SARS-CoV-2 Virus Detection Via a Polymeric Nanochannel-Based Electrochemical Biosensor.

The development of simple, cost-effective, rapid, and quantitative diagnostic tools remains critical to monitor infectious COVID-19 disease. Although numerous diagnostic platforms, including rapid antigen tests, are developed and used, they suffer from limited accuracy, especially when tested with asymptomatic patients. Here, a unique approach to fabricate a nanochannel-based electrochemical biosensor that can detect the entire virion instead of virus fragments, is demonstrated. The sensing platform has uniform nanoscale channels created by the convective assembly of polystyrene (PS) beads on gold electrodes. The PS beads are then functionalized with bioreceptors while the gold surface is endowed with anti-fouling properties. When added to the biosensor, SARS-CoV-2 virus particles block the nanochannels by specific binding to the bioreceptors. The nanochannel blockage hinders the diffusion of a redox probe; and thus, allows quantification of the viral load by measuring the changes in the oxidation current before and after virus incubation. The biosensor shows a low limit of detection of ≈1.0 viral particle mL-1 with a wide detection range up to 108 particles mL-1 in cell culture media. Moreover, the biosensor is able to differentiate saliva samples with SARS-CoV-2 from those without, demonstrating the potential of this technology for translation into a point-of-care biosensor product.

Orientation-Dependent Soft Plasmonics of Gold Nanobipyramid Plasmene Nanosheets.

In parallel to the burgeoning field of soft electronics, soft plasmonics focuses on the design and fabrication of plasmonic structures supported on elastomers and to understand how their properties respond to mechanical deformations. Here, we report on a partial ligand-stripping strategy to fabricate elastomer-supported gold nanobipyramid (NBP) plasmene nanosheets. Unlike spherelike building blocks, NBP-building blocks display complex orientation-dependent plasmonic responses to external strains. By collecting polarized plasmonic resonance spectra in conjunction with electrostatic eigenmode modeling, we reveal simultaneous changes in interparticle spacing and spatial orientations of NBP building blocks under mechanical strains. Such changes are directly related to initial NBP packing orders. Further analysis of strain sensitivities for various NBP plasmenes indicated that plasmonic spectra of ∼45° oriented samples are mostly susceptible to strain at acute polarized angles. The results presented may enable novel applications in future soft optoelectronic devices in sensing, encryption, and data storage.

Vertically Aligned Gold Nanowires as Stretchable and Wearable Epidermal Ion-Selective Electrode for Noninvasive Multiplexed Sweat Analysis.

The noninvasive continuous analysis of human sweat is of great significance for improved healthcare diagnostics and treatment in the future, for which a wearable potentiometry-based ion-selective electrode (ISE) has attracted increasing attention, particularly involving ion detection. Note that traditional solid-state ISE electrodes are rigid ion-to-electron transducers that are not conformal to soft human skin and cannot function under stretched states. Here, we demonstrated that vertically aligned mushroom-like gold nanowires (v-AuNW) could serve as stretchable and wearable ion-to-electron transducers for multiplexed, in situ potentiometric analysis of pH, Na+, and K+ in sweat. By modifying v-AuNW electrodes with polyaniline, Na ionophore X, and a valinomycin-based selective membrane, we could specifically detect pH, Na+, and K+, respectively, with high selectivity, reproducibility, and stability. Importantly, the electrochemical performance could be maintained even under 30% strain and during stretch-release cycles without the need of extrinsic structural design. Furthermore, our stretchable v-AuNW ISEs could be seamlessly integrated with a flexible printed circuit board, enabling wireless on-body detection of pH, Na+, and K+ with fast response and negligible cross-talk, indicating considerable promise for noninvasive wearable sweat analysis.

Real-Time and In-Situ Monitoring of H2O2 Release from Living Cells by a Stretchable Electrochemical Biosensor Based on Vertically Aligned Gold Nanowires.

Traditional electrochemical biosensing electrodes (e.g., gold disk, glassy carbon electrode, etc.) can undergo sophisticated design to detect chemicals/biologicals from cells. However, such electrodes are typically rigid and nonstretchable, rendering it challenging to detect cellular activities in real-time and in situ when cells are in mechanically deformed states. Here, we report a new stretchable electrochemical cell-sensing platform based on vertically aligned gold nanowires embedded in PDMS (v-AuNWs/PDMS). Using H2O2 as a model analyte, we show that the v-AuNWs/PDMS electrode can display an excellent sensing performance with a wide linear range, from 40 µM to 15 mM, and a high sensitivity of 250 mA/cm2/M at a potential of -0.3 V. Moreover, living cells can grow directly on our stretchable high-surface area electrodes with strong adhesion, demonstrating their excellent biocompatibility. Further cell stimulation by adding chemicals induced H2O2 generation, which can be detected in real-time and in situ using our v-AuNWs/PDMS platform for both natural and stretched states of cells. Our results indicate the v-AuNWs/PDMS electrochemical biosensor may serve as a general cell-sensing platform for living organisms under deformed states.

A soft and ultrasensitive force sensing diaphragm for probing cardiac organoids instantaneously and wirelessly.

Time-lapse mechanical properties of stem cell derived cardiac organoids are important biological cues for understanding contraction dynamics of human heart tissues, cardiovascular functions and diseases. However, it remains difficult to directly, instantaneously and accurately characterize such mechanical properties in real-time and in situ because cardiac organoids are topologically complex, three-dimensional soft tissues suspended in biological media, which creates a mismatch in mechanics and topology with state-of-the-art force sensors that are typically rigid, planar and bulky. Here, we present a soft resistive force-sensing diaphragm based on ultrasensitive resistive nanocracked platinum film, which can be integrated into an all-soft culture well via an oxygen plasma-enabled bonding process. We show that a reliable organoid-diaphragm contact can be established by an 'Atomic Force Microscope-like' engaging process. This allows for instantaneous detection of the organoids' minute contractile forces and beating patterns during electrical stimulation, resuscitation, drug dosing, tissue culture, and disease modelling.

