Diffusion-modulated colorimetric sensor for continuous gas detection.

Due to their high sensitivity and selectivity, low cost, and good compatibility for sensor array integration, colorimetric gas sensors are widely used in hazardous gas detection, food freshness assessment, and gaseous biomarker identification. However, colorimetric gas sensors are usually designed for one-time discrete measurement because the sensing materials are entirely exposed to analytes during the sensing process. The fast consumption of sensing materials limits colorimetric sensors' applications in continuous analytes monitoring, increases the operation complexity and brings challenges for calibration. In this work, we reported a novel sensor design to prolong the lifetime of colorimetric gas sensors by engineering the gas diffusion process to preserve the sensing materials. We compared two geometries for gas diffusion control in a sensing matrix through simulation and experiment on an ammonia sensing platform. We found that the 2-dimensional gas diffusion geometry enabled a better sensor performance, including more stable and higher sensitivity and a more linear response to ammonia concentration compared to 1-dimensional gas diffusion geometry. We also demonstrated the usability of this diffusion-modulated colorimetric sensor for continuous environmental ammonia monitoring.

Hydrogel-incorporated Colorimetric Sensors with High Humidity Tolerance for Environmental Gases Sensing.

Humidity interferes most gas sensors, especially colorimetric sensors. The conventional approaches to minimize the humidity interference in colorimetric gas sensing require using extra components, causing unwanted analytes loss, or limiting the choices of sensing probes to only hydrophobic ones. To explore the possibility of minimizing the humidity interference in a hydrophilic colorimetric sensing system, we have developed a hydrogel-incorporated approach to buffer the humidity influence on the colorimetric gas sensing. The hydrogel-incorporated colorimetric sensors show not only high humidity tolerance but also the improved analytical performance. The accuracy and reliability of the hydrogel-incorporated colorimetric sensors have also been validated in field tests. This hydrogel-incorporated approach will open up an avenue to implement hydrophilic recipes into colorimetric gas sensors and extend the application of colorimetric sensors to humid gases detection.

Wearable Transcutaneous CO2 Monitor Based on Miniaturized Nondispersive Infrared Sensor.

Transcutaneous oxygen and carbon dioxide provide the status of pulmonary gas exchange and are of importance in diagnosis and management of respiratory diseases. Though significant progress has been made in oximetry, not much has been explored in developing wearable technologies for continuous monitoring of transcutaneous carbon dioxide. This research reports the development of a truly wearable sensor for continuous monitoring of transcutaneous carbon dioxide using miniaturized nondispersive infrared sensor augmented by hydrophobic membrane to address the humidity interference. The wearable transcutaneous CO2 monitor shows well-behaved response curve to humid CO2 with linear response to CO2 concentration. The profile of transcutaneous CO2 monitored by the wearable device correlates well with the end-tidal CO2 trend in human test. The feasibility of the wearable device for passive and unobstructed tracking of transcutaneous CO2 in free-living conditions has also been demonstrated in field test. The wearable transcutaneous CO2 monitoring technology developed in this research can be widely used in remote assessment of pulmonary gas exchange efficiency for patients with respiratory diseases, such as COVID-19, sleep apnea, and chronic obstructive pulmonary disease (COPD).

Integrating Electrochemical and Colorimetric Sensors with a Webcam Readout for Multiple Gas Detection.

Multisensor detectors have merits of low cost, compact size, and capability of supplying accurate and reliable information otherwise hard to obtain by any single sensors. They are therefore highly desired in various applications. Despite the advantages and needs, they face great challenges in technique especially when integrating sensors with different sensing principles. To bridge the gap between the demand and technique, we here demonstrated an integration of electrochemical and colorimetric sensors with a webcam readout for multiple gas detection. Designed with two parallel gas channels but independent sensor cells, the dual-sensor detector could simultaneously detect each gas from their gas mixture by analysis of the group photo of the two sensors. Using Ag electro-dissolution as reporter, the bipolar electrochemical sensor achieved quantitative analysis for the first time thanks to application of pulse voltage. The sacrificed Ag layer used in the bipolar electrochemical (EC) sensor was recycled from CD, which further decreased the sensor cost and supplied a new way of CD recycling. The EC O2 sensor response, edge displacement of Ag layer due to electrochemical dissolution, has a linear relationship with O2 concentration ranging from 0 to 30% and has good selectivity to common oxidative gases. The colorimetric NO2 sensor linearly responded to NO2 concentrations ranging from 0 to 230 ppb with low detection limit of 10 ppb, good selectivity, and humidity tolerance. This integration method could be extended to integrating other gas sensors.

