Nonspecific Interactions Research Articles

An AIEgen-based "turn-on" probe for sensing cancer cells and tiny tumors with high furin expression.

Peptide-aggregation-induced emission (AIE) luminogen (AIEgen) conjugates are widely used in the bioimaging field for their good resistance to photobleaching, red and near-infrared light emission, good biocompatibility, etc. However, their peptides are mainly negatively charged and the positively charged peptide-AIEgen conjugates are rarely used in in vivo imaging due to their high non-specific interaction with protein to cause "false-positive" results and their potential risk of triggering hemolysis. Herein, we introduce a black hole quencher 3 (BHQ3) to RVRRGFF-AIE (FA) to build a "turn-on" probe, named BHQ3-RVRRGFF-AIE (BFA). Compared with FA, BFA has advantages in the anti-interference ability for different proteins and many solution environments. But, both BFA and FA have high risks of inducing hemolysis, which restricts their further application. Through co-assembly with poly-γ-glutamic acid (γ-PGA), molecular probes BFA and FA are formed into PGA-BFA and PGA-FA nanoparticles with high biocompatibility and suppressed phototoxicity. Cell studies show that PGA-BFA can discriminate cancer cells with high furin expression from low furin-expressed cancer cells and normal cells. In vivo studies show that PGA-BFA can light up tiny tumors in the abdominal cavity with a better tumor-to-intestine ratio (3.14) than that of PGA-FA (1.47), which is helpful for the accurate excision of tiny tumors. This study will advance the development of constructing good biosafety probes with a high signal-to-noise ratio for fluorescence image-guided cancer surgery.

Rationalizing hydrogen bond solvation with Kamlet-Taft LSER and molecular torsion balances.

The strength of a weak intramolecular hydrogen bond was quantified using molecular torsion balances and found to vary between -0.99 kcal mol-1 and +1.00 kcal mol-1 due to solvation. Analyzing the results using Kamlet-Taft's Linear Solvation Energy Relationship enabled partitioning of the hydrogen-bond strength into physically meaningful solvent parameters through a linear equation: ΔGH-Bond = -1.37 - 0.14α + 2.10β + 0.74(π* - 0.38δ) kcal mol-1 (R2 = 0.99, n = 14), where α and β represent the solvent hydrogen-bond acceptor and donor parameters, respectively, and π* associates with the solvent nonspecific polarity/dipolarity parameter. Based on the coefficient of each solvent parameter (derived by linear regression), the β electrostatic term emerged as the dominant contributor to solvent effects on hydrogen bonding. This finding aligns with the natural attributes of hydrogen bonds as electrostatic interactions, but the contributions from the nonspecific interactions of the solvent (e.g., dispersion) are also important. Hydrogen bond solvation affects molecular properties and functions, and this study provides a predictive tool to harness the efficiency of hydrogen bonds.

Accurate calculation of second osmotic virial coefficients of proteins using mixed Poisson–Boltzmann and extended DLVO theory

New model xDLVO-CGhybr calculating second osmotic virial coefficient of protein solutions is developed. Data calculated agrees well with experiments due to accurate estimation of electrostatic protein–protein interactions using a hybrid methodology.

Synthesis and Characterization of Polyethylene Glycol-Grafted Photoreactive Polyethylene Glycols for Antibiofouling Applications.

Notably, antibiofouling is an important and predominant technique adopted to improve the surfaces of biomaterials. In this study, polyethylene glycol-grafted polyethylene glycols bearing azidophenyl groups were synthesized and immobilized on polystyrene surfaces via photoirradiation. The prepared polymers were found to be highly soluble in water, and photoimmobilization with fluorescent proteins was confirmed based on micropatterning using a photomask. These polymers suppressed nonspecific interactions between proteins and cells on the substrate. Considering that photoimmobilization can be adopted for the covalent bond modification of various surfaces, the developed water-soluble and highly antibiofouling polymers appear to be useful in biomaterial preparation.

