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.
Development of high-performance fiber-shaped wearable sensors is of great significance for next-generation smart textiles for real-time and out-of-clinic health monitoring. The previous focus has been mainly on monitoring physical parameters such as pressure and strains associated with human activities. Development of an enzyme-based non-invasive wearable electrochemical sensor to monitor biochemical vital signs of health such as the glucose level in sweat has attracted increasing attention recently, due to the unmet clinical needs for the diabetic patients. To achieve this, the key challenge lies in the design of a highly stretchable fiber with high conductivity, facile enzyme immobilization, and straininsensitive properties. Herein, we demonstrate an elastic gold fiberbased three-electrode electrochemical platform that can meet the aforementioned criteria toward wearable textile glucose biosensing. The gold fiber could be functionalized with Prussian blue and glucose oxidase to obtain the working electrode and modified by Ag/AgCl to serve as the reference electrode; and the nonmodified gold fiber could serve as the counter electrode. The as-fabricated textile glucose biosensors achieved a linear range of 0−500 μM and a sensitivity of 11.7 μA mM −1 cm −2 . Importantly, such sensing performance could be maintained even under a large strain of 200%, indicating the potential applications in real-world wearable biochemical diagnostics from human sweat.
Closing both the carbon and nitrogen loops is a critical venture to support the establishment of the circular, net‐zero carbon economy. Although single atom catalysts (SACs) have gained interest for the electrochemical reduction reactions of both carbon dioxide (CO2RR) and nitrate (NO3RR), the structure–activity relationship for Cu SAC coordination for these reactions remains unclear and should be explored such that a fundamental understanding is developed. To this end, the role of the Cu coordination structure is investigated in dictating the activity and selectivity for the CO2RR and NO3RR. In agreement with the density functional theory calculations, it is revealed that Cu‐N4 sites exhibit higher intrinsic activity toward the CO2RR, whilst both Cu‐N4 and Cu‐N4−x‐Cx sites are active toward the NO3RR. Leveraging these findings, CO2RR and NO3RR are coupled for the formation of urea on Cu SACs, revealing the importance of *COOH binding as a critical parameter determining the catalytic activity for urea production. To the best of the authors’ knowledge, this is the first report employing SACs for electrochemical urea synthesis from CO2RR and NO3RR, which achieves a Faradaic efficiency of 28% for urea production with a current density of −27 mA cm–2 at −0.9 V versus the reversible hydrogen electrode.
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.
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.
In the present work, an enhanced and stable anodic electrochemiluminescence (ECL) was observed from a suspension of boron nitride quantum dots (BNQDs) and Ru(bpy), which had a 400-fold enhancement compared with individual Ru(bpy). Interestingly, different from the previous research on BNQDs as a type of optical probe, BNQDs were demonstrated as an efficient coreactant of Ru(bpy)-based ECL for the first time and confirmed by collecting the ECL spectra. The amino-bearing groups and the electrocatalytic effect of the BNQDs endowed them as potential coreactants for ECL of Ru(bpy), and the possible mechanism of the electrode surface reaction was discussed. Several factors including electrode material, the pH of the buffer solution, and the amount of BNQDs were investigated and also further confirmed the role of the BNQDs in the proposed Ru(bpy)/BNQDs system. On the basis of the quenching effect between the excited state of Ru(bpy) and the oxidation form of DA in the ECL system of Ru(bpy)/BNQDs, the ECL sensing platform for DA was successfully established. The proposed ECL system with the outstanding ECL efficiency may hold great potential in the bioanlysis because of the biocompatibility and good stability of BNQDs.
In this work, we report a nanoscale multichannel closed bipolar electrode (BPE) array based on the poly(ethylene terephthalate) (PET) membrane for the first time. With our design, oxidants, coreactants, quenchers, and even biomarkers can be detected in a Ru(bpy)3(2+)/TPA (tripropylamine) electrochemiluminescence (ECL) system. The multichannel PET membrane was etched according to our desire by NaOH, and then Au nanofibers were decorated in the inner region of the channel as a BPE array. Using ECL as a signal readout, a series of targets including TPA, Ru(bpy)3(2+), dopamine, H2O2, alpha-fetoprotein (AFP), and carcino-embryonic antigen (CEA) can be detected with this device. The practical application of the proposed multichannel closed BPE array was verified in the detection of AFP and CEA in human serum with satisfying results. This kind of nanoscale device holds promising potential for multianalysis. More importantly, as the PET membrane used in this device can be etched with a desirable diameter (nano- to microscale) and different BPE array densities (ion tracks of 10(8)/cm(2), 10(6)/cm(2), 10(4)/cm(2)), our design can be served as a useful platform for future advances in nanoscale bipolar electrochemistry.
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