Reliable Breathing Tracking with Wearable Mask Device.

Breathing tracking is critical for the assessment of lung functions, exercise physiologies, and energy expenditure. Conventional methods require using a face mask or mouthpiece that is connected to a stationary equipment through a tube, restricting the location, movement, or even the posture. To obtain accurate breathing physiology parameters that represent the true state of the patient during different scenarios, a wearable technology that has less intervention to patient's activities in free-living conditions is highly preferred. Here, we propose a miniaturized, reliable, and wide-dynamic ranged flow sensing technology that is immune to orientation, movement, and noise. As far as we know, this is the first work of introducing a fully integrated mask device focusing on breath tracking in free-living conditions. There are two key challenges for achieving this goal: miniaturized flow sensing and motion-induced artifacts elimination. To address these challenges, we come up with two technical innovations: 1) in hardware wise, we have designed an integrated flow sensing technique based on differential pressure Pneumotach approach and motion sensing; 2) in software wise, we have developed comprehensive algorithms based baseline tracking and orientation and motion compensation. The effectiveness of the proposed technology has been proven by the experiments. Experimental results from simulator and real breath conditions show high correlation (R2 = 0.9994 and 0.9964 respectively) and mean error within 2.5% for Minute Volume (VE), when compared to values computed from reference methods. These results show that the proposed method is accurate and reliable to track the key breath parameters in free-living conditions.

Light-Controlled Configurable Colorimetric Sensing Array.

Colorimetry is a popular gas-sensing platform, but it is typically limited to one-time use only. Here, we introduce a light-controlled configurable colorimetric sensing array to overcome this limitation. It features a photoactivated reaction between an analyte and a sensing material, such that sensing of an array element can be turned on and off with light. By sequential turning on of each array element, the sensor array can be used multiple times as determined by the number of array elements. This is analogous to a data storage device, which lasts until every storage element is used up. The total number of array elements and the area of each array element are configurable with light. With use of a smartphone screen as a programmable light source, we applied the sensing platform to the detection of oxygen gas and studied the relationship between sensitivity, noise, detection time, and array size. The relationship can be used to configure the array to meet the specifications of different applications.

Chemical Sensing in Real Time with Plants Using a Webcam.

It has been established that plants can smell and respond to chemicals in order to adapt to and survive in a changing chemical environment. Here we show that a plant responds to chemicals in air, and the response can be detected rapidly to allow tracking of air pollution in real time. We demonstrate this capability by detecting subtle color and shape changes in the leaves of mosses upon exposure to sulfur dioxide in air with a simple webcam and an imaging-processing algorithm. The leaves of mosses consist of a monolayer of cells, providing a large surface-to-volume ratio for highly sensitive chemical sensing. The plant sensor responds linearly to sulfur dioxide within a wide concentration range (0-180 ppm), and it can tolerate humidity variation (15-85% relative humidity) and chemical interference and regenerate itself. We envision that plants can help alert chemical exposure danger as a part of our living environment using low-cost CMOS imagers, and their chemical-sensing capabilities may be further improved with genetic engineering.

Gradient-Based Colorimetric Sensors for Continuous Gas Monitoring.

Colorimetry detects a color change resulted from a chemical reaction or molecular binding. Despite its widespread use in sensing, continuous monitoring of analytes with colorimetry is difficult, especially when the color-producing reaction or binding is irreversible. Here, we report on a gradient-based colorimetric sensor (GCS) to overcome this limitation. Lateral transport of analytes across a colorimetric sensor surface creates a color gradient that shifts along the transport direction over time, and GCS tracks the gradient shift and converts it into analyte concentration in real time. Using a low cost complementary metal-oxide semiconductor imager and imaging processing algorithm, we show submicrometer gradient shift tracking precision and continuous monitoring of ppb-level ozone.

Tracking Personal Health-Environment Interaction with Novel Mobile Sensing Devices.