Crowded Environment Regulates the Coacervation of Biopolymers via Nonspecific Interactions.

The membrane-less organelles (MLOs) with subcompartments are formed via liquid-liquid phase separation (LLPS) in the crowded cell interior whose background molecules are up to 400 mg/mL. It is still a puzzle how the background molecules regulate the formation, dynamics, and functions of MLOs. Using biphasic coacervate droplets formed by poly(l-lysine) (PLL), quaternized dextran (Q-dextran), and single-stranded oligonucleotides (ss-oligo) as a model of MLO, we online monitored the LLPS process in Bovine Serine Albumin (BSA) solution up to 200.0 mg/mL. Negatively charged BSA is able to form complex or coacervate with positively charged PLL and Q-dextran and thus participates in the LLPS via nonspecific interactions. Results show that BSA effectively regulates the LLPS by controlling the phase distribution, morphologies, and kinetics. With increasing BSA concentration, the spherical biphasic droplets evolve in sequence into phase-inverted flower-like structure, worm-like chains, network structures, and confined coacervates. Each kind of morphology is formed via its own specific growth and fusion pathway. Our work suggests that MLOs could be controlled solely by the crowded environment and provides a further step toward understanding the life process in cell.

Specific and Nonspecific Interactions of Yersinia pseudotuberculosis Lipopolysaccharide with Monoclonal Antibodies Assessed by Atomic Force Microscopy

Specific and Nonspecific Interactions of Yersinia pseudotuberculosis Lipopolysaccharide with Monoclonal Antibodies Assessed by Atomic Force Microscopy

Interaction of Graphitic Carbon Nitride with Cell Membranes: Probing Phospholipid Extraction and Lipid Bilayer Destruction.

Understanding how nanomaterials interact with cell membranes has important implications for ecotoxicology and human health. Here, we investigated the interactions between graphitic carbon nitride (g-C3N4, CN) and red blood cells, a plausible contact target for nanoparticles when they enter the bloodstream. Through a hemolysis assay, the cytotoxicity of CN derived from different precursors was quantitatively assessed, which is highly related to the surface area of CN. Reactive oxygen species (ROS) generation and lipid peroxidation detection confirmed that CN causes rapid cell membrane rupture by a physical interaction mechanism rather than ROS-related chemical oxidation. Dye leakage assay and theoretical simulation indicated that the less-layered CN is prone to folding inward to wrap and extract lipid molecules from cell membranes. The electron-rich inherent pores of CN play a dominant role in capturing the headgroups of phospholipids, whereas the hydrophobic interaction is critical for the anchoring of lipid tails. Our further experimental evidence demonstrated that the destructive extraction of phospholipids from cell membranes by CN occurs primarily in the outer leaflet, and phosphatidylcholine is the most easily extracted lipid. Moreover, the formation of protein corona on CN was found to decrease the nonspecific interactions but increase steric repulsion, thus mitigating CN cytotoxicity. Overall, our data provide a molecular basis for CN's cytotoxicity.

Effect of Surfactants on the Binding Properties of a Molecularly Imprinted Polymer.

In molecularly imprinted polymers, non-specific interactions are generally based on weak forces between the polymer surface and the sample matrix. Thus, additives able to interfere with such interactions should be able to significantly reduce any non-specific binding effect. Surfactants represent an interesting class of substances as they are cheap and easily available. Here, we present a study of the effect of three surfactants (the anionic sodium dodecylsulphate, SDS, the cationic cetyltrimethylammonium bromide (CTAB) and the non-ionic polyoxyethylene-(20)-sorbitan monolaurate Tween 20) on the binding affinity of a 2,4,5-trichlorophenoxyacetic acid (2,4,5-T)-imprinted polymer for the template and its analogue 2,4-dichlorophenoxyacetic acid (2,4-D). The experimental results indicate that increasing amounts of surfactant decrease the binding affinity for the ligands strongly for the ionic ones, and more weakly for the non-ionic one. This effect is general, as it occurs for both 2,4,5-T and 2,4-D and for both the imprinted and the not-imprinted polymers. It also proves that the magnitude of this effect mainly depends on the presence or absence of an ionic charge, and that the hydrophobic "tail" of surfactants plays only a minor role.

