Design and Optimization of Molecularly Imprinted Polymer Targeting Epinephrine Molecule: A Theoretical Approach.

Molecularly imprinted polymers (MIPs) are a growing highlight in polymer chemistry. They are chemically and thermally stable, may be used in a variety of environments, and fulfill a wide range of applications. Computer-aided studies of MIPs often involve the use of computational techniques to design, analyze, and optimize the production of MIPs. Limited information is available on the computational study of interactions between the epinephrine (EPI) MIP and its target molecule. A rational design for EPI-MIP preparation was performed in this study. First, density functional theory (DFT) and molecular dynamic (MD) simulation were used for the screening of functional monomers suitable for the design of MIPs of EPI in the presence of a crosslinker and a solvent environment. Among the tested functional monomers, acrylic acid (AA) was the most appropriate monomer for EPI-MIP formulation. The trends observed for five out of six DFT functionals assessed confirmed AA as the suitable monomer. The theoretical optimal molar ratio was 1:4 EPI:AA in the presence of ethylene glycol dimethacrylate (EGDMA) and acetonitrile. The effect of temperature was analyzed at this ratio of EPI:AA on mean square displacement, X-ray diffraction, density distribution, specific volume, radius of gyration, and equilibrium energies. The stability observed for all these parameters is much better, ranging from 338 to 353 K. This temperature may determine the processing and operating temperature range of EPI-MIP development using AA as a functional monomer. For cost-effectiveness and to reduce time used to prepare MIPs in the laboratory, these results could serve as a useful template for designing and developing EPI-MIPs.

Portable Saliva Sensor Based on Dual Recognition Elements for Detection of Caries Pathogenic Bacteria.

Dental caries is one of the most common diseases affecting more than 2 billion people's health worldwide. In a clinical setting, it is challenging to predict and proactively guard against dental cavities prior to receiving a confirmed diagnosis. Streptococcus mutans (S. mutans) in saliva has been recognized as the main causative bacterial agent that causes dental caries. High sensitivity, good selectivity, and a wide detection range are incredibly important factors to affect S. mutans detection in practical applications. In this study, we present a portable saliva biosensor designed for the early detection of S. mutans with the potential to predict the occurrence of dental cavities. The biosensor was fabricated using a S. mutans-specific DNA aptamer and S. mutans-imprinted polymers. Methylene blue was utilized as a redox probe in the sensor to generate current signals for analysis. When S. mutans enters complementarily S. mutans cavities, it blocks electron transfer between methylene blue and the electrode, resulting in decreases in the reduction current signal. The signal variations are associated with S. mutans concentrations that are useful for quantitative analysis. The linear detection range of S. mutans is 102-109 cfu mL-1, which covers the critical concentration of high caries risk. The biosensor exhibited excellent selectivity toward S. mutans in the presence of other common oral bacteria. The biosensor's wide detection range, excellent selectivity, and low limit of detection (2.6 cfu mL-1) are attributed to the synergistic effect of aptamer and S. mutans-imprinted polymers. The sensor demonstrates the potential to prevent dental caries.

An Integrated Sweat Sensor for Synchronous Detection of Multiple Atherosclerosis Biomarkers.

Atherosclerosis conditions are often assessed in the clinic by measuring blood viscosity, blood flow, and blood lesion levels. In alignment with precision medicine, it is essential to develop convenient and noninvasive approaches for atherosclerosis diagnostics. Herein, an integrated electrochemical sensor was successfully demonstrated for simultaneously detecting cholesterol, transferrin, and K+ in sweat, all biomarker indicators of atherosclerosis. The sensing substrate was based on carbon quantum dots integrated within multiwalled carbon nanotubes, creating a hybrid framework with low electron transfer resistance and highly efficient electron transfer rate, yielding a highly electrochemical active platform for ultrasensitive detection of trace sweat biomarkers. To ensure specificity to corresponding targets, the sensing mechanisms were based on molecular recognition reactions of cholesterol and ß-cyclodextrin, transferrin and molecular cavities, and K+ and ion-selective permeation membrane. Moreover, the integrated nonenzymatic sensor exhibited excellent long-term stability. Furthermore, the practical utility of the sensor was successfully demonstrated by the simultaneous detection of three atherosclerosis biomarkers in sweat from volunteers who underwent predesigned daily activities. The sensor shows promise for convenient indexing of atherosclerosis conditions in a noninvasive way.

A molecularly imprinted screen-printed carbon electrode for electrochemical epinephrine, lactate, and cortisol metabolites detection in human sweat.

