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      • Colloid-inspired nanoplasmonic biosensing strategies for antiviral peptide evaluation

        ( Joshua A. Jackman ) 한국공업화학회 2020 한국공업화학회 연구논문 초록집 Vol.2020 No.-

        Surface-based nanoplasmonic sensors are powerful tools to characterize biomacromolecular interactions with biomembrane-mimicking platforms. In this talk, I will discuss how nanoparticle- and nanohole-based nanoplasmonic sensing platforms can be utilized to characterize the mechanistic properties of a membrane-active, antiviral peptide. Three examples will be covered: (i) peptide-induced rupture of a close-packed lipid vesicle adlayer on titanium oxide-coated gold nanodisks; (ii) peptide-induced rupture of individual virus-like particles within long-range-ordered, polymer-functionalized gold nanoholes; and (iii) peptide-induced disruption of positively curved membranes in short-range-ordered, silica-coated gold nanoholes.

      • Temperature-Induced Denaturation of BSA Protein Molecules for Improved Surface Passivation Coatings

        Park, Jae Hyeon,Jackman, Joshua A.,Ferhan, Abdul Rahim,Ma, Gamaliel Junren,Yoon, Bo Kyeong,Cho, Nam-Joon American Chemical Society 2018 ACS APPLIED MATERIALS & INTERFACES Vol.10 No.38

        <P>Bovine serum albumin (BSA) is the most widely used protein for surface passivation applications, although it has relatively weak, nonsticky interactions with hydrophilic surfaces such as silica-based materials. Herein, we report a simple and versatile method to increase the stickiness of BSA protein molecules adsorbing onto silica surfaces, resulting in up to a 10-fold improvement in blocking efficiency against serum biofouling. Circular dichroism spectroscopy, dynamic light scattering, and nanoparticle tracking analysis showed that temperature-induced denaturation of BSA proteins in bulk solution resulted in irreversible unfolding and protein oligomerization, thereby converting weakly adhesive protein monomers into a more adhesive oligomeric form. The heat-treated, denatured BSA oligomers remained stable after cooling. Room-temperature quartz crystal microbalance-dissipation and localized surface plasmon resonance experiments revealed that denatured BSA oligomers adsorbed more quickly and in larger mass quantities onto silica surfaces than native BSA monomers. We also determined that the larger surface contact area of denatured BSA oligomers is an important factor contributing to their more adhesive character. Importantly, denatured BSA oligomers were a superior passivating agent to inhibit biofouling on silica surfaces and also improved Western blot application performance. Taken together, the findings demonstrate how temperature-induced denaturation of BSA protein molecules can lead to improved protein-based coatings for surface passivation applications.</P> [FIG OMISSION]</BR>

      • Nanoplasmonic Ruler for Measuring Separation Distance between Supported Lipid Bilayers and Oxide Surfaces

        Ferhan, Abdul Rahim,,pač,ková,, Barbora,Jackman, Joshua A.,Ma, Gamaliel J.,Sut, Tun Naw,Homola, Jiř,,Cho, Nam-Joon American Chemical Society 2018 ANALYTICAL CHEMISTRY - Vol.90 No.21

        <P>Unraveling the details of how supported lipid bilayers (SLBs) are coupled to oxide surfaces is experimentally challenging, and there is an outstanding need to develop highly surface-sensitive measurement strategies to determine SLB separation distances. Indeed, subtle variations in separation distance can be associated with significant differences in bilayer-substrate interaction energy. Herein, we report a nanoplasmonic ruler strategy to measure the absolute separation distance between SLBs and oxide surfaces. A localized surface plasmon resonance (LSPR) sensor was employed to track SLB formation onto titania- and silica-coated gold nanodisk arrays. To interpret measurement data, an analytical model relating the LSPR measurement response to bilayer-substrate separation distance was developed based on finite-difference time-domain (FDTD) simulations and theoretical calculations. The results indicate that there is a larger separation distance between SLBs and titania surfaces than silica surfaces, and the trend was consistent across three tested lipid compositions. We discuss these findings within the context of the interfacial forces underpinning bilayer-substrate interactions, and the nanoplasmonic ruler strategy provides the first direct experimental evidence comparing SLB separation distances on titania and silica surfaces.</P> [FIG OMISSION]</BR>