Surface Control of Nanodiamond: From Homogeneous Termination to Complex Functional Architectures for Biomedical Applications.

ConspectusInterest in nanodiamond (ND) has been spurred by its unique properties such as high biocompatibility, versatile surface chemistry, and the possibility to apply it as drug delivery agent, cross-linker, or coating and for sensing applications when luminescent lattice defects such as the NV centers are present in the crystal lattice. Currently, nanodiamond has been used for targeted drug delivery, phototherapeutic applications, and sensing and imaging in cellular environments and in vitro. Furthermore, suitably functionalized nanodiamond is a promising material for tissue engineering applications. However, the application of nanodiamond has long been hampered by a number of obstacles and challenges met with commercially available nanodiamonds of different origins. A major issue is related to the strong agglomeration of the individual particles resulting in covalently linked aggregates with larger sizes and a broad size distribution. Furthermore, the surface termination of typical nanodiamond particles tends to be rather inhomogeneous, containing a multitude of different functional groups. The retention of functionality of immobilized moieties for bioapplications is often not known. And finally, the surface of nanodiamond possesses a strong propensity for nonspecific interaction, especially proteins from serum, cell fluids, or the culture media used for the incubation of cells with nanodiamond. The resulting protein corona influences the possibility to access functional moieties on the diamond surface and leads to a reduced reproducibility of observations in physiological environments and a limited attribution of effects to the presence of the functional moieties on the diamond surface. In this Account, we describe our efforts to address these challenges using multiple strategies mainly for the example of detonation nanodiamond (DND). First, a homogeneous size distribution of the nanoparticles and an initial surface termination with a unique type of atoms or groups can be achieved using mechanochemical methods and treatments with different reagents in both solution and gas phases. Reactions in liquid media typically lead to more uniform results as the entire surface of the particles becomes equally accessible. We have then worked on the development of different covalent linker strategies to accommodate the grafting needs of different functional moieties and thus to enable the production of orthogonally functionalized ND particles, which can be modified with multiple moieties in a controlled fashion. The noncovalent immobilization of functional units is equally useful as it permits the conservation of functionality for sensitive proteins, which denature upon covalent immobilization. In summary, our work aims to gain full control over the surface properties of diamond nanoparticles and to develop a toolbox of chemical methods to provide functionalized and tailored nanodiamond for a plethora of biomedical applications. Further research in the field of diamond functionalization will cover also the transfer of already existing methods to other types of diamond surfaces, the production of stoichiometrically functionalized particles, the covalent and dynamic self-assembly of nanodiamond particles, and the continuing development of suitable characterization techniques.

Preparation of miniaturized hydrophilic affinity monoliths: Towards a reduction of non-specific interactions and an increased target protein density

In affinity chromatography, non-specific interactions between the ligands and the affinity column may affect the results, leading to misinterpretations during the investigation of protein-ligand interactions (detection of false positives in ligand screening, lack of specificity in purification). Such non-specific interactions may arise both from the underlying support or from the target protein itself. If the second ones are protein-dependent (and cannot be studied in a general framework), the first ones occur in the same way regardless of the immobilized target. We propose a methodology to identify the origin of such non-specific interactions with the underlying material of the affinity column. This methodology relies on the systematic investigation of the retention behavior of a set of 41 low-molecular weight compounds covering a wide chemical space (net charge, log D, functionality). We first demonstrate that the main source of non-specific interactions on the most commonly used GMA-co-EDMA monolith comes from hydrophobic effects. To reduce such non-specific interactions, we developed a new hydrophilic glycidyl methacrylate-based monolith by replacing the EDMA crosslinker by the more hydrophilic NN’ Methylenebisacrylamide (MBA). Optimization of the synthesis parameters (monomer content, initiation type, temperature) has focused on the reduction of non-specific interaction with the monolithic support while maximizing the amount of protein that can be grafted onto the monolith at the issue of its synthesis. The retention data of the 41 test solutes on the new poly(GMA-co-MBA) monolith shows a drastic reduction of non-specific interactions except for cationic compounds. The particular behavior of cationic compounds is due to their electrostatic interactions with carboxylic groups resulting from the partial acidic hydrolysis of amide groups of MBA during the epoxide ring opening step. So, the ring opening step in acidic media was replaced by a hot water treatment to avoid side reaction on MBA. The new monolith poly(GMA-co-MBA) not only has improved hydrophilic surface properties but also a higher protein density (16 ± 0.8 pmol cm−1 instead of 8 ± 0.3 pmol cm−1). To highlight the benefits of this new hydrophilic monolith for affinity chromatographic studies, frontal affinity chromatography experiments were conducted on these monoliths grafted with con A.