This study presents a novel approach to the detection of epinephrine, lactate, and cortisol biomarkers in human sweat using molecularly-imprinted polymers (MIP) embedded screen printed carbon electrode (SPCE) sensors. The epinephrine and lactate MIP SPCE sensors were fabricated by epinephrine or lactate-imprinted polyaniline co-polymerized with 3-aminophenylboronic acid and gold nanoparticles (PANI-co-PBA/AuNP) selective membrane on a commercial SPCE. The cortisol sensor was comprised of a cortisol-imprinted poly(glycidyl methacryate-co-ethylene glycol dimethacrylate) (poly (GMA-co-EGDMA)@AuNP selective membrane deposited on a SPCE. Both cyclic voltammetry (CV) and differential pulse voltammetry (DPV) were used as modes of analysis for the MIP SPCE sensors. All sensors exhibited a rapid (∼1 min) and selective response to the epinephrine, lactate, and cortisol target analytes, with excellent precision between scans for both CV and DPV analysis modes. For CV, the LOD for epinephrine, lactate, and cortisol was 8.2 nM, 13 mM, and 0.042 µM, respectively. The LOD for DPV were 0.60 nM, 2.2 mM, and 0.025 µM for epinephrine, lactate, and cortisol, respectively. The MIP SPCE sensor platforms were further validated through the successful quantification of epinephrine, lactate, and cortisol in human sweat.

Anthraquinone-Polyaniline-Integrated Textile Platforms for In Situ Electrochemical Production of Hydrogen Peroxide for Microbial Deactivation.

Hydrogen peroxide (H2O2) is a versatile and effective disinfectant against common pathogenic bacteria such as Escherichia coli (E. coli). Electrochemical H2O2 generation has been studied in the past, but a lack of studies exists on miniaturized electrochemical platforms for the on-demand synthesis of H2O2 for antibacterial applications. In this article, a chemically modified cotton textile platform capable of in situ H2O2 production is demonstrated for E. coli deactivation. The cotton textile was modified by layer-by-layer coating with conductive carbon nanotubes/cellulose nanocrystals (CNT/CNC) and a polymer of polyaniline (PANI) decorated with anthraquinone (AQ), designated as the AQ@PANI@CNT/CNC@textile antibacterial patch. The AQ@PANI@CNT/CNC@textile antibacterial textile patch H2O2 production capabilities were evaluated using both electrochemical and colorimetric methods. The AQ@PANI@CNT/CNC@textile antibacterial patch electrochemically produced H2O2 concentrations up to 209 ± 25 µM over a 40 min period and displayed a log reduction of 3.32 for E. coli over a period of 2 h. The AQ@PANI@CNT/CNC@textile antibacterial patch offers promise for use as a self-disinfecting pathogen control platform.

A molecularly imprinted electrochemical microneedle sensor for multiplexed metabolites detection in human sweat.

This article demonstrates an array of inexpensive molecularly imprinted microneedle platforms for the multiplexed electrochemical detection of pH, epinephrine, dopamine, and lactate biomarkers in human sweat. The multiplexed sensors were fabricated via layer-by-layer (LbL) assembly on a polydimethylsiloxane (PDMS) microneedle platform coated with a conductive PDMS/carbon nanotube (CNT)/cellulose nanocrystal (CNC) composite (PDMS/CNT/CNC@PDMS). The pH sensor was comprised of a pH-responsive polyaniline (PANI)/CNT/CNC/silver nanoparticle (AgNP) composite layer. The epinephrine, dopamine, and lactate sensors consisted of an additional epinephrine, dopamine, or lactate-imprinted PANI-co-3-aminophenylboronic acid (PBA)/gold nanoparticle (AuNP) layer atop the PANI/CNT/CNC/AgNP composite layer. Each sensor rapidly (∼2 min) and selectively responded to their target analytes, with excellent precision between scans. The limits of detection (LOD) for the epinephrine, dopamine, and lactate sensors were 0.0007 ± 0.0002 µM, 2.11 ± 0.05 nM, and 0.07 ± 0.07 mM, respectively. The pH sensor accurately responded to a pH range of 4.25-10. The applicability of the sensor platforms were successfully verified through quantification of pH, epinephrine, dopamine, and lactate in a human sweat sample, showing promise for use as a wearable, point of need (PON) sensor for sweat analytics.

A Hybrid Stainless-Steel SPME Microneedle Electrode Sensor for Dual Electrochemical and GC-MS Analysis.