Soft Wearable Healthcare Materials and Devices.

In spite of advances in electronics and internet technologies, current healthcare remains hospital-centred. Disruptive technologies are required to translate state-of-art wearable devices into next-generation patient-centered diagnosis and therapy. In this review, recent advances in the emerging field of soft wearable materials and devices are summarized. A prerequisite for such future healthcare devices is the need of novel materials to be mechanically compliant, electrically conductive, and biologically compatible. It is begun with an overview of the two viable design strategies reported in the literatures, which is followed by description of state-of-the-art wearable healthcare devices for monitoring physical, electrophysiological, chemical, and biological signals. Self-powered wearable bioenergy devices are also covered and sensing systems, as well as feedback-controlled wearable closed-loop biodiagnostic and therapy systems. Finally, it is concluded with an overall summary and future perspective.

Mechanically-gated electrochemical ionic channels with chemically modified vertically aligned gold nanowires.

Mechanically-gated ion channels play an important role in the human body, whereas it is challenging to design artificial mechanically-controlled ionic transport devices as the intrinsically rigidity of traditional electrodes. Here, we report on a mechanically-gated electrochemical channel by virtue of vertically aligned gold nanowires (v-AuNWs) as 3D stretchable electrodes. By surface modification with a self-assembled 1-Dodecanethiol monolayer, the v-AuNWs become hydrophobic and inaccessible to hydrated redox species (e.g., Fe ( CN ) 6 3 - / 4 - and Ru ( bpy ) 3 2 + ). Under mechanical strains, the closely-packed v-AuNWs unzip/crack to generate ionic channels to enable redox reactions, giving rise to increases in Faradaic currents. The redox current increases with the strain level until it reaches a certain threshold value, and then decreases as the strain-induced conductivity decreases. The good reversible "on-off" behaviors for multiple cycles were also demonstrated. The results presented demonstrate a new strategy to control redox reactions simply by tensile strain, indicating the potential applications in future soft smart mechanotransduction devices.

Design of Stretchable Holey Gold Biosensing Electrode for Real-Time Cell Monitoring.

In bioelectronics, gold thin films have been widely used as sensing electrodes for probing biological events due to their high conductivity, chemical inertness, biocompatibility, wide electrochemical window, and facile surface modification. However, they are intrinsically not stretchable, which limits their applications in detecting biological reactions when a soft biological system is mechanically deformed. Here, we report on a nanosphere lithography-based strategy to generate ordered microhole gold thin-film electrodes supported by elastomeric substrates. Both experimental and theoretical studies show that the presence of microholes substantially suppresses the catastrophic crack propagation-the main reason for electrical failure for a continuous gold film. As a result, the holey gold film achieves a ∼94% stretchable limit, after which the conductivity is lost, in contrast to ∼4% for the nonstructured counterpart. Furthermore, the pinhole gold electrode is successfully used to monitor the H2O2 released from living cells under dynamic stretching conditions.

Enokitake Mushroom-like Standing Gold Nanowires toward Wearable Noninvasive Bimodal Glucose and Strain Sensing.

We have recently demonstrated that Enokitake mushroom-like gold with nanoparticles as the "head" and nanowires as the "tail" could grow directly on elastomeric substrates, which are extremely stretchable electrodes that can be used as wearable sensors for detecting strain and pressure. In this work, we show that such electrodes can also be used as intrinsically stretchable glucose biosensors. By modifying the vertical gold nanowire electrodes with glucose oxidase and Prussian blue nanoparticles, a limit of detection of 10 µM, sensitivity of 23.72 µA·mM-1·cm-2, and high selectivity can be achieved. The as-obtained glucose biosensors were able to maintain a high sensing performance under various mechanical deformations. Even for 30% strain, a sensitivity of 4.55 µA·mM-1·cm-2 toward glucose detection in the artificial sweat was possible. Furthermore, it was found that strains could be simultaneously detected with a gauge factor of 2.30 (strain 0-10%) and 22.64 (strain 10-20%), demonstrating the potential of such bimodal sensors to allow simultaneous monitoring of physical and biological signals.

Local Crack-Programmed Gold Nanowire Electronic Skin Tattoos for In-Plane Multisensor Integration.

Sensitive, specific, yet multifunctional tattoo-like electronics are ideal wearable systems for "any time, any where" health monitoring because they can virtually become parts of the human skin, offering a burdenless "unfeelable" wearing experience. A skin-like, multifunctional electronic tattoo made entirely from gold using a standing enokitake-mushroom-like vertically aligned nanowire membrane in conjunction with a programmable local cracking technology is reported. Unlike previous multifunctional systems, only a single material type is needed for the integrated gold circuits involved in interconnects and multiplexed specific sensors, thereby avoiding the use of complex multimaterials interfaces. This is possiblebecause the programmable local cracking technology allows for the arbitrary fine-tuning of the properties of elastic gold conductors from strain-insensitive to highly strain-sensitive simply by adjusting localized crack size, shape, and orientations-a capability impossible to achieve with previous bulk cracking technology. Furthermore, in-plane integration of strain/pressure sensors, anisotropic orientation-specific sensors, strain-insensitive stretchable interconnects, temperature sensors, glucose sensors, and lactate sensors without the need of soldering or gluing are demonstrated. This strategy opens a new general route for the design of next-generation wearable electronic tattoos.