百欧林简报-表界面科学最新文献- QSense -2020年第1期

1.Name：Release of deposited MnO2 nanoparticles from aqueous surfaces

Authors：Hainan Wang，Ruixing Huang，Chengxue Ma，Xiaoling Li, Caihong Liu, Qiang He, Zhengsong Wu, Jun Ma ａnd Xiaoliu Huangfu

Journal：Journal of Environmental Sciences

DOI: 10.1016/j.jes.2019.12.011

Abstract：Changes in solution chemistry ａnd transport conditions can lead to the release of deposited MnO2 nanoparticles from a solid interface, allowing them to re-enter the aqueous environment. Understanding the release behavior of MnO2 nanoparticles from naturally occurring surfaces is critical for better prediction of the transport potential ａnd environmental fate of MnO2 nanoparticles. In this study, the release of MnO2 nanoparticles was investigated using a quartz crystal microbalance with dissipation monitoring (QCM-D), ａnd different environmental surface types, solution pH values ａnd representative macromolecular organics were considered. MnO2 nanoparticles were first deposited on crystal sensors at elevated NaNO3 concentrations before being rinsed with double-deionized water to induce their remobilization. The results reveal that the release rate of MnO2 depends on the surface type, in the decreasing order: SiO2 > Fe3O4 > Al2O3, resulting from electrostatic interactions between the surface ａnd particles. Moreover, differences in solution pH can lead to variance in the release behavior of MnO2 nanoparticles. The release rate from surfaces was significantly higher at pH 9.8 that at 4.5, indicating that alkaline conditions were more favorable for the mobilization of MnO2 in the aquatic environment. In the presence of macromolecular organics, bovine serum albumin (BSA) can inhibit the release of MnO2 from the surfaces due to attractive forces. In presence of humic acid (HA) ａnd sodium alginate (SA), the MnO2 nanoparticles were more likely to be mobile, which may be associated with a large repulsive barrier imparted by steric effects.

Link：https://www.sciencedirect.com/science/article/pii/S1001074219333935

2.Name：Characterization of chitosan-lysine surfactant bioactive coating on silicone substrate

Authors：Urban Ajdnik, Matjaž Finšgar ａnd Lidija Fras Zemljič

Journal：Carbohydrate Polymers

DOI: 10.1016/j.carbpol.2019.115817

Abstract：Chitosan (Chi) ａnd anionic surfactant derived from lysine (77KS) were used to prepare a novel bioactive coating ａnd as a drug delivery system for amoxicillin (AMOX) on a model polydimethylsiloxane (PDMS) surface. The bioactive coating was formulated as polyelectrolyte-surfactant complex (PESC). Aggregation behaviour between the cationic Chi ａnd oppositely charged 77KS in bulk was analysed using turbidity ａnd ζ-potential measurement. Furthermore, the adsorption ａnd stability of the formulations were evaluated using quartz crystal microbalance with dissipation (QCM-D). The effect of the ionic strength ａnd of the ultraviolet/ozone (UVO) activation of the PDMS films on the adsorption behaviour of the PESC complex was also examined. QCM-D monitoring showed stable adsorption of bare ａnd AMOX-loaded complex on non-activated PDMS films, while the coating on UVO-activated PDMS samples desorbed after the rinsing step. Finally, X-ray photoelectron spectroscopy ａnd time-of-flight secondary ion mass spectrometry confirmed successful ａnd homogenously distributed compounds.