The development of connected health devices has allowed for a more accurate assessment of a person's state under free-living conditions. In this work, we use two mobile sensing devices and investigate the correlation between individual's resting metabolic rate (RMR) and volatile organic compounds (VOCs) exposure levels. A total of 17 healthy, young, and sedentary office workers were recruited, measured for RMR with a mobile indirect calorimetry (IC) device, and compared with their corresponding predicted RMR values from the Academy of Nutrition and Dietetics' recommended epidemiological equation, the Mifflin⁻St Jeor equation (MSJE). Individual differences in the RMR values from the IC device and the epidemiological equation were found, and the subjects' RMRs were classified as normal, high, or low based on a cut-off of ±200 kcal/day difference with respect to the predicted value. To study the cause of the difference, VOCs exposure levels of each participant's daytime working environment and nighttime resting environment were assessed using a second mobile sensing device for VOCs exposure detection. The results showed that all sedentary office workers had a low VOCs exposure level (<2 ppmC), and there was no obvious correlation between VOCs exposure and the RMR difference. However, an additional participant who was a worker in an auto repair shop, showed high VOCs exposure with respect to the sedentary office worker population and a significant difference between measured and predicted RMR, with a low RMR of 500 kcal/day difference. The mobile sensing devices have been demonstrated to be suitable for the assessment of direct information of human health⁻environment interactions at free-living conditions.

Thermochemical Humidity Detection in Harsh or Non-Steady Environments.

We present a new method of chemical quantification utilizing thermal analysis for the detection of relative humidity. By measuring the temperature change of a hydrophilically-modified temperature sensing element vs. a hydrophobically-modified reference element, the total heat from chemical interactions in the sensing element can be measured and used to calculate a change in relative humidity. We have probed the concept by assuming constant temperature streams, and having constant reference humidity (~0% in this case). The concept has been probed with the two methods presented here: (1) a thermistor-based method and (2) a thermographic method. For the first method, a hydrophilically-modified thermistor was used, and a detection range of 0-75% relative humidity was demonstrated. For the second method, a hydrophilically-modified disposable surface (sensing element) and thermal camera were used, and thermal signatures for different relative humidity were demonstrated. These new methods offer opportunities in either chemically harsh environments or in rapidly changing environments. For sensing humidity in a chemically harsh environment, a hydrophilically-modified thermistor can provide a sensing method, eliminating the exposure of metallic contacts, which can be easily corroded by the environment. On the other hand, the thermographic method can be applied with a disposable non-contact sensing element, which is a low-cost upkeep option in environments where damage or fouling is inevitable. In addition, for environments that are rapidly changing, the thermographic method could potentially provide a very rapid humidity measurement as the chemical interactions are rapid and their changes are easily quantified.

A Novel Wireless Wearable Volatile Organic Compound (VOC) Monitoring Device with Disposable Sensors.

A novel portable wireless volatile organic compound (VOC) monitoring device with disposable sensors is presented. The device is miniaturized, light, easy-to-use, and cost-effective. Different field tests have been carried out to identify the operational, analytical, and functional performance of the device and its sensors. The device was compared to a commercial photo-ionization detector, gas chromatography-mass spectrometry, and carbon monoxide detector. In addition, environmental operational conditions, such as barometric change, temperature change and wind conditions were also tested to evaluate the device performance. The multiple comparisons and tests indicate that the proposed VOC device is adequate to characterize personal exposure in many real-world scenarios and is applicable for personal daily use.

Acetone as biomarker for ketosis buildup capability--a study in healthy individuals under combined high fat and starvation diets.

BACKGROUND: Ketogenic diets are high fat and low carbohydrate or very low carbohydrate diets, which render high production of ketones upon consumption known as nutritional ketosis (NK). Ketosis is also produced during fasting periods, which is known as fasting ketosis (FK). Recently, the combinations of NK and FK, as well as NK alone, have been used as resources for weight loss management and treatment of epilepsy. METHODS: A crossover study design was applied to 11 healthy individuals, who maintained moderately sedentary lifestyle, and consumed three types of diet randomly assigned over a three-week period. All participants completed the diets in a randomized and counterbalanced fashion. Each weekly diet protocol included three phases: Phase 1 - A mixed diet with ratio of fat: (carbohydrate + protein) by mass of 0.18 or the equivalence of 29% energy from fat from Day 1 to Day 5. Phase 2- A mixed or a high-fat diet with ratio of fat: (carbohydrate + protein) by mass of approximately 0.18, 1.63, or 3.80 on Day 6 or the equivalence of 29%, 79%, or 90% energy from fat, respectively. Phase 3 - A fasting diet with no calorie intake on Day 7. Caloric intake from diets on Day 1 to Day 6 was equal to each individual's energy expenditure. On Day 7, ketone buildup from FK was measured. RESULTS: A statistically significant effect of Phase 2 (Day 6) diet was found on FK of Day 7, as indicated by repeated analysis of variance (ANOVA), F(2,20) = 6.73, p < 0.0058. Using a Fisher LDS pair-wise comparison, higher significant levels of acetone buildup were found for diets with 79% fat content and 90% fat content vs. 29% fat content (with p = 0.00159**, and 0.04435**, respectively), with no significant difference between diets with 79% fat content and 90% fat content. In addition, independent of the diet, a significantly higher ketone buildup capability of subjects with higher resting energy expenditure (R(2) = 0.92), and lower body mass index (R(2) = 0.71) was observed during FK.