A mechanically robust in-tube stainless steel microneedle solid phase microextraction (SPME) platform for dual electrochemical and chromatographic detection has been demonstrated. The SPME microneedle was fabricated by layer-by-layer (LbL) in-tube coating, consisting of carbon nanotube (CNT)/cellulose nanocrystal (CNC) film layered with an electrically conductive polyaniline (PANI) hydrogel layer (PANI@CNT/CNC SPME microneedle (MN)). The PANI@CNT/CNC SPME MN showed effective analysis of caffeine by GC-MS with an LOD of 26 mg/L and excellent precision across the dynamic range. Additionally, the PANI@CNT/CNC SPME MN demonstrated a 67% increase in sensitivity compared to a commercial SPME fiber, while being highly robust for repeated use without loss in performance. For electrochemical detection, the PANI@CNT/CNC SPME MN showed excellent performance for the detection of 3-caffeoylquinic acid (3-CQA). The dynamic range and limits of detection (LOD) for 3-CQA analysis were 75-448 mg/L and 11 mg/L, respectively. The PANI@CNT/CNC SPME MN was demonstrated to accurately determine the caffeine content and 3-CQA in tea samples and dark roast coffee, respectively. The PANI@CNT/CNC SPME MN was used for semiquantitative antioxidant determination and composition analysis in kiwi fruit using electrochemistry and SPME-coupled GC-MS, respectively.

Hydrovoltaic Nanogenerators for Self-Powered Sweat Electrolyte Analysis.

Human sweat comprises various electrolytes that are health status indicators. Conventional potentiometric electrolyte sensors require an electrical power source, which is expensive, bulky, and requires a complex architecture. Herein, this work demonstrates an electric nanogenerator fabricated using silicon nanowire (SiNW) arrays comprising modified carbon nanoparticles. The SiNW arrays platform is demonstrated as an effective self-powered sensor for sweat electrolyte analysis. It has been shown that an evaporation-induced water flow in nanochannels can yield an open-circuit voltage (Voc ) of 0.45 V and a short-circuit current of 10.2 µA at room temperature as a result of overlapped electric double layers. The electrolyte in the water flow results in a Voc decrease due to the charge shielding effect. The Voc is inversely proportional to the electrolyte concentration. The fabricated hydrovoltaic device shows the capability for sensing electrolytes in human sweat, which is useful in evaluating the hydration status of volunteers following intense physical exercise. The device depicts a novel response mechanism compared to conventional electrochemical sensors. Furthermore, the hydrovoltaic device shows a maximum output power of 1.42 µW, and as such has been successfully shown to drive various electronic devices including light-emitting diodes, a calculator, and an electronic timer.

Electron Conductive and Transparent Hydrogels for Recording Brain Neural Signals and Neuromodulation.

Recording brain neural signals and optogenetic neuromodulations open frontiers in decoding brain neural information and neurodegenerative disease therapeutics. Conventional implantable probes suffer from modulus mismatch with biological tissues and an irreconcilable tradeoff between transparency and electron conductivity. Herein, a strategy is proposed to address these tradeoffs, which generates conductive and transparent hydrogels with polypyrrole-decorated microgels as cross-linkers. The optical transparency of the electrodes can be attributed to the special structures that allow light waves to bypass the microgel particles and minimize their interaction. Demonstrated by probing the hippocampus of rat brains, the biomimetic electrode shows a prolonged capacity for simultaneous optogenetic neuromodulation and recording of brain neural signals. More importantly, an intriguing brain-machine interaction is realized, which involves signal input to the brain, brain neural signal generation, and controlling limb behaviors. This breakthrough work represents a significant scientific advancement toward decoding brain neural information and developing neurodegenerative disease therapies.

A Multipurpose and Multilayered Microneedle Sensor for Redox Potential Monitoring in Diverse Food Analysis.