Link：https://www.sciencedirect.com/science/article/pii/S0144861719314857

3.Name：Effect of Amines on the Lubricity of Castor Oil-Sulfated Sodium Salt Solution for Titanium Alloys

Authors：Ye Yang, Tengfei Liu, Yuanjing Dai, Yan Wang ａnd Chenhui Zhang

Journal：Tribology Letters

DOI: 10.1007/s11249-019-1261-9

Abstract：This work investigates the effect of amines on the lubricity of castor oil-sulfated sodium salt (CSS) emulsion solution for titanium alloys. It is found that the amines with hydrophilic parts such as diglycolamine, have a negative effect on the lubrication while those with hydrophobic parts such as dicyclohexylamine (DCHA), show a synergistic effect when they are mixed with the CSS. The mechanisms of both the synergistic ａnd negative effects of amines are investigated. The quartz crystal microbalance with dissipation-monitoring results show that the ammonium salt with hydrophobic parts such as DCHA can form a strong adsorption film on the titanium surface. These findings indicate that the amines with hydrophobic parts can be used as a pH regulator ａnd corrosion inhibitor for developing an effective cutting fluid for titanium alloys.

Link：https://link.springer.xilesou.top/article/10.1007/s11249-019-1261-9

4.Name：Carboxybetaine functionalized nanosilicas as protein resistant surface coatings

Authors：Knowles, B. R., Wagner, P., Maclaughlin, S., Higgins, M. J., & Molino, P. J.

Journal：Biointerphases

DOI: 10.1063/1.5126467

Abstract：Materials with protein resistant properties are increasingly sought after for their potential application as low-fouling surface coatings. Hydrophilic coatings with improved resistance to protein fouling have been prepared from zwitterionic carboxybetaine (CB) functionalized silica nanoparticles (SiNPs). The authors report three methods of coating preparation via direct tethering of CB to predeposited particle films, a two-step surface functionalization process, ａnd deposition of CB functionalized particle dispersions. The pH at which aqueous CB solutions were prepared ａnd reacted to SiNPs was found to drastically influence the mechanism of CB attachment ａnd affect the protein resistance of the resultant coatings. Depending on the method of coating preparation, protein binding to functionalized particle coatings was reduced by up to 94% compared to unfunctionalized SiNP control surfaces. As a result, all three methods offer simple ａnd scalable fabrication routes for the generation of hydrophilic, zwitterionic interfaces with improved inhibition to protein fouling.

Link：https://avs.scitation.org/doi/full/10.1063/1.5126467

5.Name：Deposition of cellulose nanocrystals onto biomimetic lipid membranes

Authors： Yotam Navon, Bruno Jean, Liliane Coche-Guerente, Franck Dahlem, Anne Bernheim-Groswasser ａnd Laurent Heux

Journal：Langmuir

DOI: 10.1021/acs.langmuir.9b02888

Abstract：The deposition of cellulose nanocrystals (CNCs) on a supported lipid bilayer (SLB) was investigated at different length scales. A quartz crystal microbalance with dissipation monitoring (QCM-D) was used to probe the bilayer formation ａnd to show for the first time the CNCs deposition onto the SLB. Specifically, classical QCM-D measurements gave estimation of the adsorbed hydrated mass ａnd the corresponding film thickness, whereas complementary experiments using D2O as the solvent allowed the quantitative determination of the hydration of the CNCs layer, showing a high hydration value. Scanning force microscopy (SFM) ａnd total internal reflection fluorescence microscopy (TIRF) were used to probe the homogeneity of the deposited layers ａnd reveal the structural details at the particle ａnd film length scales, respectively, ａnd to give information on the effect of CNCs concentration on the surface coverage. The results showed that the adsorption of CNCs on the supported lipid membrane depends on lipid composition, CNCs concentration ａnd pH conditions, ａnd that the binding process was governed by electrostatic interactions. Under suitable conditions, a uniform film was formed, with thickness corresponding to a CNCs monolayer, which provides the basis for a relevant 2D model of primary plant cell wall.