Colorimetric humidity sensor based on liquid composite materials for the monitoring of food and pharmaceuticals.

Using supported ionic-liquid membrane (SILM)-inspired methodologies, we have synthesized, characterized, and developed a humidity sensor by coating a liquid composite material onto a hygroscopic, porous substrate. Similar to pH paper, the sensor responds to the environment's relative humidity and changes color accordingly. The humidity indicator is prepared by casting a few microliters of low-toxicity reagents on a nontoxic substrate. The sensing material is a newly synthesized liquid composite that comprises a hygroscopic medium for environmental humidity capture and a color indicator that translates the humidity level into a distinct color change. Sodium borohydride was used to form a liquid composite medium, and DenimBlu30 dye was used as a redox indicator. The liquid composite medium provides a hygroscopic response to the relative humidity, and DenimBlu30 translates the chemical changes into a visual change from yellow to blue. The borate-redox dye-based humidity sensor was prepared, and then Fourier transform infrared spectroscopy, differential scanning calorimetry, and image analysis methods were used to characterize the chemical composition, optimize synthesis, and gain insight into the sensor reactivity. Test results indicated that this new sensing material can detect relative humidity in the range of 5-100% in an irreversible manner with good reproducibility and high accuracy. The sensor is a low-cost, highly sensitive, easy-to-use humidity indicator. More importantly, it can be easily packaged with products to monitor humidity levels in pharmaceutical and food packaging.

A Novel Real-time Carbon Dioxide Analyzer for Health and Environmental Applications.

To be able to detect carbon dioxide (CO2) with high accuracy and fast response time is critical for many health and environmental applications. We report on a pocket-sized CO2 sensor for real-time analysis of end-tidal CO2, and environmental CO2. The sensor shows fast and reversible response to CO2 over a wide concentration range, covering the needs of both environmental and health applications. It is also immune to the presence of various interfering gases in ambient or expired air. Furthermore, the sensor has been used for real-time breath analysis, and the results are in good agreement with those from a commercial CO2 detector.

Manipulating the diffusion energy barrier at the lithium metal electrolyte interface for dendrite-free long-life batteries.

Constructing an artificial solid electrolyte interphase (SEI) on lithium metal electrodes is a promising approach to address the rampant growth of dangerous lithium morphologies (dendritic and dead Li0) and low Coulombic efficiency that plague development of lithium metal batteries, but how Li+ transport behavior in the SEI is coupled with mechanical properties remains unknown. We demonstrate here a facile and scalable solution-processed approach to form a Li3N-rich SEI with a phase-pure crystalline structure that minimizes the diffusion energy barrier of Li+ across the SEI. Compared with a polycrystalline Li3N SEI obtained from conventional practice, the phase-pure/single crystalline Li3N-rich SEI constitutes an interphase of high mechanical strength and low Li+ diffusion barrier. We elucidate the correlation among Li+ transference number, diffusion behavior, concentration gradient, and the stability of the lithium metal electrode by integrating phase field simulations with experiments. We demonstrate improved reversibility and charge/discharge cycling behaviors for both symmetric cells and full lithium-metal batteries constructed with this Li3N-rich SEI. These studies may cast new insight into the design and engineering of an ideal artificial SEI for stable and high-performance lithium metal batteries.

Frontiers of Wearable Biosensors for Human Health Monitoring.

Wearable biosensors offer noninvasive, real-time, and continuous monitoring of diverse human health data, making them invaluable for remote patient tracking, early diagnosis, and personalized medicine [...].

Decreasing Water Activity Using the Tetrahydrofuran Electrolyte Additive for Highly Reversible Aqueous Zinc Metal Batteries.