      • KCI등재

        Interfacial approach to fabricate covalently and noncovalently attached inverse-phosphocholine supported lipid bilayers on TiO2 and SiO2 surfaces

        Tun Naw Sut,Sigalit Meker,Dong Jun Koo,Joshua A. Jackman,Nam-Joon Cho 한국공업화학회 2023 Journal of Industrial and Engineering Chemistry Vol.128 No.-

        Inverse-phosphocholine lipids such as DOCP are intriguing biomolecules for surface functionalizationbecause they can form supported lipid bilayers (SLBs) on titania surfaces but adsorb weakly on silica surfaces. Interestingly, these trends are nearly opposite to those of conventional phosphocholine lipids,motivating deeper investigation of how environmental parameters affect DOCP lipid vesicle adsorptionphenomena. Herein, we systematically investigated how solution pH (4, 6, 8, 10) and ionic strength(50, 150, 250 mM NaCl) influence DOCP lipid vesicle adsorption behavior on titania and silica surfaces. On titania, DOCP lipid vesicles either adsorbed and ruptured to form a covalently attached SLB (acidicpH), adsorbed but did not rupture (basic pH with high salt), or did not adsorb (basic pH with low salt). Conversely, on silica, a narrow range of acidic pH, high-salt conditions triggered DOCP lipid vesicleadsorption and rupture to form a noncovalently attached SLB whereas negligible adsorption occurredin other conditions. The corresponding energetics of the vesicle-surface interaction and lipid attachmentproperties were analyzed and clarify how the interplay of solution pH and ionic strength modulates DOCPlipid vesicle adsorption behavior. Based on these insights, we identified suitable strategies to fabricatecovalently and noncovalently stabilized inverse-phosphocholine lipid bilayers on oxide surfaces.

      • Complement activation in vitro and reactogenicity of low-molecular weight dextran-coated SPIONs in the pig CARPA model: Correlation with physicochemical features and clinical information

        ,,p, Tamá,s,Nemes, Ré,ka,,szá,ros, Tamá,s,Urbanics, Rudolf,Kok, Robbert Jan,Jackman, Joshua A.,Cho, Nam-Joon,Storm, Gert,Szebeni, Já,nos Elsevier 2018 Journal of controlled release Vol.270 No.-

        <P><B>Abstract</B></P> <P>The unique magnetic properties of superparamagnetic iron oxide nanoparticles (SPIONs) have led to their increasing use in drug delivery and imaging applications. Some polymer-coated SPIONs, however, share with many other nanoparticles the potential of causing hypersensitivity reactions (HSRs) known as complement (C) activation-related pseudoallergy (CARPA). In order to explore the roles of iron core composition and particle surface coating in SPION-induced CARPA, we measured C activation by 6 different SPIONs in a human serum that is known to react to nanoparticles (NPs) with strong C activation. Remarkably, only the carboxymethyldextran-coated (ferucarbotran, Resosvist®) and dextran-coated (ferumoxtran-10, Sinerem®) SPIONs caused significant C activation, while the citric acid, phosphatidylcholine, starch and chitosan-coated SPIONs had no such effect. Focusing on Resovist and Sinerem, we found Sinerem to be a stronger activator of C than Resovist, although the individual variation in 15 different human sera was substantial. Further analysis of C activation by Sinerem indicated biphasic dose dependence and significant production of C split product Bb but not C4d, attesting to alternative pathway C activation only at low doses. Consistent with the strong C activation by Sinerem and previous reports of HSRs in man, injection of Sinerem in a pig led to dose-dependent CARPA, while Resovist was reaction-free. Using nanoparticle tracking analysis, it was further determined that Sinerem, more than Resovist, displayed multimodal size distribution and significant fraction of aggregates – factors which are known to promote C activation and CARPA. Taken together, our findings offer physicochemical insight into how key compositional factors and nanoparticle size distribution affect SPION-induced CARPA, a knowledge that could lead to the development of SPIONs with improved safety profiles.</P> <P><B>Graphical abstract</B></P> <P>[DISPLAY OMISSION]</P>