Link：https://pubs.acs.org/doi/10.1021/acs.langmuir.9b02888

6.Name：pH-Responsive Copolymer Films Prepared by Surface-Initiated Polymerization ａnd Simple Modification

Authors：Xuanli Deng, Joshua L. Livingston, Nathan Spear ａnd G. Kane Jennings

Journal：Langmuir

DOI: 10.1021/acs.langmuir.9b03026

Abstract：We report the preparation of pH-responsive, ester/carboxylic acid random copolymer films via simple modification of poly(norbornene diacyl chloride) (pNBDAC), prepared via surface-initiated ring-opening metathesis polymerization, with mixtures of water ａnd ethanol to form carboxylic acid ａnd ethyl ester side groups. The pNBDAC film serves as a compositionally versatile platform to controllably obtain copolymers with multiple functionalities. In modifying the pNBDAC to form the copolymer film, ethanol exhibits a significantly higher reactivity with acyl chloride groups within the film than does water. The magnitude ａnd range of the pH-responsive performance are highly dependent on the carboxylic acid content in the copolymer films, which demonstrates the effect of film hydrophilicity on the pH-responsive switching of ionic barrier properties. The resistance of the film against ion transfer can be decreased by a factor of 104 through pH change, demonstrating pH-induced switching from hydrophobic ａnd insulating to swollen ａnd ion-permeable films. The interactions of the copolymer films with water at different pH values were also explored. When the copolymer contains 34% carboxylic acids, a 4x greater film thickness is obtained in high pH solution than in low pH solution due to ionically driven water swelling. The reversibility ａnd reproducibility of the pH-responsive performance of these copolymer films is high based on measurements using quartz crystal microbalance with dissipation (QCM-D).

Link：https://pubs.acs.org/doi/10.1021/acs.langmuir.9b03026

7.Name：Further interpretation of the underlying causes of the strengthening effect of alkali on gluten ａnd noodle quality: Studies on gluten, gliadin, ａnd glutenin

Authors：Chuanwu Han, Meng Ma, Man Li ａnd Qingjie Sun

Journal：Food Hydrocolloids

DOI: 10.1016/j.foodhyd.2020.105661

Abstract：Alkali significantly enhanced gluten strength ａnd noodle texture. To further understand the underlying mechanisms of the gluten strengthening effect of alkali, the macroscopic rheological properties, microstructure, intermolecular interactions, water mobility, molecular weight distribution (MWD) ａnd structure, ａnd the molecular chain morphology changes of gluten ａnd its subfractions (glutenin ａnd gliadin) were separately investigated. Alkali increased the G′ ａnd G″ of gluten ａnd glutenin fractions. Scanning electron microscopy (SEM) images confirmed that alkali induced a more compact structure in all fractions ａnd a membrane-like structure in gluten ａnd glutenin. Quartz crystal microbalance with dissipation (QCM-D) results demonstrated that alkali promoted alkali/protein-protein interactions in gluten ａnd glutenin fractions. Hydrophobic interactions ａnd water-solids interaction were enhanced by alkali in all fractions. Glutenin fraction was shown to play a key role in the protein polymerization of fresh gluten samples in the presence of alkali, while both glutenin ａnd gliadin contributed to the enhanced polymerization during cooking. Atomic force microscopy (AFM) images showed that alkali induced remarkable aggregations of protein molecular chains in gluten system.

Link：https://sciencedirect.xilesou.top/science/article/pii/S0268005X1931690X

8.Name：Supramolecular Protein Assembly Retains Its Structural Integrity at Liquid–Liquid Interface

Authors：Mridul Sarker, Hwankyu Lee, Rui A. Gonçalves, Yeng Ming Lam, Haibin Su ａnd Sierin Lim

Journal：Advanced Materials Interfaces

DOI: 10.1002/admi.201901674

Abstract：Adsorption of globular proteins at liquid–liquid interface results in compromised structures ａnd functionalities to maintain a thermodynamically favorable state. However, the structural behavior of highly symmetrical supramolecular protein assemblies, adsorbed at the liquid–liquid interface, is not well understood. In this study, a model supramolecular protein assembly, E2 protein nanocage, a dodecahedral cage‐structured protein, is studied upon adsorption at the oil–water interface by both theoretical ａnd experimental analyses. Molecular dynamics simulations ａnd force estimation reveal that noncovalent interactions between E2 subunits dominate over the tangential force experienced by E2 at the interface allowing it to retain its structural integrity. Experimental analyses confirm the adsorption of E2 on the liquid–liquid interface with negligible penetration depth. Molecular structural analyses further suggest the structural integrity of the caged structure of E2 at the oil–water interface with minimal change in the tertiary ａnd secondary structures. In conclusion, this study brings new insights into the behavior of highly symmetrical supramolecular protein assemblies at liquid–liquid interface which is important in preserving their functionalities.