Serotype-dependent adhesion of Shiga toxin-producing Escherichia coli to bovine milk fat globule membrane proteins.

Shiga toxin-producing Escherichia coli (STEC) are food-borne pathogens that can cause severe symptoms for humans. Raw milk products are often incriminated as vehicule for human STEC infection. However, raw milk naturally contains molecules, such as the milk fat globule membrane and associated proteins, that could inhibit pathogen adhesion by acting as mimetic ligands. This study aimed to: (i) evaluate the capability of STEC cells to adhere to bovine milk fat globule membrane proteins (MFGMPs), (ii) highlight STEC surface proteins associated with adhesion and (iii) evaluate the variation between different STEC serotypes. We evaluated the physicochemical interactions between STEC and milk fat globules (MFGs) by analyzing hydrophobic properties and measuring the ζ-potential. We used a plate adhesion assay to assess adhesion between MFGMPs and 15 Escherichia coli strains belonging to three key serotypes (O157:H7, O26:H11, and O103:H2). A relative quantitative proteomic approach was conducted by mass spectrometry to identify STEC surface proteins that may be involved in STEC-MFG adhesion. The majority of E. coli strains showed a hydrophilic profile. The ζ-potential values were between -3.7 and - 2.9 mV for the strains and between -12.2 ± 0.14 mV for MFGs. Our results suggest that non-specific interactions are not strongly involved in STEC-MFG association and that molecular bonds could form between STEC and MFGs. Plate adhesion assays showed a weak adhesion of O157:H7 E. coli strains to MFGMPs. In contrast, O26:H11 and O103:H2 serotypes attached more to MFGMPs. Relative quantitative proteomic analysis showed that the O26:H11 str. 21,765 differentially expressed five outer membrane-associated proteins or lipoproteins compared with the O157:H7 str. EDL933. This analysis also found strain-specific differentially expressed proteins, including four O26:H11 str. 21,765-specific proteins/lipoproteins and eight O103:H2 str. PMK5-specific proteins. For the first time, we demonstrated STEC adhesion to MFGMPs and discovered a serotype effect. Several outer membrane proteins-OmpC and homologous proteins, intimin, Type 1 Fimbriae, and AIDA-I-that may be involved in STEC-MFG adhesion were highlighted. More research on STEC's ability to adhere to MFGMs in diverse biological environments, such as raw milk cheeses and the human gastrointestinal tract, is needed to confirm the anti-adhesion properties of the STEC-MFG complex.

Photophysical properties of push-pull monocationic D-π-A+ thiophene based derivatives: Fluorosolvatochromism and pH studies

