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            Wearable sweat biosensors have shown great progress in noninvasive, in situ, and continuous health monitoring to demonstrate individuals’ physiological states. Advances in novel nanomaterials and fabrication methods promise to usher in a new era of wearable biosensors. Here, we introduce a threedimensional (3D)-printed flexible wearable health monitor fabricated through a unique one-step continuous manufacturing process with self-supporting microfluidic channels and novel single-atom catalyst-based bioassays for measuring the sweat rate and concentration of three biomarkers. Direct ink writing is adapted to print the microfluidic device with self-supporting structures to harvest human sweat, which eliminates the need for removing sacrificial supporting materials and addresses the contamination and sweat evaporation issues associated with traditional sampling methods. Additionally, the pick-and-place strategy is employed during the printing process to accurately integrate the bioassays, improving manufacturing efficiency. A single-atom catalyst is developed and utilized in colorimetric bioassays to improve sensitivity and accuracy. A feasibility study on human skin successfully demonstrates the functionality and reliability of our health monitor, generating reliable and quantitative in situ results of sweat rate, glucose, lactate, and uric acid concentrations during physical exercise.more » « less
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            Abstract Designing cost‐efffective electrocatalysts for the oxygen evolution reaction (OER) holds significant importance in the progression of clean energy generation and efficient energy storage technologies, such as water splitting and rechargeable metal–air batteries. In this work, an OER electrocatalyst is developed using Ni and Fe precursors in combination with different proportions of graphene oxide. The catalyst synthesis involved a rapid reduction process, facilitated by adding sodium borohydride, which successfully formed NiFe nanoparticle nests on graphene support (NiFe NNG). The incorporation of graphene support enhances the catalytic activity, electron transferability, and electrical conductivity of the NiFe‐based catalyst. The NiFe NNG catalyst exhibits outstanding performance, characterized by a low overpotential of 292.3 mV and a Tafel slope of 48 mV dec−1, achieved at a current density of 10 mA cm−2. Moreover, the catalyst exhibits remarkable stability over extended durations. The OER performance of NiFe NNG is on par with that of commercial IrO2in alkaline media. Such superb OER catalytic performance can be attributed to the synergistic effect between the NiFe nanoparticle nests and graphene, which arises from their large surface area and outstanding intrinsic catalytic activity. The excellent electrochemical properties of NiFe NNG hold great promise for further applications in energy storage and conversion devices.more » « less
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            Abstract Fe–N–C single‐atom catalysts (SACs) exhibit excellent peroxidase (POD)‐like catalytic activity, owing to their well‐defined isolated iron active sites on the carbon substrate, which effectively mimic the structure of natural peroxidase's active center. To further meet the requirements of diverse biosensing applications, SAC POD‐like activity still needs to be continuously enhanced. Herein, a phosphorus (P) heteroatom is introduced to boost the POD‐like activity of Fe–N–C SACs. A 1D carbon nanowire (FeNCP/NW) catalyst with enriched Fe–N4active sites is designed and synthesized, and P atoms are doped in the carbon matrix to affect the Fe center through long‐range interaction. The experimental results show that the P‐doping process can boost the POD‐like activity more than the non‐P‐doped one, with excellent selectivity and stability. The mechanism analysis results show that the introduction of P into SAC can greatly enhance POD‐like activity initially, but its effect becomes insignificant with increasing amount of P. As a proof of concept, FeNCP/NW is employed in an enzyme cascade platform for highly sensitive colorimetric detection of the neurotransmitter acetylcholine.more » « less
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            Abstract Multifunctional nanozymes can benefit biochemical analysis via expanding sensing modes and enhancing analytical performance, but designing multifunctional nanozymes to realize the desired sensing of targets is challenging. In this work, single‐atomic iron doped carbon dots (SA Fe‐CDs) are designed and synthesized via a facile in situ pyrolysis process. The small‐sized CDs not only maintain their tunable fluorescence, but also serve as a support for loading dispersed active sites. Monoatomic Fe offers SA Fe‐CDs exceptional oxidase‐mimetic activity to catalyze 3,3′,5,5′‐tetramethylbenzidine (TMB) oxidation with fast response (Vmax = 10.4 nM s‐1) and strong affinity (Km = 168 µM). Meanwhile, their photoluminescence is quenched by the oxidation product of TMB due to inner filter effect. Phosphate ions (Pi) can suppress the oxidase‐mimicking activity and restore the photoluminescence of SA Fe‐CDs by interacting with Fe active sites. Based on this principle, a dual‐mode colorimetric and fluorescence assay of Pi with high sensitivity, selectivity, and rapid response is established. This work paves a path to develop multifunctional enzyme‐like catalysts, and offers a simple but efficient dual‐mode method for phosphate monitoring, which will inspire the exploration of multi‐mode sensing strategies based on nanozyme catalysis.more » « less
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