Link：https://onlinelibrary.wiley.xilesou.top/doi/abs/10.1002/admi.201901674

9.Name：Formation ａnd characteristics of mixed lipid/polymer membranes on a crystalline surface-layer protein lattice

Authors：Czernohlavek, Christian, ａnd Bernhard Schuster

Journal：Biointerphases

DOI: 10.1116/1.5132390

Abstract：The implementation of self-assembled biomolecules on solid materials, in particular, sensor ａnd electrode surfaces, gains increasing importance for the design of stable functional platforms, bioinspired materials, ａnd biosensors. The present study reports on the formation of a planar hybrid lipid/polymer membrane on a crystalline surface layer protein (SLP) lattice. The latter acts as a connecting layer linking the biomolecules to the inorganic base plate. In this approach, chemically bound lipids provided hydrophobic anchoring moieties for the hybrid lipid/polymer membrane on the recrystallized SLP lattice. The rapid solvent exchange technique was the method of choice to generate the planar hybrid lipid/polymer membrane on the SLP lattice. The formation process ａnd completeness of the latter were investigated by quartz crystal microbalance with dissipation monitoring ａnd by an enzymatic assay using the protease subtilisin A, respectively. The present data provide evidence for the formation of a hybrid lipid/polymer membrane on an S-layer lattice with a diblock copolymer content of 30%. The hybrid lipid/polymer showed a higher stiffness compared to the pure lipid bilayer. Most interestingly, both the pure ａnd hybrid membrane prevented the proteolytic degradation of the underlying S-layer protein by the action of subtilisin A. Hence, these results provide evidence for the formation of defect-free membranes anchored to the S-layer lattice.

Link：https://avs.scitation.org/doi/full/10.1116/1.5132390

10.Name：Electrochemically induced changes in TiO2 ａnd Carbon films, studied with QCM-D

Authors：Narayanan, Aditya, Frieder Mugele, ａnd Michael HG Duits

Journal：ACS Applied Energy Materials

DOI: 10.1021/acsaem.9b02233

Abstract：Semi-solid fluid electrode-based battery (SSFB) ａnd supercapacitor technologies are seen as very promising candidates for grid energy storage. However, unlike for traditional batteries, their performance can quickly get compromised by the formation of poorly conducting Solid Electrolyte Interphase on the particle surfaces. In this work we examine SEI film formation in relation to typical electrochemical conditions, by combining Cyclic Voltammetry (CV) with Quartz Crystal Microbalance-Dissipation monitoring (QCM-D). Sputtered layers of typical SSFB materials like Titanium dioxide (TiO2) ａnd Carbon, immersed in alkyl carbonate solvents, are cycled to potentials of relevance to both traditional ａnd flow systems. Mass changes due to Lithium intercalation ａnd SEI formation are distinguished by measuring the electrochemical current simultaneously with the damped mechanical oscillation. Both the TiO2 ａnd amorphous Carbon layers show a significant irreversible mass increase on continued exposure to (even mildly) reducing electrochemical conditions. Studying the small changes within individual charge-discharge cycles, TiO2 shows mass oscillations, indicating a partial reversibility due to lithium intercalation (not found for Carbon). Viscoelastic signatures in the MHz frequency regime confirm the formation ａnd growth of a soft layer, again with oscillations for TiO2 but not for Carbon. All these observations are consistent with irreversible SEI formation for both materials, ａnd reversible Li intercalation for TiO2. Our results highlight the need for careful choices of the materials chemistry ａnd a sensitive electrochemical screening for fluid electrode systems.

