Advances in materials chemistry offer a range of nanostructured shapes and textures for building new biosensors. Previous reports have implied that controlling the properties of sensor substrates can improve detection sensitivities, but the evidence remains indirect. Here we show that by nanostructuring the sensing electrodes, it is possible to create nucleic acid sensors that have a broad range of sensitivities and that are capable of rapid analysis. Only highly branched electrodes with fine structuring attained attomolar sensitivity. Nucleic acid probes immobilized on finely nanostructured electrodes appear more accessible and therefore complex more rapidly with target molecules in solution. By forming arrays of microelectrodes with different degrees of nanostructuring, we expanded the dynamic range of a sensor system from two to six orders of magnitude. The demonstration of an intimate link between nanoscale sensor structure and biodetection sensitivity will aid the development of high performance diagnostic tools for biology and medicine.
The global COVID-19 pandemic has attracted considerable attention toward innovative methods and technologies for suppressing the spread of viruses. Transmission via contaminated surfaces has been recognized as an important route for spreading SARS-CoV-2. Although significant efforts have been made to develop antibacterial surface coatings, the literature remains scarce for a systematic study on broad-range antiviral coatings. Here, we aim to provide a comprehensive overview of the antiviral materials and coatings that could be implemented for suppressing the spread of SARS-CoV-2 via contaminated surfaces. We discuss the mechanism of operation and effectivity of several types of inorganic and organic materials, in the bulk and nanomaterial form, and assess the possibility of implementing these as antiviral coatings. Toxicity and environmental concerns are also discussed for the presented approaches. Finally, we present future perspectives with regards to emerging antimicrobial technologies such as omniphobic surfaces and assess their potential in suppressing surface-mediated virus transfer. Although some of these emerging technologies have not yet been tested directly as antiviral coatings, they hold great potential for designing the next generation of antiviral surfaces.
Due to inspiration from the Nepenthes pitcher plant, a frontier of devices has emerged with unmatched capabilities. Liquid-infused surfaces (LISs), particularly known for their liquid-repelling behavior under low tilting angles (<5°), have demonstrated a plethora of applications in medical, marine, energy, industrial, and environmental materials. This review presents recent developments of LIS technology and its prospective to define the future direction of this technology in solving tomorrow’s real-life challenges. First, an introduction to the different models explaining the physical phenomena of these surfaces, their wettability, and viscous-dependent frictional forces is discussed. Then, an outline of different emerging strategies required to fabricate a stable liquid-infused interface is presented, including different substrates, lubricants, surface chemistries, and design parameters which can be tuned depending on the application. Furthermore, applications of LIS coatings in the areas of anticorrosion, antifouling, anti-icing, self-healing, droplet manipulation, and biomedical devices will be presented followed by the limitations and future direction of this technology.
Fabrication of hierarchical materials, with highly optimized features from the millimeter to the nanometer scale, is crucial for applications in diverse areas including biosensing, energy storage, photovoltaics, and tissue engineering. In the past, complex material architectures have been achieved using a combination of top‐down and bottom‐up fabrication approaches. A remaining challenge, however, is the rapid, inexpensive, and simple fabrication of such materials systems using bench‐top prototyping methods. To address this challenge, the properties of hierarchically structured electrodes are developed and investigated by combining three bench‐top techniques: top‐down electrode patterning using vinyl masks created by a computer‐aided design (CAD)‐driven cutter, thin film micro/nanostructuring using a shrinkable polymer substrate, and tunable electrodeposition of conductive materials. By combining these methods, controllable electrode arrays are created with features in three distinct length scales: 40 μm to 1 mm, 50 nm to 10 μm, and 20 nm to 2 μm. The electrical and electrochemical properties of these electrodes are analyzed and it is demonstrated that they are excellent candidates for next generation low‐cost electrochemical and electronic devices.