This work presents a multipurpose and multilayered stainless steel microneedle sensor for the in situ redox potential monitoring in food and drink samples, termed MN redox sensor. The MN redox sensor was fabricated by layer-by-layer (LbL) approach. The in-tube multilayer coating comprised carbon nanotubes (CNTs)/cellulose nanocrystals (CNCs) as the first layer, polyaniline (PANI) as the second layer, and the ferrocyanide redox couple as the third layer. Using cyclic voltammetry (CV) as a transduction method, the MN redox sensor showed facile electron transfer for probing both electrical capacitance and redox potential, useful for both analyte specific and bulk quantification of redox species in various food and drink samples. The bulk redox species were quantified based on the anodic/cathodic redox peak shifts (Ea/Ec) on the voltammograms resulting from the presence of redox-active species. The MN redox sensor was applied to detect selected redox species including ascorbic acid, H2O2, and putrescine, with capacitive limits of detection (LOD) of 49.9, 17.8, and 263 ng/mL for each species, respectively. For the bulk determination of redox species, the MN redox sensor displayed LOD of 5.27 × 103, 55.4, and 25.8 ng/mL in ascorbic acid, H2O2, and putrescine equivalents, respectively. The sensor exhibited reproducibility of ~ 1.8% relative standard deviation (%RSD). The MN redox sensor was successfully employed for the detection of fish spoilage and antioxidant quantification in king mushroom and brewed coffee samples, thereby justifying its potential for food quality and food safety applications. Lastly, the portability, reusability, rapid sampling time, and capability of in situ analysis of food and drink samples makes it amenable for real-time sensing applications.

Molecularly Imprinted Polymer-Modified Microneedle Sensor for the Detection of Imidacloprid Pesticides in Food Samples.

A portable, molecularly imprinted polymer (MIP)-based microneedle (MN) sensor for the electrochemical detection of imidacloprid (IDP) has been demonstrated. The MN sensor was fabricated via layer-by-layer (LbL) in-tube coating using a carbon nanotube (CNT)/cellulose nanocrystal (CNC) composite, and an IDP-imprinted polyaniline layer co-polymerized with imidazole-functionalized CNCs (PANI-co-CNC-Im) as the biomimetic receptor film. The sensor, termed MIP@CNT/CNC MN, was analyzed using both cyclic voltammetry (CV) and differential pulse voltammetry (DPV) and showed excellent electrochemical performance for the detection of IDP. The CV detection range for IDP was 2.0-99 µM, with limits of detection (LOD) of 0.35 µM, while the DPV detection range was 0.20-92 µM with an LOD of 0.06 µM. Additionally, the MIP@CNT/CNC MN sensor showed excellent reusability and could be used up to nine times with a 1.4 % relative standard deviation (% RSD) between uses. Lastly, the MIP@CNT/CNC MN sensor successfully demonstrated the quantification of IDP in a honey sample.

A Wearable, Textile-Based Polyacrylate Imprinted Electrochemical Sensor for Cortisol Detection in Sweat.

A wearable, textile-based molecularly imprinted polymer (MIP) electrochemical sensor for cortisol detection in human sweat has been demonstrated. The wearable cortisol sensor was fabricated via layer-by-layer assembly (LbL) on a flexible cotton textile substrate coated with a conductive nanoporous carbon nanotube/cellulose nanocrystal (CNT/CNC) composite suspension, conductive polyaniline (PANI), and a selective cortisol-imprinted poly(glycidylmethacrylate-co-ethylene glycol dimethacrylate) (poly(GMA-co-EGDMA)) decorated with gold nanoparticles (AuNPs), or plated with gold. The cortisol sensor rapidly (<2 min) responded to 9.8−49.5 ng/mL of cortisol, with an average relative standard deviation (%RSD) of 6.4% across the dynamic range, indicating excellent precision. The cortisol sensor yielded an excellent limit of detection (LOD) of 8.00 ng/mL, which is within the typical physiological levels in human sweat. A single cortisol sensor patch could be reused 15 times over a 30-day period with no loss in performance, attesting to excellent reusability. The cortisol sensor patch was successfully verified for use in quantification of cortisol levels in human sweat.

A Portable Sweat Sensor Based on Carbon Quantum Dots for Multiplex Detection of Cardiovascular Health Biomarkers.

The future of personalized diagnostics and treatment of cardiovascular diseases lies in the use of portable sensors. Portable sensors can acquire biomarker information in biological fluids such as sweat, an approach that mitigates the shortcomings of conventional hospital-centered healthcare. Low sensitivity, selectivity, and specificity remain bottlenecks for the widespread use of portable sensors. Herein, we demonstrate a portable sensor that simultaneously detects Na+, ascorbic acid, and human neuropeptide Y in sweat, all useful biomarkers to index cardiovascular health. The portable sensor comprises a six-electrode system containing three working electrodes, two reference electrodes, and one counter electrode. The working electrodes were prepared by depositing sensing components on carbon quantum dot (CQD) electrodes. The sensing mechanisms were based on selective ion recognition, enzyme catalytic reaction, and immune response, which guarantees specificity to corresponding targets. The CQDs offer massive reactive sites and effectively reduce the interfacial impedance during the sensing reaction, thereby enhancing the three biomarkers' detection sensitivity. As evidence of portable sensor capability, we demonstrate herein its effective simultaneous detection of the three biomarkers in a real sweat from healthy volunteers during routine activities including exercise, extra ascorbic acid ingestion, and extra Na+ ingestion. As such, the sensor shows promise for real-time noninvasive personalized medical diagnostics and metabolic wellness management.