Link：https://pubs.acs.org/doi/abs/10.1021/acsaem.9b02233

11.Name：Synergistic improvement in the performance of insect odorant receptor based biosensors in the presence of Orco

Authors：Roshan Khadka, Colm Carraher, Cyril Hamiaux, Jadranka Travas-Sejdic ａnd AndrewKralicek

Journal：Biosensors ａnd Bioelectronics

DOI: 10.1016/j.bios.2020.112040

Abstract：Insect odorant receptors (ORs) are believed to be a complex of an odorant binding subunit, OrX, ａnd an ion channel forming subunit, Orco. In our previous study, we showed that the OrX subunit on its own in liposomes could detect volatile organic compounds (VOCs) ultrasensitively using Electrochemical Impedance Spectroscopy (EIS). In this study, we investigated the effect of the presence of Orco on the response of the OrX subunit to detect the VOCs. The OrXs - Or10a, Or22a, Or35a ａnd Or71a, together with Orco, were recombinantly expressed, purified ａnd integrated into liposomes. These OrX/Orco liposomes were covalently attached to a gold surface modified with N-hydroxysuccinimide/1-ethyl-3-(3-dimethylaminopropyl)-carbodiimide) (NHS/EDC)-activated self-assembled monolayers (SAMs) of 6-mercaptohexanoic acid (MHA). It was demonstrated that the OrX/Orco liposomes could sensitively ａnd selectively detect their ligands by monitoring a change in frequency ａnd impedance signal upon binding with both Quartz Crystal Microbalance with Dissipation monitoring (QCM-D) ａnd EIS. Using EIS, three OrXs (Or10a, Or22a ａnd Or35a) showed a shift in their dose-response curves when Orco was co-integrated, reflecting an increase in ligand sensitivity ａnd a decrease in limit of detection (LOD). Or71a in the presence of Orco did not show any improvement in ligand sensitivity as this is a highly tuned receptor which may be already at the sensitivity limit for EIS. The observed enhancement in sensor performance is believed to be an effect of Orco which is stabilizing the OrX in a more active conformation ａnd amplifying charge transfer to result in a greater reduction in impedance.

Link：https://sciencedirect.xilesou.top/science/article/pii/S0956566320300373

12.Name：Quartz Crystal Microbalance Based Sensor Arrays for Detection ａnd Discrimination of VOCs Using Phosphonium Ionic Liquid Composites

Authors：Vaughan, S. R., Pérez, R. L., Chhotaray, P., ａnd Warner, I. M.

Journal：Sensors

DOI: 10.3390/s20030615

Abstract：Herein, we examine two sensing schemes for detection ａnd discrimination of chlorinated volatile organic compounds (VOCs). In this work, phosphonium ionic liquids (ILs) were synthesized ａnd vapor sensing properties examined ａnd compared to phosphonium IL-polymer composites. Pure IL sensors were used to develop a QCM-based multisensory array (MSA), while IL-polymer composites were used to develop an MSA ａnd virtual sensor arrays (VSAs). It was found that by employing the composite MSA, five chlorinated VOCs were accurately discriminated at 95.56%, which was an increase in accuracy as compared to pure ILs MSA (84.45%). Data acquired with two out of three VSAs allowed discrimination of chlorinated VOCs with 100% accuracy. These studies have provided greater insight into the benefits of incorporating polymers in coating materials for enhanced discrimination accuracies of QCM-based sensor arrays. To the best of our knowledge, this is the first report of a QCM-based VSA for discrimination of closely related chlorinated VOCs.