Aqueous zinc metal batteries show great promise in large-scale energy storage. However, the decomposition of water molecules leads to severe side reactions, resulting in the limited lifespan of Zn batteries. Here, the tetrahydrofuran (THF) additive was introduced into the zinc sulfate (ZnSO4) electrolyte to reduce water activity by modulating the solvation structure of the Zn hydration layer. The THF molecule can play as a proton acceptor to form hydrogen bonds with water molecules, which can prevent water-induced undesired reactions. Thus, in an optimal 2 M ZnSO4/THF (5% by volume) electrolyte, the hydrogen evolution reaction and byproduct precipitation can be suppressed, which greatly improves the cycling stability and Coulombic efficiency of reversible Zn plating/stripping. The Zn symmetrical cells exhibit ultralong working cycles with a wide range of current density and capacity. The THF additive also enables a high Coulombic efficiency in the Zn||Cu cell with an average value of 99.59% over 400 cycles and a high reversible capacity with a capacity retention of 97.56% after 250 cycles in the Zn||MnO2 full cells. This work offers an effective strategy with high scalability and low cost for the protection of the Zn metal electrodes in aqueous rechargeable batteries.

A Novel Acetone Sensor for Body Fluids.

Ketones are well-known biomarkers of fat oxidation produced in the liver as a result of lipolysis. These biomarkers include acetoacetic acid and ß-hydroxybutyric acid in the blood/urine and acetone in our breath and skin. Monitoring ketone production in the body is essential for people who use caloric intake deficit to reduce body weight or use ketogenic diets for wellness or therapeutic treatments. Current methods to monitor ketones include urine dipsticks, capillary blood monitors, and breath analyzers. However, these existing methods have certain disadvantages that preclude them from being used more widely. In this work, we introduce a novel acetone sensor device that can detect acetone levels in breath and overcome the drawbacks of existing sensing approaches. The critical element of the device is a robust sensor with the capability to measure acetone using a complementary metal oxide semiconductor (CMOS) chip and convenient data analysis from a red, green, and blue deconvolution imaging approach. The acetone sensor device demonstrated sensitivity of detection in the micromolar-concentration range, selectivity for detection of acetone in breath, and a lifetime stability of at least one month. The sensor device utility was probed with real tests on breath samples using an established blood ketone reference method.

Online sample conditioning for portable breath analyzers.

Various innovative chemical sensors have been developed in recent years to sense dangerous substances in air and trace biomarkers in breath. However, in order to solve real world problems, the sensors must be equipped with efficient sample conditioning that can, e.g., control the humidity, which is discussed much less in the literature. To meet the demand, a miniaturized mouthpiece was developed for personal breath analyzers. A key function of the mouthpiece is to condition the humidity in real breath samples without changing the analyte concentrations and introducing substantial backpressure, which is achieved with optimized packing of desiccant particles. Numerical simulations were carried out to determine the performance of the mouthpiece in terms of various controllable parameters, such as the size, density, and geometry of the packing. Mouthpieces with different configurations were built and tested, and the experimental data validated the simulation findings. A mouthpiece with optimized performance reducing relative humidity from 95% (27,000 ppmV) to 29% (8000 ppmV) whereas retaining 92% nitric oxide (50 ppbV to 46 ppbV) was built and integrated into a hand-held exhaled nitric oxide sensor, and the performance of exhaled nitric oxide measurement was in good agreement with the gold standard chemiluminescence technique. Acetone, carbon dioxide, oxygen, and ammonia samples were also measured after passing through the desiccant mouthpiece using commercial sensors to examine wide applicability of this breath conditioning approach.

Detection of transdermal biomarkers using gradient-based colorimetric array sensor.

Accurate assessment of dietary macronutrients intake is critical for the effective management of multiple diseases, such as obesity, diabetes, cardiovascular disease, metabolic disease, and cancer. Conventional self-reporting method is burdensome, inaccurate, and often biased. Though blood analysis and breath analysis can provide evidence-based information, they are either invasive or subject to human errors. Here we reported a wearable transdermal volatile biomarkers detection system based on novel colorimetric sensing technology for dietary macronutrients intake assessment. This technique quantifies the emission rates of transdermal volatile biomarkers via a gradient-based colorimetric array sensor (GCAS). The optical system of the GCAS device tracks the localized color development associated with the chemical reaction between the volatile biomarkers and the porous sensing probes, and determines the biomarkers emission rates through image processing algorithms. The localized chemical reaction and the image-based signal processing also make the GCAS capable for multiplexed detection of multiple analytes simultaneously. The GCAS sensor has been applied for transdermal acetone detection on 5 subjects in a keto diet intervention. The study indicates that the transdermal acetone increases after the subjects consuming keto diets and it decreases to basal level after intaking carb-rich diets. The transdermal acetone response from the GCAS sensor correlates well with breath acetone concentration in the range between 0 and 40 ppm and the correlation factor (R2) is as high as 0.8877. This method provides a noninvasive, low-cost, and wearable tool for assessing dietary macronutrients intake outside of lab or hospital settings. It could be widely applied in disease management, weight control, and nutrition management.