Self-Assembly Strategy for Reducing Non-Specific Adsorption on Substrates and Application for Quantitative Immunoassay

Background The development of functionalized surfaces with low non-specific adsorption is important for biomedical applications. To inhibit non-specific adsorption on a substrate, we prepared a novel optical biochip based on a quantum dot fluorescence immunosorbent assay (QD-FLISA), specifically by modifying a layer of dense negatively charged film (SO32−) on the glass substrate surface via self-assembly. Results Using optimized conditions, we constructed a biochip on functionalized glass substrates to achieve quantitative detection of C-reactive protein (CRP). We subsequently achieved quantitative determination of CRP in the range of 1-1,000 ng/mL, with a limit of detection (LOD) of 1.26 ng/mL or 5.17 ng/mL, using poly(styrene sulfonic acid) sodium salt (PSS) or meso-tetra (4-sulfonatophenyl) porphine dihydrochloride (TSPP) on individually modified glass substrate biochips. The experimental protocol was further optimized and the LOD achieved a sensitivity of 0.69 ng/mL using functionalized TSPP and PSS co-treated glass substrate surfaces for the quantitative detection of CRP. Conclusions This work demonstrated an effective and convenient strategy to obtain biochips with low non-specific adsorption properties on functionalized surfaces, thus providing a new approach for creating ultra-high sensitivity microchannels or microarrays on glass substrates.

Hydrophilic and Hydrophobic Nanostructured Copper Surfaces for Efficient Pool Boiling Heat Transfer with Water, Water/Butanol Mixtures and Novec 649

Increasing heat dissipation requirements of small and miniature devices demands advanced cooling methods, such as application of immersion cooling via boiling heat transfer. In this study, functionalized copper surfaces for enhanced heat transfer are developed and evaluated. Samples are functionalized using a chemical oxidation treatment with subsequent hydrophobization of selected surfaces with a fluorinated silane. Pool boiling tests with water, water/1-butanol mixture with self-rewetting properties and a novel dielectric fluid with low GWP (Novec™ 649) are conducted to evaluate the boiling performance of individual surfaces. The results show that hydrophobized functionalized surfaces covered by microcavities with diameters between 40 nm and 2 µm exhibit increased heat transfer coefficient (HTC; enhancements up to 120%) and critical heat flux (CHF; enhancements up to 64%) values in comparison with the untreated reference surface, complemented by favorable fabrication repeatability. Positive surface stability is observed in contact with water, while both the self-rewetting fluids and Novec™ 649 gradually degrade the boiling performance and in some cases also the surface itself. The use of water/1-butanol mixtures in particular results in surface chemistry and morphology changes, as observed using SEM imaging and Raman spectroscopy. This seems to be neglected in the available literature and should be focused on in further studies.

Probing Multivalent Carbohydrate-Protein Interactions With On-Chip Synthesized Glycopeptides Using Different Functionalized Surfaces

Multivalent ligand–protein interactions are a commonly employed approach by nature in many biological processes. Single glycan–protein interactions are often weak, but their affinity and specificity can be drastically enhanced by engaging multiple binding sites. Microarray technology allows for quick, parallel screening of such interactions. Yet, current glycan microarray methodologies usually neglect defined multivalent presentation. Our laser-based array technology allows for a flexible, cost-efficient, and rapid in situ chemical synthesis of peptide scaffolds directly on functionalized glass slides. Using copper(I)-catalyzed azide–alkyne cycloaddition, different monomer sugar azides were attached to the scaffolds, resulting in spatially defined multivalent glycopeptides on the solid support. Studying their interaction with several different lectins showed that not only the spatially defined sugar presentation, but also the surface functionalization and wettability, as well as accessibility and flexibility, play an essential role in such interactions. Therefore, different commercially available functionalized glass slides were equipped with a polyethylene glycol (PEG) linker to demonstrate its effect on glycan–lectin interactions. Moreover, different monomer sugar azides with and without an additional PEG-spacer were attached to the peptide scaffold to increase flexibility and thereby improve binding affinity. A variety of fluorescently labeled lectins were probed, indicating that different lectin–glycan pairs require different surface functionalization and spacers for enhanced binding. This approach allows for rapid screening and evaluation of spacing-, density-, ligand and surface-dependent parameters, to find optimal lectin binders.

Synthesis and characterization of biological nanomaterial/poly(vinylidene fluoride) composites

The properties of composite materials are strongly influenced by both the physical and chemical properties of their individual constituents, as well as the interactions between them. For nanocomposites, the incorporation of nano-sized dopants inside a host material matrix can lead to significant improvements in mechanical strength, toughness, thermal or electrical conductivity, etc. In this work, the effect of cellulose nanofibrils on the structure and mechanical properties of cellulose nanofibril poly(vinylidene fluoride) (PVDF) composite films was investigated. Cellulose is one of the most abundant organic polymers with superior mechanical properties and readily functionalized surfaces. Under the current processing conditions, cellulose nanofibrils, as-received and 2,2,6,6-tetramethylpiperidine-1-oxyl radical (TEMPO) oxidized, alter the crystallinity and mechanical properties of the composite films while not inducing a crystalline phase transformation on the 𝛾 phase PVDF composites. Composite films obtained from hydrated cellulose nanofibrils remain in a majority 𝛾 phase, but also exhibit a small, yet detectable fraction of 𝛼 and ß PVDF phases.