      • Supported lipid membrane platform technology for anti-infective applications

        윤보경,문수지,( Joshua A. Jackman ) 한국공업화학회 2020 한국공업화학회 연구논문 초록집 Vol.2020 No.-

        We demonstrate that adding mixtures of lauric acid (LA) and glycerol monolaurate (GML) - two of the most biologically active antimicrobial fatty acids and monoglycerides - to a supported lipid bilayer platform triggers concurrent tubule and bud formation, which unexpectedly results in synergistic phospholipid membrane remodeling that far exceeds the effects of GML or LA alone. The most pronounced effects occurred with equimolar concentrations of GML and LA in the micellar state, highlighting that synergistic membrane disruption and an inability to relieve membrane strains. These findings offer a new model to explain how fatty acid and monoglyceride interactions can trigger phospholipid membrane remodeling events relevant to various biophysical and biological systems.

      • Nanoplasmonic sensors for detecting circulating cancer biomarkers

        Ferhan, Abdul Rahim,Jackman, Joshua A.,Park, Jae Hyeon,Cho, Nam-Joon,Kim, Dong-Hwan Elsevier 2018 Advanced drug delivery reviews Vol.125 No.-

        <P><B>Abstract</B></P> <P>The detection of cancer biomarkers represents an important aspect of cancer diagnosis and prognosis. Recently, the concept of liquid biopsy has been introduced whereby diagnosis and prognosis are performed by means of analyzing biological fluids obtained from patients to detect and quantify circulating cancer biomarkers. Unlike conventional biopsy whereby primary tumor cells are analyzed, liquid biopsy enables the detection of a wide variety of circulating cancer biomarkers, including microRNA (miRNA), circulating tumor DNA (ctDNA), proteins, exosomes and circulating tumor cells (CTCs). Among the various techniques that have been developed to detect circulating cancer biomarkers, nanoplasmonic sensors represent a promising measurement approach due to high sensitivity and specificity as well as ease of instrumentation and operation. In this review, we discuss the relevance and applicability of three different categories of nanoplasmonic sensing techniques, namely surface plasmon resonance (SPR), localized surface plasmon resonance (LSPR) and surface-enhanced Raman scattering (SERS), for the detection of different classes of circulating cancer biomarkers.</P> <P><B>Graphical abstract</B></P> <P>[DISPLAY OMISSION]</P>

      • SCISCIESCOPUS

        Characterizing How Acidic pH Conditions Affect the Membrane-Disruptive Activities of Lauric Acid and Glycerol Monolaurate

        Valle-Gonzá,lez, Elba R.,Jackman, Joshua A.,Yoon, Bo Kyeong,Park, Soohyun,Sut, Tun Naw,Cho, Nam-Joon American Chemical Society 2018 Langmuir Vol.34 No.45

        <P>Fatty acids and monoglycerides are single-chain lipid amphiphiles that interact with phospholipid membranes as part of various biological activities. For example, they can exhibit membrane-disruptive behavior against microbial pathogens on the human skin surface. Supported lipid bilayers (SLBs) provide a useful experimental platform to characterize these membrane-disruptive behaviors, although related studies have been limited to neutral pH conditions. Herein, we investigated how lauric acid (LA) and glycerol monolaurate (GML) interact with SLBs and cause membrane morphological changes under acidic pH conditions that are representative of the human skin surface. Although LA induces tubule formation under neutral pH conditions, we discovered that LA causes membrane phase separation under acidic pH conditions. By contrast, GML induced membrane budding in both pH environments, although there was more extensive membrane remodeling under acidic pH conditions. We discuss these findings in the context of how solution pH affects the ionization states and micellar aggregation properties of LA and GML as well as its effect on the bending stiffness of lipid bilayers. Collectively, the findings demonstrate that solution pH plays an important role in modulating the interaction of fatty acids and monoglycerides with phospholipid membranes, and hence influences the scope and potency of their membrane-disruptive activities.</P> [FIG OMISSION]</BR>

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