for the Demulsification of O/W Emulsion under Pulsed Electric Field.

A bidirectional pulsed electric field (BPEF) method is considered a simple and novel technique to demulsify O/W emulsions. In this paper, molecular dynamics simulation was used to investigate the transformation and aggregation behavior of oil droplets in O/W emulsion under BPEF. Then, the effect of surfactant (sodium dodecyl sulfate, SDS) on the demulsification of O/W emulsion was investigated. The simulation results showed that the oil droplets transformed and moved along the direction of the electric field. SDS molecules can shorten the aggregation time of oil droplets in O/W emulsion. The electrostatic potential distribution on the surface of the oil droplet, the elongation length of the oil droplets, and the mean square displacement (MSD) of SDS and asphaltene molecules under an electric field were calculated to explain the aggregation of oil droplets under the simulated pulsed electric field. The simulation also showed that the two oil droplets with opposite charges have no obvious effect on the aggregation of the oil droplets. However, van der Waals interactions between oil droplets was the main factor in the aggregation.

Mechanistic study of the adsorption and penetration of modified SiO2 nanoparticles on cellular membrane.

SiO2 nanoparticles (NPs) are ubiquitous in the atmosphere and have been proved to be harmful to human by bioaccumulation. The bioaccumulation of SiO2 NPs begins with their partitioning into membrane phospholipids. However, the uptake of SiO2 particle onto lipid bilayers has been not completely understood. In this study, the uptake process of different modified SiO2 particles (with adsorbed trace gas molecules, including formic acid (FA), methyl vinyl ketone (MVK), and methacrolein (MAC)) into DPPC bilayers were investigated by molecular dynamics (MD) simulations. Results suggest that after the SiO2 particle absorbed on the surface of bilayers, it spun by itself to form the most stable adsorption configurations. MAC and MVK molecule tend to be absorbed into DPPC bilayer while FA molecule was more likely located at the surface region of bilayer from the viewpoint of thermodynamics. Besides, it was also found apart from the commonly accepted "Trojan-horse" effect, SiO2 NPs may increase biohazard via modulating the concentration of pollutants. This work is beneficial for understanding the toxicity and bioaccumulation of FA, MVK, MAC, and SiO2 NPs at molecular level.

Degradation evaluation of acrylamide in advanced oxidation processes based on theoretical method: Mechanisms, kinetics, toxicity evaluation and the role of soil particles.

Acrylamide (AA) is now recognized as an imminent hazardous chemical in the aqueous environment, causing a potential threat to human health. As a neo-formed contaminant (NFC), the degradation measure of AA is largely lacking. In this work, we used quantum chemistry and experimental methods to identify the main degradation mechanism of AA in the UV/H2O2 advanced oxidation process (AOP) for the first time. Radical addition reactions dominate the •OH-initiated AA reaction, resulting in few toxic nitrosamines formation. The interaction between AA and the surface model of soil particles (SixOy(OH)z) is weak, and AA can rapidly migrate down to groundwater via seepage. However, the total rate constants of AA and COMADS2-AA with •OH are 2.75 × 109 and 2.09 × 109 M-1 s-1, and the removal of AA from aqueous and heterogeneous systems reaches 62.30% and 62.05% within 2 h. Whether in the aqueous-phase or on the surface of soil particles, •OH initiated AA reaction is an efficient way to remove AA. Furthermore, the toxicity of the main by-products of AA show less harmful to three aquatic organisms and rats than AA. UV/H2O2 AOP is evaluated as an efficient method to degrade AA while decreasing harm.

Molecular insights into the uptake of SiO2 nanoparticles on phospholipid membrane: Effect of surface properties and particle size.

Silica (SiO2) nanoparticles (NPs) have attracted much attention due to the potential for a wide range of applications and they have been confirmed to be hazardous to humans. Partitioning to phospholipid bilayers is an important way for their bioaccumulation. However, the detailed mechanism of SiO2 NPs uptake by membrane phospholipids remains uncertain. In this work, molecular dynamics (MD) simulations were employed to study the uptake process of SiO2 NPs into DPPC bilayers. Results show that these SiO2 NPs uptake onto DPPC bilayer surface is favorable from the viewpoint of thermodynamics. During the uptake process, the SiO2 NP needed to adjust the angle of interaction with the DPPC surface until the most stable adsorption configuration was reached. After incorporating into DPPC bilayers, the interaction between PO4- group and SiO2 particle is stronger than -N+(CH3)3 group and SiO2. Small SiO2 NP was found to adsorb to the surface of DPPC bilayer without disturbing the morphology or membrane. In contract, bioaccumulation of large SiO2 NP to DPPC induced a strong local membrane deformation. In addition, the effect of SiO2 NP surface functionalization on its interaction with DPPC was also investigated. This molecular-level study reports a complete description of the interaction between SiO2 NPs and DPPC bilayer, aiming to provide some insights for the further work on the bioaccumulation and hemolytic activity of SiO2 NPs.