Removal of Oily Contaminants from Water by Using the Hydrophobic Ag Nanoparticles Incorporated Dopamine Modified Cellulose Foam

The presence of oil-related contaminants in water has emerged as a severe threat to the environment. The separation of these contaminants from water has become a great challenge, and extensive efforts are being made to develop suitable, environmentally friendly materials. Highly hydrophobic materials are effective in the selective separation of oil from water. In this work, silver (Ag)-incorporated, highly hydrophobic dopamine-modified cellulose sponge was prepared by functionalizing with the range of alkyl silanes. The Ag nanoparticle-incorporated dopamine provided the appropriate roughness, whereas the alkyl component provided the low surface energy that made it selective towards oil. It was found that the alkyl groups with a longer chain length were more effective in enhancing the hydrophobicity of the Ag nanoparticle-incorporated, dopamine-modified cellulose. The developed materials were characterized by Fourier transform infrared spectroscopy (FTIR), field emission-scanning electron microscopy (FE-SEM), energy-dispersive X-ray spectroscopy (EDX), elemental mapping, and contact angle goniometry. The maximum water contact angle on the functionalized surfaces was observed at 148.4°. The surface of the C18s-Ag-DA-Cell-F showed excellent selectivity towards the oily component that rapidly permeated, and water was rejected wholly. The developed material showed a separation efficiency of 96.2% for the oil/water mixture. The C18s-Ag-DA-Cell-F material showed excellent reusability. Due to their environmentally friendly nature, excellent selectivity, and good separation efficiency, the functionalized cellulose materials can be used to separate oil and water effectively.

Surface Modification Enabling Reproducible Cantilever Functionalization for Industrial Gas Sensors

Micro-cantilever sensors are a known reliable tool for gas sensing in industrial applications. We have demonstrated the application of cantilever sensors on the detection of a meat freshness volatile biomarker (cadaverine), for determination of meat and fish precise expiration dates. For achieving correct target selectivity, the cantilevers need to be functionalized with a cadaverine-selective binder, based on a cyclam-derivative. Cantilever surface properties such as surface energy strongly influence the binder morphology and material clustering and, therefore, target binding. In this paper, we explore how chemical and physical surface treatments influence cantilever surface, binder morphology/clustering and binding capabilities. Sensor measurements with non-controlled surface properties are presented, followed by investigations on the binder morphology versus surface energy and cadaverine capture. We demonstrated a method for hindering binder crystallization on functionalized surfaces, leading to reproducible target capture. The results show that cantilever surface treatment is a promising method for achieving a high degree of functionalization reproducibility for industrial cantilever sensors, by controlling binder morphology and uniformity.

Metal-Free Fabrication of Fused Silica Extended Nanofluidic Channel to Remove Artifacts in Chemical Analysis

In microfluidics, especially in nanofluidics, nanochannels with functionalized surfaces have recently attracted attention for use as a new tool for the investigation of chemical reaction fields. Molecules handled in the reaction field can reach the single–molecule level due to the small size of the nanochannel. In such surroundings, contamination of the channel surface should be removed at the single–molecule level. In this study, it was assumed that metal materials could contaminate the nanochannels during the fabrication processes; therefore, we aimed to develop metal-free fabrication processes. Fused silica channels 1000 nm-deep were conventionally fabricated using a chromium mask. Instead of chromium, electron beam resists more than 1000 nm thick were used and the lithography conditions were optimized. From the results of optimization, channels with 1000 nm scale width and depth were fabricated on fused silica substrates without the use of a chromium mask. In nanofluidic experiments, an oxidation reaction was observed in a device fabricated by conventional fabrication processes using a chromium mask. It was found that Cr6+ remained on the channel surfaces and reacted with chemicals in the liquid phase in the extended nanochannels; this effect occurred at least to the micromolar level. In contrast, the device fabricated with metal-free processes was free of artifacts induced by the presence of chromium. The developed fabrication processes and results of this study will be a significant contribution to the fundamental technologies employed in the fields of microfluidics and nanofluidics.

Pool Boiling Performance of Water and Self-Rewetting Fluids on Hybrid Functionalized Aluminum Surfaces

The boiling performance of functionalized hybrid aluminum surfaces was experimentally investigated for water and self-rewetting mixtures of water and 1-butanol. Firstly, microstructured surfaces were produced via chemical etching in hydrochloric acid and the effect of the etching time on the surface morphology was evaluated. An etching time of 5 min was found to result in pitting corrosion and produced weakly hydrophilic microstructured surfaces with many microcavities. Observed cavity-mouth diameters between 3.6 and 32 μm are optimal for efficient nucleation and provided a superior boiling performance. Longer etching times of 10 and 15 min resulted in uniform corrosion and produced superhydrophilic surfaces with a micropeak structure, which lacked microcavities for efficient nucleation. In the second stage, hybrid surfaces combining lower surface energy and a modified surface microstructure were created by hydrophobization of etched aluminum surfaces using a silane agent. Hydrophobized surfaces were found to improve boiling heat transfer and their boiling curves exhibited a significantly lower superheat. Significant heat transfer enhancement was observed for hybrid microcavity surfaces with a low surface energy. These surfaces provided an early transition into nucleate boiling and promoted bubble nucleation. For a hydrophobized microcavity surface, heat transfer coefficients of up to 305 kW m−2 K−1 were recorded and an enhancement of 488% relative to the untreated reference surface was observed. The boiling of self-rewetting fluids on functionalized surfaces was also investigated, but a synergistic effect of developed surfaces and a self-rewetting working fluid was not observed. An improved critical heat flux was only obtained for the untreated surface, while a lower critical heat flux and lower heat transfer coefficients were measured on functionalized surfaces, whose properties were already tailored to promote nucleate boiling.