Acoustofluidics-Assisted Engineering of Multifunctional Three-Dimensional Zinc Oxide Nanoarrays.
ABSTRACT: The integration of acoustics and microfluidics (termed acoustofluidics) presents a frontier in the engineering of functional micro-/nanomaterials. Acoustofluidic techniques enable active and precise spatiotemporal control of matter, providing great potential for the design of advanced nanosystems with tunable material properties. In this work, we introduce an acoustofluidic approach for engineering multifunctional three-dimensional nanostructure arrays and demonstrate their potential in enrichment and biosensing applications. In particular, our acoustofluidic device integrates an acoustic transducer with a sharp-edge-based acoustofluidic reactor that enables uniform patterning of zinc oxide (ZnO) nanoarrays with customizable lengths, densities, diameters, and other properties. The resulting ZnO nanoarray-coated glass capillaries can rapidly and efficiently capture and enrich biomolecules with sizes ranging from a few nanometers to several hundred nanometers. In order to enable the detection of these biomolecules, silver (Ag) nanoparticles are deposited onto the ZnO nanoarrays, and the integrated ZnO-Ag capillary device functions as a label-free plasmonic biosensing system for surface-enhanced Raman spectroscopy (SERS) based detection of exosomes, DNA oligonucleotides, and E. coli bacteria. The optical sensing enhancement of ZnO-Ag capillary is further validated through finite-difference time-domain (FDTD) simulations. These findings not only provide insights into the engineering of functional micro/nanomaterials using acoustofluidics but also shed light onto the development of portable microanalytical devices for point-of-care applications.
Project description:Synthesis of nanoparticles and particulate nanomaterials with tailored properties is a central step toward many applications ranging from energy conversion and imaging/display to biosensing and nanomedicine. While existing microfluidics-based synthesis methods offer precise control over the synthesis process, most of them rely on passive, partial mixing of reagents, which limits their applicability and potentially, adversely alter the properties of synthesized products. Here, an acoustofluidic (i.e., the fusion of acoustic and microfluidics) synthesis platform is reported to synthesize nanoparticles and nanomaterials in a controllable, reproducible manner through acoustic-streaming-based active mixing of reagents. The acoustofluidic strategy allows for the dynamic control of the reaction conditions simply by adjusting the strength of the acoustic streaming. With this platform, the synthesis of versatile nanoparticles/nanomaterials is demonstrated including the synthesis of polymeric nanoparticles, chitosan nanoparticles, organic-inorganic hybrid nanomaterials, metal-organic framework biocomposites, and lipid-DNA complexes. The acoustofluidic synthesis platform, when incorporated with varying flow rates, compositions, or concentrations of reagents, will lend itself unprecedented flexibility in establishing various reaction conditions and thus enable the synthesis of versatile nanoparticles and nanomaterials with prescribed properties.
Project description:Biomolecular engineering can be used to purposefully manipulate biomolecules, such as peptides, proteins, nucleic acids and lipids, within the framework of the relations among their structures, functions and properties, as well as their applicability to such areas as developing novel biomaterials, biosensing, bioimaging, and clinical diagnostics and therapeutics. Nanotechnology can also be used to design and tune the sizes, shapes, properties and functionality of nanomaterials. As such, there are considerable overlaps between nanotechnology and biomolecular engineering, in that both are concerned with the structure and behavior of materials on the nanometer scale or smaller. Therefore, in combination with nanotechnology, biomolecular engineering is expected to open up new fields of nanobio/bionanotechnology and to contribute to the development of novel nanobiomaterials, nanobiodevices and nanobiosystems. This review highlights recent studies using engineered biological molecules (e.g., oligonucleotides, peptides, proteins, enzymes, polysaccharides, lipids, biological cofactors and ligands) combined with functional nanomaterials in nanobio/bionanotechnology applications, including therapeutics, diagnostics, biosensing, bioanalysis and biocatalysts. Furthermore, this review focuses on five areas of recent advances in biomolecular engineering: (a) nucleic acid engineering, (b) gene engineering, (c) protein engineering, (d) chemical and enzymatic conjugation technologies, and (e) linker engineering. Precisely engineered nanobiomaterials, nanobiodevices and nanobiosystems are anticipated to emerge as next-generation platforms for bioelectronics, biosensors, biocatalysts, molecular imaging modalities, biological actuators, and biomedical applications.