Self-Healing and Shape-Editable Wearable Supercapacitors Based on Highly Stretchable Hydrogel Electrolytes.

Shape editability combined with a self-healing capability and long-term cycling durability are highly desirable properties for wearable supercapacitors. Most wearable supercapacitors have rigid architecture and lack the capacity for editability into desirable shapes. Through sandwiching hydrogel electrolytes between two electrodes, a suite of wearable supercapacitors that integrate desirable properties namely: repeated shape editability, excellent self-healing capability, and long-term cycling durability is demonstrated. A strategy is proposed to enhance the long-term cycling durability by utilizing hydrogel electrolytes with unique cross-linking structures. The dynamic crosslinking sites are formed by quadruple H bonds and hydrophobic association, stabilizing the supercapacitors from inorganic ion disruption during charge-discharge processes. The fabricated supercapacitors result in the capacitance retention rates of 99.6% and 95.8% after 5000 and 10 000 charge-discharge cycles, respectively, which are much higher than others reported in the literature. Furthermore, the supercapacitor sheets can be repeatedly processed into various shapes without any capacitance loss. The supercapacitors exhibit a 95% capacitance retention rate after five cutting/self-healing cycles, indicative of their excellent self-healing performance. To demonstrate real-life applicability, the wearable supercapacitors are successfully used to power a light-emitting diode and an electronic watch.

A MIP-enabled stainless-steel hypodermic needle sensor for electrochemical detection of aflatoxin B1.

Aflatoxin B1 (AFB1) has been identified as one of the most potent naturally occurring carcinogens with high toxicity. The maximum permissible levels of total aflatoxin contamination in food products are limited to 10-15 µg kg-1, as established by the Codex Alimentarius Commission. The widespread occurrence of AFB1 in the food chain identifies them as significant agricultural contaminants of global concern. We herewith demonstrate a molecularly imprinted polymer (MIP)-enabled stainless steel hypodermic needle sensor for sensitive electrochemical detection of AFB1. The stainless-steel hypodermic needle sensor was fabricated using a layer by layer (LbL) film coating comprising multiwalled carbon nanotubes (MWCNTs), cellulose nanocrystals (CNC), and an AFB1 imprinted polyaniline (PANI) biomimetic receptor film. The PANI@MIP/CNC-CNT hypodermic needlesensor showed excellent electrochemical capacitance response (∼10 min) to AFB1 with a linear range of 0-25 nM and a limit of detection (LOD) of 3 nM. Demonstrating good reusability, a single PANI@MIP/CNC-CNT hypodermic needle AFB1 sensor could be reused up to 7 times with a 2.8% relative standard deviation (% RSD) in the sensor's capacitive response. The PANI@MIP/CNC-CNT hypodermic needle sensor was effective in the detection of AFB1 spiked in milk.

Stainless steel electrochemical capacitive microneedle sensors for multiplexed simultaneous measurement of pH, nitrates, and phosphates.

Concerns for agri-food safety and environmental management require development of simple to use and cost- and time-effective multiplex sensors for point-of-need (PON) chemical analytics by public end-user. Simultaneous detection of nitrates, phosphates, and pH is of importance in soil and water analysis, agriculture, and food quality assessment. This article demonstrates a suite of stainless steel microneedle electrochemical sensors for multiplexed measurement of pH, nitrate, and phosphate using faradaic capacitance derived from cyclic voltammetry as the mode of detection. The multi-target microneedle sensors were fabricated by layer-by-layer (LbL) assembly in a stainless steel hypodermic microneedle substrate. For nitrate sensing, the stainless steel was coated with carbon nanotube/cellulose nanocrystal (CNT)/CNC) decorated with silver nanoparticles (Ag). For pH measurement, the polyaniline (pANI) was coated onto the CNT/CNC@Ag film, while for phosphate detection, the CNT/CNC/Ag @pANI microneedle was further decorated with ammonium molybdenum tetrahydrate (AMT). The microelectrode platforms were characterized by FTIR, Raman, and microscopic techniques. The nitrate- and phosphate-based microneedle electrochemical sensors had excellent selectivity and sensitivity, with a determined limit of detection (LOD) of 0.008 mM and 0.007 mM, respectively. The pH microneedle sensor was responsive to pH in the linear range of 3-10. The three microneedle sensors yielded repeatable results, with a precision ranging from 4.0 to 7.5% RSD over the concentration ranges tested. The inexpensive (~ 1 $ CAD) microneedle sensors were successfully verified for use in quantification of nitrate, pH, and phosphate in brewed black coffee as a real sample. As such, the microneedle sensors are economical devices and show great promise as robust platforms for PON precision chemical analytics.

