Abstract Complex graphene electrode fabrication protocols including conventional chemical vapor deposition and graphene transfer techniques as well as more recent solution‐phase printing and postprint annealing methods have hindered the wide‐scale implementation of electrochemical devices including solid‐state ion‐selective electrodes (ISEs). Herein, a facile graphene ISE fabrication technique that utilizes laser induced graphene (LIG), formed by converting polyimide into graphene by a CO2laser and functionalization with ammonium ion (NH4+) and potassium ion (K+) ion‐selective membranes, is demonstrated. The electrochemical LIG ISEs exhibit a wide sensing range (0.1 × 10−3–150 × 10−3mfor NH4+and 0.3 × 10−3–150 × 10−3mfor K+) with high stability (minimal drop in signal after 3 months of storage) across a wide pH range (3.5–9.0). The LIG ISEs are also able to monitor the concentrations of NH4+and K+in urine samples (29–51% and 17–61% increase for the younger and older patient; respectively, after dehydration induction), which correlate well with conventional hydration status measurements. Hence, these results demonstrate a facile method to perform in‐field ion sensing and are the first steps in creating a protocol for quantifying hydration levels through urine testing in human subjects. 
                        more » 
                        « less   
                    
                            
                            Wearable Organic Electrochemical Transistor Patch for Multiplexed Sensing of Calcium and Ammonium Ions from Human Perspiration
                        
                    
    
            Abstract Wearable health monitoring has garnered considerable interest from the healthcare industry as an evolutionary alternative to standard practices with the ability to provide rapid, off‐site diagnosis and patient‐monitoring. In particular, sweat‐based wearable biosensors offer a noninvasive route to continuously monitor a variety of biomarkers for a range of physiological conditions. Both the accessibility and wealth of information of sweat make it an ideal target for noninvasive devices that can aid in early diagnosis of disease or to monitor athletic performance. Here, the integration of ammonium (NH4+) and calcium (Ca2+) ion‐selective membranes with a poly(3,4‐ethylenedioxythiophene):poly(styrenesulfonate)‐based (PEDOT:PSS) organic electrochemical transistor (OECT) for multiplexed sensing of NH4+and Ca2+in sweat with high sensitivity and selectivity is reported for the first time. The presented wearable sweat sensor is designed by combining a flexible and stretchable styrene‐ethylene‐butene‐styrene substrate with a laser‐patterned microcapillary channel array for direct sweat acquisition and delivery to the ion‐selective OECT. The resulting dermal sensor exhibits a wide working range between 0.01 × 10−3and 100 × 10−3m, well within the physiological levels of NH4+and Ca2+in sweat. The integrated devices are successfully implemented with both ex situ measurements and on human subjects with real‐time analysis using a wearable sensor assembly. 
        more » 
        « less   
        
    
                            - Award ID(s):
- 1804915
- PAR ID:
- 10458533
- Publisher / Repository:
- Wiley Blackwell (John Wiley & Sons)
- Date Published:
- Journal Name:
- Advanced Healthcare Materials
- Volume:
- 8
- Issue:
- 24
- ISSN:
- 2192-2640
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
More Like this
- 
            
- 
            Abstract Although increasing efforts have been devoted to the development of non‐invasive wearable electrochemical sweat sensors for monitoring physiological and metabolic information, most of them still suffer from poor stability and specificity over time and fluctuating temperatures. This study reports the design and fabrication of a long‐term stable and highly sensitive flexible electrochemical sensor based on nanocomposite‐modified porous graphene by facile laser treatment for detecting biomarkers such as glucose in sweat. The laser‐reduced and patterned stable conductive nanocomposite on the porous graphene electrode provides the resulting glucose sensor with an excellent sensitivity of 1317.69 µA mm−1cm−2and an ultra‐low limit of detection of 0.079 µm. The sensor can also detect pH and exhibit extraordinary stability to maintain more than 91% sensitivity over 21 days in ambient conditions. Taken together with a temperature sensor based on the same material system, the dual glucose and pH sensor integrated with a flexible microfluidic sweat sampling network further results in accurate continuous on‐body glucose detection calibrated by the simultaneously measured pH and temperature. The low‐cost, highly sensitive, and long‐term stable platform could facilitate the early identification and continuous monitoring of different biomarkers for non‐invasive disease diagnosis and treatment evaluation.more » « less
- 
            Abstract Low‐cost biosensors that can rapidly and widely monitor plant nutritional levels will be critical for better understanding plant health and improving precision agriculture decision making. In this work, fully printed ion‐selective organic electrochemical transistors (OECTs) that can detect macronutrient concentrations in whole plant sap are described. Potassium, the most concentrated cation in the majority of plants, is selected as the target analyte as it plays a critical role in plant growth and development. The ion sensors demonstrate high current (170 µA dec−1) and voltage (99 mV dec−1) sensitivity, and a low limit of detection (10 × 10−6 m). These OECT biosensors can be used to determine potassium concentration in raw sap and sap‐like aqueous environments demonstrating a log‐linear response within the expected physiological range of cations in plants. The performance of these printed devices enables their use in high‐throughput plant health monitoring in agricultural and ecological applications.more » « less
- 
            In recent years, the field of wearable sensors has undergone significant evolution, emerging as a pivotal topic of research due to the capacity of such sensors to gather physiological data during various human activities. Transitioning from basic fitness trackers, these sensors are continuously being improved, with the ultimate objective to make compact, sophisticated, highly integrated, and adaptable multi-functional devices that seamlessly connect to clothing or the body, and continuously monitor bodily signals without impeding the wearer’s comfort or well-being. Potentiometric sensors, leveraging a range of different solid contact materials, have emerged as a preferred choice for wearable chemical or biological sensors. Nanomaterials play a pivotal role, offering unique properties, such as high conductivity and surface-to-volume ratios. This article provides a review of recent advancements in wearable potentiometric sensors utilizing various solid contacts, with a particular emphasis on nanomaterials. These sensors are employed for precise ion concentration determinations, notably sodium, potassium, calcium, magnesium, ammonium, and chloride, in human biological fluids. This review highlights two primary applications, that is, (1) the enhancement of athletic performance by continuous monitoring of ion levels in sweat to gauge the athlete’s health status, and (2) the facilitation of clinical diagnosis and preventive healthcare by monitoring the health status of patients, in particular to detect early signs of dehydration, fatigue, and muscle spasms.more » « less
- 
            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
 An official website of the United States government
An official website of the United States government 
				
			 
					 
					