Project description:Ag and Ni/ZnO photocatalyst nanostructures were successfully synthesized by a sol-gel method. In this work, the photocatalyst sample was systematically studied based on several factors affecting the performance of photocatalyst, which are size, morphology, band gap, textural properties and the number of active sites presence on the surface of the nanocatalyst. X-ray diffraction revealed that Ag/ZnO nanomaterials experienced multiple phases, meanwhile for Ni/ZnO the phase of nanomaterials were pure and single phase for stoichiometry less than 5%. Field emission scanning electron microscope (FESEM) showed almost all of the synthesized nanomaterials possessed a mixture of nanorods and spherical-like shape morphology. The Ag/ZnO showed high photocatalytic activity, producing at least 14th trials of nanocatalyst reusability on degradation of methyl orange under UV irradiation. Interestingly, this phenomenon was not observed in larger surface area of Ni/ZnO nanomaterials which supposedly favour photocatalytic activity, but instead producing poor photocatalytic performance. The main reasons were studied and exposed by temperature-programmed desorption of carbon dioxide (TPD-CO2) which showed that incorporation of Ag into ZnO lattice has enhanced the number of active sites on the surface of the nanocatalyst. Whereas incorporation of Ni in ZnO has lowered the number of active sites with respect to undoped ZnO. Active sites measurement is effective and significant, providing opportunities in developing an intensive study as an additional factor.
Project description:Nanobiohybrids, synthesized by integrating functional nanomaterials with living systems, have emerged as an exciting branch of research at the interface of materials engineering and biological science. Nanobiohybrids use synthetic nanomaterials to impart organisms with emergent properties outside their scope of evolution. Consequently, they endow new or augmented properties that are either innate or exogenous, such as enhanced tolerance against stress, programmed metabolism and proliferation, artificial photosynthesis, or conductivity. Advances in new materials design and processing technologies made it possible to tailor the physicochemical properties of the nanomaterials coupled with the biological systems. To date, many different types of nanomaterials have been integrated with various biological systems from simple biomolecules to complex multicellular organisms. Here, we provide a critical overview of recent developments of nanobiohybrids that enable new or augmented biological functions that show promise in high-tech applications across many disciplines, including energy harvesting, biocatalysis, biosensing, medicine, and robotics.
Project description:Over the past several decades, a litany of acoustofluidic devices have been developed which purport to have significant advantages over traditional benchtop analytical tools. These acoustofluidic devices are frequently labeled as "labs-on-chips"; however, many do an insufficient job of limiting their dependence on the lab. Often, acoustofluidic devices still require skilled operators and complex external equipment. In an effort to address these shortcomings, we developed a low-cost, expandable, and multifunctional system for controlling acoustofluidic devices in the audible to low ultrasonic frequency range (31 Hz to 65 kHz). The system was designed around the readily available Arduino prototyping platform because of its user-friendly coding environment and expansive network of open source material; these factors enabled us to create a system capable of generating high voltage oscillatory signals and controlling microscale flows in acoustofluidic devices. Utilizing the established open source system, we achieved a series of acoustofluidic applications involving the manipulation of fluids and biological objects in a portable fashion. In particular, we used our open source acoustofluidic devices to achieve active rotation of cells and microorganisms, and operation of an acoustofluidic mixing device which has previously shown potential for viscous sample preparation, in a portable fashion. Additionally, using low frequency flexural waves and our portable system, we achieved acoustofluidic separation of particles based on size. It is our hope that the open source platform presented here can pave the way for future acoustofluidic devices to be used at the point-of-care, as well as simplify the operation of these devices to enable resource limited users to leverage the benefits of acoustofluidics in their work.
Project description:Nanomaterials for highly selective and sensitive sensors toward specific gas molecules of volatile organic compounds (VOCs) are most important in developing new-generation of detector devices, for example, for biomarkers of diseases as well as for continuous air quality monitoring. Here, we present an innovative preparation approach for engineering sensors, which allow for full control of the dopant concentrations and the nanoparticles functionalization of columnar material surfaces. The main outcome of this powerful design concept lies in fine-tuning the reactivity of the sensor surfaces toward the VOCs of interest. First, nanocolumnar and well-distributed Ag-doped zinc oxide (ZnO:Ag) thin films are synthesized from chemical solution, and, at a second stage, noble nanoparticles of the required size are deposited using a gas aggregation source, ensuring that no percolating paths are formed between them. Typical samples that were investigated are Ag-doped and Ag nanoparticle-functionalized ZnO:Ag nanocolumnar films. The highest responses to VOCs, in particular to (CH3)2CHOH, were obtained at a low operating temperature (250 °C) for the samples synergistically enhanced with dopants and nanoparticles simultaneously. In addition, the response times, particularly the recovery times, are greatly reduced for the fully modified nanocolumnar thin films for a wide range of operating temperatures. The adsorption of propanol, acetone, methane, and hydrogen at various surface sites of the Ag-doped Ag8/ZnO(0001) surface has been examined with the density functional theory (DFT) calculations to understand the preference for organic compounds and to confirm experimental results. The response of the synergistically enhanced sensors to gas molecules containing certain functional groups is in excellent agreement with density functional theory calculations performed in this work too. This new fabrication strategy can underpin the next generation of advanced materials for gas sensing applications and prevent VOC levels that are hazardous to human health and can cause environmental damages.