Photophysical properties of two thiophene salts of the form D-π-A+ are studied in several solvents and at various pH values of the aqueous solution. The studied compounds embrace methoxy group as electron donating moiety at one end and cationic amidine group with and without fluorine atom at the ortho position of the amidine group as the electron withdrawing group at the other end of the molecules and separated by thiophene ring. The two thiophene derivatives are 4-(5-(4-methoxyphenyl)thiophen-2-yl)benzamidine hydrochloride salt (MOTB) and 2-fluoro-4-(5-(4-methoxyphenyl) thiophen-2-yl)benzamidine hydrochloride salt (FMOTB). The observed changes in the fluorescence emission spectra with the nature of the solvent were found to be much more pronounced than the corresponding absorption spectra which signify an emission from the intramolecular charge transfer state. The higher bathochromic shift in the fluorescence emission spectra than the absorption spectra indicates that the excited state dipole moment is larger than that of the ground state. It has also been observed that the presence of the fluorine atom in the electron withdrawing part does not show any changes in the absorption spectra while a clear bathochromic shift is observed in the fluorescence emission spectra indicating an enhanced strength of the electron withdrawing ability in case of FMOTB. Effect of pH was also studied and pKa values were evaluated. The observed photophysical properties were correlated to the normalized solvent polarity parameter (ETN) when solvents are classified to protic and aprotic solvents. This designates the importance of hydrogen bonding interactions. We have also applied a couple of linear solvation energy relationships for better understanding of the exact contribution of each solvent parameter on each photophysical property. We have found that both Catalán’s and Laurence’s treatments show that the photophysical properties are mainly controlled by the solvent’s non-specific interactions. However, these models were not sufficient to interpret the observed data without the inclusion of the participation of the specific interactions.

Non-specificity as the sticky problem in therapeutic antibody development.

Antibodies are highly potent therapeutic scaffolds with more than a hundreddifferent products approved on the market. Successful development of antibody-based drugs requires a trade-off between high target specificity and target binding affinity. In order to better understand this problem, we here review non-specific interactions and explore their fundamental physicochemical origins. We discuss the role of surface patches - clusters of surface-exposed amino acid residues with similar physicochemical properties - as inducers of non-specific interactions. These patches collectively drive interactions including dipole-dipole, π-stacking and hydrophobic interactions to complementary moieties. We elucidate links between these supramolecular assembly processes and macroscopic development issues, such as decreased physical stability and poor in vivo half-life. Finally, we highlight challenges and opportunities for optimizing protein binding specificity and minimizing non-specificity for future generations of therapeutics.

Spectral characteristics of 3,5-diaminobenzoic acid in pure and mixed solvents: Experimental and theoretical study

The effect of solvents on the absorption and fluorescence (FL) spectra of 3,5-diaminobenzoic acid (DABA) was explored in pure solvents of diverse polarities and hydrogen bonding abilities. A bathochromic shift was observed in FL spectra while moving from non-polar to polar aprotic/protic solvents. The solvatochromic-based approaches showed that the dipole moment of DABA in the excited state (ES) is higher than its ground state (GS), which signifies that the ES is more polarized, corresponding to the GS. Moreover, the Catalan solvent polarity scale analysis suggested that the solvent acidity (SA) and dipolarity (SdP) influenced the absorption and FL spectra of DABA in solvents, signifying the presence of non-specific and specific interactions. The FL decay analysis in solvents was correlated with the observed steady-state results and suggested the presence of intramolecular charge transfer (ICT). The preferential solvation concept was utilized to understand the spectral variations of DABA in MeOH-water and DMSO-water mixtures. Further, the computational calculations utilizing the DFT (density functional theory) and TD-DFT (its time extension) for DABA were performed in the gas phase and solvents to estimate the electronic transitions and dipole moments. Furthermore, the natural bond orbital analysis and non-linear optical parameters were also obtained by DFT, and the findings revealed that ICT stabilizes the molecular system. Thus, DABA may have potential applications in the field of optoelectronics and fluorescence sensing.