Highly Stretchable Hydrogels as Wearable and Implantable Sensors for Recording Physiological and Brain Neural Signals.

Recording electrophysiological information such as brain neural signals is of great importance in health monitoring and disease diagnosis. However, foreign body response and performance loss over time are major challenges stemming from the chemomechanical mismatch between sensors and tissues. Herein, microgels are utilized as large crosslinking centers in hydrogel networks to modulate the tradeoff between modulus and fatigue resistance/stretchability for producing hydrogels that closely match chemomechanical properties of neural tissues. The hydrogels exhibit notably different characteristics compared to nanoparticles reinforced hydrogels. The hydrogels exhibit relatively low modulus, good stretchability, and outstanding fatigue resistance. It is demonstrated that the hydrogels are well suited for fashioning into wearable and implantable sensors that can obtain physiological pressure signals, record the local field potentials in rat brains, and transmit signals through the injured peripheral nerves of rats. The hydrogels exhibit good chemomechanical match to tissues, negligible foreign body response, and minimal signal attenuation over an extended time, and as such is successfully demonstrated for use as long-term implantable sensory devices. This work facilitates a deeper understanding of biohybrid interfaces, while also advancing the technical design concepts for implantable neural probes that efficiently obtain physiological information.

Electrochemical aptasensor based on electrodeposited poly(3,4-ethylenedioxythiophene)-graphene oxide coupled with Au@Pt nanocrystals for the detection of 17ß-estradiol.

An electrochemical aptasensor is reported for the sensitive and specific monitoring of 17ß-estradiol (E2) based on the modification of electrodeposited poly(3,4-ethylenedioxythiophene) (PEDOT)-graphene oxide (GO) coupled with Au@Pt nanocrystals (Au@Pt). With excellent conductivity, chemical stability and active sites, the PEDOT-GO nanocomposite film was firstly in situ polymerized on the glassy carbon electrode by cyclic voltammetry. Subsequently, one-step synthesized Au@Pt were decorated on the conductive polymer, providing a platform for immobilizing the aptamer and enhancing the detecting sensitivity. With the addition of E2, since the interfacial electron transfer process was retarded by the E2-aptamer complex, the differential pulse voltammetry signal decreased gradually. Under optimum conditions, the calibration curve of E2 exhibited a linear range between 0.1 pM and 1 nM, with a low detection limit (S/N = 3) of 0.08 pM. The developed aptasensor showed admiring selectivity, stability, and reproducibility. It was tested in human serum, lake water and tap water samples after low-cost and simple pretreatment. Consequently, the developed platform could provide a new design thought for ultrasensitive detection of E2 in clinical and environmental samples.

Integrated Wearable Sensors for Sensing Physiological Pressure Signals and ß-Hydroxybutyrate in Physiological Fluids.

Flexible and wearable sensors have attracted much attention for their applications in health monitoring and the human-machine interaction. The most studied wearable sensors have been demonstrated for sensing a limited range of metabolites such as ions, glucose, uric acid, lactate, etc. Both sweat and urine contain numerous other physiologically relevant metabolites indicative of health and wellness. This work demonstrates the use of the wearable sensor for the detection of ß-hydroxybutyrate (HB) in sweat. HB is an important biomarker for diabetic ketoacidosis, a condition caused by the accumulation of ketone bodies in hyperglycemia or metabolic acidosis patients. Herein, we fabricated an integrated sensing system coupling an HB detection chamber with a serpentine electrode for sensing physiological signals such as pulse beat, vocal cord vibration, etc. The real-time HB detection was based on a ß-hydroxybutyrate dehydrogenase enzymatic reaction. The stability of the enzyme and the cofactor couple was achieved by cross-linking networks and a redox mediator, thereby achieving high selectivity and low detection limits to HB in urine and sweat. The dual-functional sensor was integrated with a signal processing circuitry for signal transduction, conditioning, processing, wireless transmission, and real-time convenient health monitoring display to a smartphone via home-developed software.