Project description:Comparative hazard identification of nanomaterials (NMs) can aid in the prioritisation for further toxicity testing. Here, we assessed the acute lung, systemic and liver responses in C57BL/6N mice for three NMs to provide a hazard ranking. A silver (Ag), non-functionalised zinc oxide (ZnO) and a triethoxycaprylylsilane functionalised ZnO NM suspended in water with 2% mouse serum were examined 24 hours following a single intratracheal instillation (I.T.). An acute pulmonary inflammation was noted (marked by a polymorphonuclear neutrophil influx) with cell damage (LDH and total protein) in broncho-alveolar lavage fluid (BALF) after administration of both non-functionalised and functionalised ZnO. The latter also induced systemic inflammation measured as an increase in blood neutrophils and a decrease in blood lymphocytes. Exposure to Ag NM was not accompanied by pulmonary inflammation or cytotoxicity, or by systemic inflammation. A decrease in glutathione levels was demonstrated in the liver following exposure to high doses of all three nanomaterials irrespective of any noticeable inflammatory or cytotoxic effects in the lung. By applying benchmark dose (BMD) modeling statistics to compare potencies of the NMs, we rank functionalised ZnO ranked the highest based on the largest number of affected endpoints, as well as the strongest responses observed after 24 hours. The non-functionalised ZnO NM gave an almost similar response, whereas Ag NM did not cause an acute response at similar doses.
Project description:The precise manipulation of acoustic fields in microfluidics is of critical importance for the realization of many biomedical applications. Despite the tremendous efforts devoted to the field of acoustofluidics during recent years, dexterous control, with an arbitrary and complex acoustic wavefront, in a prescribed, microscale region is still out of reach. Here, we introduce the concept of acoustofluidic waveguide, a three-dimensional compact configuration that is capable of locally guiding acoustic waves into a fluidic environment. Through comprehensive numerical simulations, we revealed the possibility of forming complex field patterns with defined pressure nodes within a highly localized, pre-determined region inside the microfluidic chamber. We also demonstrated the tunability of the acoustic field profile through controlling the size and shape of the waveguide geometry, as well as the operational frequency of the acoustic wave. The feasibility of the waveguide concept was experimentally verified via microparticle trapping and patterning. Our acoustofluidic waveguiding structures can be readily integrated with other microfluidic configurations and can be further designed into more complex types of passive acoustofluidic devices. The waveguide platform provides a promising alternative to current acoustic manipulation techniques and is useful in many applications such as single-cell analysis, point-of-care diagnostics, and studies of cell-cell interactions.
Project description:Zinc oxide nanoparticles (ZnO NPs) are applied in various applications in catalysis, biosensing, imaging, and as antibacterial agents. Here we to prepare ZnO nanomaterials decorated by <i>?</i>-amino butyric acid (GABA), curcumin derivatives (CurBF<sub>2</sub>) and silver nanoparticles (CurBF<sub>2</sub>-AgNPs). The structures of all ZnO nanostructures were characterized using Fourier transform infrared (FT-IR) spectroscopy, X-ray diffraction (XRD), UV-VIS spectrophotometry, fluorescence spectrophotometry, scanning electron microscopy (SEM), transmission electron microscopy (TEM), and high-resolution transmission electron microscopy (HR-TEM). Further, their antibacterial activities against Gram-negative (<i>Escherichia coli</i>) and Gram-positive (<i>Staphylococcus aureus</i>) bacteria were investigated through analysis of minimum inhibitory concentration (MIC) method. Among the prepared nanostructures, the ZnO NPs-GABA/CurBF<sub>2</sub>-AgNPs showed excellent antibacterial activity against both Gram-positive and -negative bacteria. ZnO NPs fabricated here may have potential use in future anti-bacterial compositions and coatings technologies.
Project description:In this work, we develop an in situ method to grow highly controllable, sensitive, three-dimensional (3D) surface-enhanced Raman scattering (SERS) substrates via an optothermal effect within microfluidic devices. Implementing this approach, we fabricate SERS substrates composed of Ag@ZnO structures at prescribed locations inside microfluidic channels, sites within which current fabrication of SERS structures has been arduous. Conveniently, properties of the 3D Ag@ZnO nanostructures such as length, packing density, and coverage can also be adjusted by tuning laser irradiation parameters. After exploring the fabrication of the 3D nanostructures, we demonstrate a SERS enhancement factor of up to ?2×10(6) and investigate the optical properties of the 3D Ag@ZnO structures through finite-difference time-domain simulations. To illustrate the potential value of our technique, low concentrations of biomolecules in the liquid state are detected. Moreover, an integrated cell-trapping function of the 3D Ag@ZnO structures records the surface chemical fingerprint of a living cell. Overall, our optothermal-effect-based fabrication technique offers an effective combination of microfluidics with SERS, resolving problems associated with the fabrication of SERS substrates in microfluidic channels. With its advantages in functionality, simplicity, and sensitivity, the microfluidic-SERS platform presented should be valuable in many biological, biochemical, and biomedical applications.