Narrowing the pore size distribution of polyamide nanofiltration membranes via dragging piperazines to enhance ion selectivity

Traditional polyamide nanofiltration membranes often can't obtain ideal ion selectivity due to their wide pore size distribution. In this work, a β-cyclodextrin modified sodium hyaluronate (HA-CD) was introduced to achieve the dragging effect of piperazine by non-specific hydrogen bond interaction between HA-CD and substrate and piperazine, thus realizing the purpose of sustained release of piperazine. The MD simulation results demonstrated that the diffusion rate of piperazine was reduced by approximately two orders of magnitude due to the interaction effect. In addition to making the polyamide layer thinner and smoother, HA-CD also narrows the pore size distribution. The salt filtration test showed that the prepared membrane has excellent anion selectivity (αmax:114) and permeability (10.66 L m−2 h−1 bar−1). Long-term filtration and nano-scratch test results demonstrated that the prepared membranes have good operational stability (the permeability only decreased about 30%) and mechanical strength (the interface bonding strength increased about 270%). By exploring the effect of the interaction between HA-CD and substrate and piperazine on the interfacial polymerization process, which proved the feasibility of realizing high permeability selectivity and stability of the membrane by constructing the functional bridge between substrates and aqueous monomers.

How Choice of Model Membrane Affects Protein-Glycosphingolipid Interactions: Insights from Native Mass Spectrometry.

Interactions between glycan-binding proteins (GBPs) and glycosphingolipids (GSLs) are involved in numerous physiological and pathophysiological processes. Many model membrane systems are available for studying GBP-GSL interactions, but a systematic investigation has not been carried out on how the nature of the model membrane affects binding. In this work, we use electrospray ionization mass spectrometry (ESI-MS), both direct and competitive assays, to measure the binding of cholera toxin B subunit homopentamer (CTB5) to GM1 ganglioside in liposomes, bilayer islands [styrene maleic acid lipid particles (SMALPs), nanodiscs (NDs), and picodiscs (PDs)], and micelles. We find that direct ESI-MS analysis of CTB5 binding to GM1 is unreliable due to non-uniform response factors, incomplete extraction of bound GM1 in the gas phase, and nonspecific CTB5-GM1 interactions. Conversely, indirect proxy ligand ESI-MS measurements show that the intrinsic (per binding site) association constants of CTB5 for PDs, NDs, and SMALPs are similar and comparable to the affinity of soluble GM1 pentasaccharide (GM1os). The observed affinity decreases with increasing GM1 content due to molecular crowding stemming from GM1 clustering. Unlike the smaller model membranes, the observed affinity of CTB5 toward GM1 liposomes is ∼10-fold weaker than GM1os and relatively insensitive to the GM1 content. GM1 glycomicelles exhibit the lowest affinity, ∼35-fold weaker than GM1os. Together, the results highlight experimental design considerations for quantitative GBP-GSL binding studies involving multisubunit GBPs and factors to consider when comparing results obtained with different membrane systems. Notably, they suggest that bilayer islands with a low percentage of GSL, wherein clustering is minimized, are ideal for assessing intrinsic strength of GBP-GSL interactions in a membrane environment, while binding to liposomes, which is sub-optimal due to extensive clustering, may be more representative of authentic cellular environments.

On the Influence of Nucleic Acid Backbone Modifications on Lipid Nanoparticle Morphology.

Nucleic acid therapeutics represent a major advance toward treating diseases at their root cause. However, nucleic acids are prone to degradation by serum endonucleases, clearance through the immune system, and rapid degradation in complex medium. To overcome these barriers, nucleic acids frequently include chemical modifications to improve stability or decrease immune responses. Lipid nanoparticles (LNPs) have enabled a dramatic reduction in the dose required to achieve a therapeutic effect by protecting these nucleic acids and improving their intracellular delivery. It has been assumed thus far that nonspecific ionic interactions drive LNP formation and chemical modifications to the nucleic acid backbone to confer improved stability do not impact LNP delivery in any way. Here, we demonstrate that these chemical modifications do impact LNP morphology substantially, and phosphorothioate modifications produce stronger interactions with ionizable amino lipids, resulting in enhanced entrapment. This work represents a major first step toward greater understanding of the interaction between the lipid components and nucleic acids within an LNP.