Detection of biomolecules at low abundances is crucial to the rapid diagnosis of disease. Impressive sensitivities, typically measured with small model analytes, have been obtained with a variety of nano- and microscale sensors. A remaining challenge, however, is the rapid detection of large native biomolecules in real biological samples. Here we develop and investigate a sensor system that directly addresses the source of this challenge: the slow diffusion of large biomolecules traveling through solution to fixed sensors, and inefficient complexation of target molecules with immobilized probes. We engineer arrayed sensors on two distinct length scales: a ∼100 μm length scale commensurable with the distance bacterial mRNA can travel in the 30 min sample-to-answer duration urgently required in point-of-need diagnostic applications; and the nanometer length scale we prove necessary for efficient target capture. We challenge the specificity of our hierarchical nanotextured microsensors using crude bacterial lysates and document the first electronic chip to sense trace levels of bacteria in under 30 min.
We performed in vitro selection experiments to identify DNA aptamers for the S1 subunit of the SARS-CoV-2 spike protein (S1 protein). Using a pool of pre-structured random DNA sequences, we obtained over 100 candidate aptamers after 13 cycles of enrichment under progressively more stringent selection pressure. The top 10 sequences all exhibited strong binding to the S1 protein. Two aptamers, named MSA1 (Kd = 1.8 nM) and MSA5 (Kd = 2.7 nM), were assessed for binding to the heat-treated S1 protein, untreated S1 protein spiked into 50% human saliva and the trimeric spike protein of both the wildtype and the B.1.1.7 variant, demonstrating comparable affinities in all cases. MSA1 and MSA5 also recognized the pseudotyped lentivirus of SARS-CoV-2 with respective Kd values of 22.7 pM and 11.8 pM. Secondary structure prediction and sequence truncation experiments revealed that both MSA1 and MSA5 adopted a hairpin structure, which was the motif pre-designed into the original library. A colorimetric sandwich assay was developed using MSA1 as both the recognition element and detection element, which was capable of detecting the pseudotyped lentivirus in 50% saliva with a limit of detection of 400 fM, confirming the potential of these aptamers as diagnostic tools for COVID-19 detection.
We report as imple and rapid saliva-based SARS-CoV-2 antigen test that utilizes an ewly developed dimeric DNAa ptamer,d enoted as DSA1N5, that specifically recognizes the spike proteins of the wildtype virus and its Alpha and Delta variants with dissociation constants of 120, 290 and 480 pM, respectively,a nd binds pseudotyped lentiviruses expressing the wildtype and alpha trimeric spike proteins with affinity constants of 2.1 pM and 2.3 pM, respectively.T o develop ah ighly sensitive test, DSA1N5 was immobilized onto gold electrodes to produce an electrochemical impedance sensor,which was capable of detecting 1000 viral particles per mL in 1:1d iluted saliva in under 10 min without any further sample processing. Evaluation of 36 positive and 37 negative patient saliva samples produced aclinical sensitivity of 80.5 % and specificity of 100 %a nd the sensor could detect the wildtype virus as well as the Alpha and Delta variants in the patient samples,w hich is the first reported rapid test that can detect any emerging variant of SARS-CoV-2.
Nanocatalyst degradation is a serious limiting factor for the commercialization of proton exchange membrane fuel cells. Although the degradation has been extensively studied in the past through various ex situ electrochemical methods, employing an in situ technique can greatly improve our understanding of the mechanisms involved during the electrochemical cycling. In this work, we have employed an in situ liquid cell inside a TEM for a simultaneous investigation of the structural evolution and electrochemical response of Pt–Fe nanocatalysts. We demonstrate that the coarsening processes of these nanocatalyst particles, including the nucleation and growth, are not uniform, both in space and in time scale. The growth rate is found to be both site- and potential-dependent. Furthermore, these particles were found to exhibit considerably different behaviors when attached to an electrode as opposed to when isolated in the electrolyte. With Pt–Fe nanoalloy system as a candidate material, this work demonstrates that the in situ structural characterization of nanocatalysts under electrochemical bias and inside the native electrolyte environment provides much deeper insight into the catalyst degradation mechanisms as compared to the routine ex situ electrochemical studies.
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