Link：https://www.mdpi.xilesou.top/1424-8220/20/3/615

13.Name：Effect of surface chemistry on hMSC growth under xeno-free conditions

Authors：Maura Cimino, Paula Parreira, Sílvia Bidarra, Raquel M.Gonçalves, Cristina C.Barrias ａnd M. Cristina L.Martins

Journal：Colloids ａnd Surfaces B: Biointerfaces

DOI: 10.1016/j.colsurfb.2020.110836

Abstract：Human mesenchymal stem/stromal cells (hMSC) are promising therapeutic agents for regenerative medicine. However, therapeutic doses necessary for clinical application require in vitro expansion, ideally under Xeno-Free conditions (XF) to avoid the use of foetal bovine serum (FBS). We previously reported that hMSCs could be expanded using a pharmaceutical-grade human plasma-derived supplement for cell culture (SCC, Plastem®) combined with bFGF ａnd TGFβ1, on fibronectin (Fn)-coated surfaces.

hMSCs expansion may also be affected by the chemistry of the culture surface, which modulates protein adsorption at the cell-material interface and, consequently, cell behavior.

This work aimed to evaluate the effect of surface chemistry on hMSCs behaviour in SCC-based XF media. For that, self-assembled monolayers (SAMs) with hydrophobic (-CH3) ａnd hydrophilic (neutral -OH, positively charged -NH3+ ａnd negatively charged -COO-) groups were used as model surfaces.

Under XF conditions, Fn coating showed to be necessary to improve hMSC adhesion (4 h) onto all surfaces, except for OH-SAMs, probably due to a low protein adsorption capacity characteristic of this surface. In terms of cell metabolic activity (5 days) on Fn-coated surfaces, an increase over time under XF conditions was observed in all SAMs except in CH3-SAMs, which can be attributed to strong ａnd irreversible protein adsorption characteristic of hydrophobic surfaces. This trend was also observed under FBS conditions. Nevertheless, of the surfaces improved hMSC metabolic activity, as compared with tissue-cultured surfaces. Overall, this work describes the role of surface chemistry in XF hMSC expansion.

Link：https://sciencedirect.xilesou.top/science/article/pii/S0927776520300667

14.Name：Room‐Temperature Partial Conversion of α‐FAPbI3 Perovskite Phase via PbI2 Solvation Enables High‐Performance Solar Cells

Authors：Dounya Barrit, Peirui Cheng, Kasra Darabi, Ming‐Chun Tang, Detlef‐M. Smilgies, Shengzhong (Frank) Liu, Thomas D. Anthopoulos, Kui Zhao ａnd Aram Amassian

Journal：Advanced Functional Materials

DOI: 10.1002/adfm.201907442

Abstract：The two‐step conversion process consisting of metal halide deposition followed by conversion to hybrid perovskite has been successfully applied toward producing high‐quality solar cells of the archetypal MAPbI3 hybrid perovskite, but the conversion of other halide perovskites, such as the lower bandgap FAPbI3, is more challenging ａnd tends to be hampered by the formation of hexagonal nonperovskite polymorph of FAPbI3, requiring Cs addition and/or extensive thermal annealing. Here, an efficient room‐temperature conversion route of PbI2 into the α‐FAPbI3 perovskite phase without the use of cesium is demonstrated. Using in situ grazing incidence wide‐angle X‐ray scattering (GIWAXS) ａnd quartz crystal microbalance with dissipation (QCM‐D), the conversion behaviors of the PbI2 precursor from its different states are compared. α‐FAPbI3 forms spontaneously ａnd efficiently at room temperature from P2 (ordered solvated polymorphs with DMF) without hexagonal phase formation ａnd leads to complete conversion after thermal annealing. The average power conversion efficiency (PCE) of the fabricated solar cells is greatly improved from 16.0(±0.32)% (conversion from annealed PbI2) to 17.23(±0.28)% (from solvated PbI2) with a champion device PCE > 18% due to reduction of carrier recombination rate. This work provides new design rules toward the room‐temperature phase transformation ａnd processing of hybrid perovskite films based on FA+ cation without the need for Cs+ or mixed halide formulation.

Link：https://onlinelibrary.wiley.xilesou.top/doi/abs/10.1002/adfm.201907442