Recognition and movement of polystyrene nanoplastics in fish cells

Although nanoplastics are being increasingly scrutinized, little is known about their kinetic behavior in living organisms, especially in cellular systems. Herein, nonspecific interactions of three polystyrene nanoplastics (pristine-PS, NH2-PS, and COOH-PS, with size range of 90–100 nm and at concentrations of 0–100 μg mL−1) with zebrafish cells were quantified for their cellular uptake and exocytosis. Cell uptake of nanoplastics reached a peak within 2 h and then decreased. The overall nanoplastics uptake was dominated by PS-particle internalization. The estimated uptake rate was comparable among the different types of PS (pristine-PS, NH2-PS, and COOH-PS), but the uptake capacity was related to their functionality. The clathrin-mediated and caveolae-mediated pathways were mainly involved in the uptake of the three nanoplastics. The internalized PS-particles were initially delivered to the cytoplasm but then transported to lysosomes using energy. Meanwhile, these PS particles were released by the cells via energy-free penetration and energy-dependent lysosomal exocytosis. PS-particles were removed by the cells at a relatively slow rate, and the estimated retention half-lives of these PS-particles were 10.1 h, 12.0 h and 15.1 h for pristine-PS, NH2-PS and COOH-PS particles, respectively, in fish cells based on our kinetic measurements. Intracellular trajectory modeling of nanoplastics movement is critical for the environmental and human health risk assessment.

SOI-FET Sensors with Dielectrophoretic Concentration of Viruses and Proteins.

Quick label-free virus screening and highly sensitive analytical tools/techniques are becoming extremely important in a pandemic. In this study, we developed a biosensing device based on the silicon nanoribbon multichannel and dielectrophoretic controlled sensors functionalized with SARS-CoV-2 spike antibodies for the use as a platform for the detection and studding of properties of viruses and their protein components. Replicatively defective viral particles based on vesicular stomatitis viruses and HIV-1 were used as carrier molecules to deliver the target SARS-CoV-2 spike S-proteins to sensory elements. It was shown that fully CMOS-compatible nanoribbon sensors have the subattomolar sensitivity and dynamic range of 4 orders. Specific interaction between S-proteins and antibodies leads to the accumulation of the negative charge on the sensor surface. Nonspecific interactions of the viral particles lead to the positive charge accumulation. It was shown that dielectrophoretic controlled sensors allow to estimate the effective charge of the single virus at the sensor surface and separate it from the charge associated with the binding of target proteins with the sensor surface.

Detection and binding interactions of pharmaceutical contaminants using quartz crystal microbalance – Role of adsorbate structure and surface functional group on adsorption

HypothesisEmerging contaminants (ECs) can interact with soft solid/aqueous interfaces of particulate organic matter and microplastics in the aquatic environment but to what extent? It is hypothesized that EC adsorption can be detected using quartz crystal microbalance (QCM), a sensitive gravimetric tool, and their adsorption energetics and uptake capacity can be measured for various substrates of distinct functional group. This in turn reveals the specific vs. nonspecific interactions. ExperimentsQCM has been used to detect and measure the adsorption of selected pharmaceuticals, amlodipine (AMP) and carbamazepine (CBZ), onto butyl, carboxyl, amine, and phenyl functionalized self-assembled monolayers (SAMs), mapping out the hydrophobic effect, H-bonding capability, and π− interactions. Adsorption free energy (ΔGads) and maximum interfacial concentration (cmax) for these surfaces are compared. Solvatochromic studies to elucidate the likelihood of H-bonding interactions for CBZ and AMP have been conducted using UV–Vis absorption spectroscopy. FindingsAmlodipine and carbamazepine adsorb onto butyl/aqueous interface with respective ΔGads values of −35.8 ± 1.1 and −37.7 ± 0.1 kJ/mol. Nonspecific interaction allows a greater extent of cmax on the hydrophobic/aqueous interface. CBZ does not bind to the phenyl surface. AMP and CBZ exhibit H-bonding and show proclivity for the amine and carboxyl SAMs. Interfacial chemical environment and adsorbate structural properties play a significant role on EC adsorption.