NFC-enabled photothermal-based microfluidic paper analytical device for glucose detection.

This study introduces the development of a photothermal-based microfluidic paper analytical device (PT-µPAD) integrated with near-field communication (NFC) technology and smartphone readout for enzyme-free glucose quantification in human samples. With the properties of gold nanoparticles (AuNPs) both as a nanozyme and as a photothermal substrate, there is no need for costly reagents like enzymes or a readout instrumentation for the selective and sensitive detection of glucose. In PT-µPADs, AuNPs are etched by hydrogen peroxide (H2O2) generated from glucose catalysis. Photothermal detection from the plasmonic heating of these AuNPs when illuminated by a 533nm LED light source is achieved by inserting the PT-µPAD sensor into a portable NFC platform suitable for smartphone readout. Temperature variation is directly proportional to the glucose concentration. After optimization, we acquired a linear range between 5.0 and 20.0 µmol L-1 (R2 = 0.9967) and a limit of detection (LOD) of 25.0 nmol L-1 for glucose. Additionally, while our sensor does not utilize any enzyme, it is remarkably selective to glucose with no effects from interferences. Recovery studies in various human control samples indicated a range of 99.73-102.66% with the highest RSD of 3.53%, making it highly accurate and precise. Moreover, our method is more sensitive than other methods relying on conventional µPADs for glucose sensing. By integrating the potential benefits of microfluidics, nanomaterials as nanozymes, and NFC technology for wireless readout, our sensor demonstrates great promise as an accessible, affordable, and shelf-stable device for glucose quantification. Moreover, this concept can be extended to detect other molecules of interest as a point-of-care (POC) diagnostics device.

Distance-based paper analytical devices integrated with molecular imprinted polymers for Escherichia coli quantification.

The development of distance-based paper analytical devices (dPADs) integrated with molecularly imprinted polymers (MIPs) to monitor Escherichia coli (E. coli) levels in food samples is presented. The fluidic workflow on the device is controlled using a designed hydrophilic bridge valve. Dopamine serves as a monomer for the formation of the E. coli-selective MIP layer on the dPADs. The detection principle relies on the inhibition of the E. coli toward copper (II) (Cu2+)-triggered oxidation of o-phenylenediamine (OPD) on the paper substrate. Quantitative detection is simply determined through visual observation of the residual yellow color of the OPD in the detection zone, which is proportional to E. coli concentration. The sensing exhibits a linear range from 25.0 to 1200.0 CFU mL-1 (R2 = 0.9992) and a detection limit (LOD) of 25.0 CFU mL-1 for E. coli detection. Additionally, the technique is highly selective with no interference even from the molecules that have shown to react with OPD to form oxidized OPD. The developed device demonstrates accuracy and precision for E. coli quantification in food samples with recovery percentages between 98.3 and 104.7% and the highest relative standard deviation (RSD) of 4.55%. T-test validation shows no significant difference in E. coli concentration measured between our method and a commercial assay. The proposed dPAD sensor has the potential for selective and affordable E. coli determination  in food samples without requiring sample preparation. Furthermore, this strategy can be extended to monitor other molecules for which MIP can be developed and integrated into paper-microfluidic platform.

Simple distance-based thread analytical device integrated with ion imprinted polymer for Zn2+ quantification in human urine samples.

This article presents the development of a distance-based thread analytical device (dTAD) integrated with an ion-imprinted polymer (IIP) for quantitative monitoring of zinc ions (Zn2+) in human urine samples. The IIP was easily chemically modified onto the thread channel using dithizone (DTZ) as a ligand to bind to Zn2+ with methacrylic acid (MAA) as a functional monomer and ethylene glycol dimethacrylate (EGDMA) as well as 2,2-azobisisobutyronitrile (AIBN) as cross-linking agents to enhance the selectivity for Zn2+ detection. The imprinted polymer was characterized using Attenuated Total Reflectance-Fourier Transform Infrared (ATR-FTIR) spectroscopy and Scanning Electron Microscopy-Energy Dispersive X-ray Spectroscopy (SEM-EDS). Under optimization, the linear detection range was from 1.0 to 20.0 mg L-1 (R2 = 0.9992) with a limit of detection (LOD) of 1.0 mg L-1. Other potentially interfering metal ions and molecules did not interfere with this approach, leading to high selectivity. Furthermore, our technique exhibits a remarkable recovery ranging from 100.48% to 103.16%, with the highest relative standard deviation (% RSD) of 5.44% for monitoring Zn2+ in human control urine samples, indicating high accuracy and precision. Similarly, there is no significant statistical difference between the results obtained using our method and standards on zinc supplement sample labels. The proposed method offers several advantages in detecting trace Zn2+ for point-of-care (POC) medical diagnostics and environmental sample analysis, such as ease of use, instrument-free readout, and cost efficiency. Overall, our developed dTAD-based IIP method holds potential for simple, affordable, and rapid detection of Zn2+ levels and can be applied to other metal ions' analysis.

Distance-based paper analytical device for multiplexed quantification of cytokine biomarkers using carbon dots integrated with molecularly imprinted polymer.

This article introduces distance-based paper analytical devices (dPADs) integrated with molecularly imprinted polymers (MIPs) and carbon dots (CDs) for simultaneous quantification of cytokine biomarkers, namely C-reactive protein (CRP), tumor necrosis factor-alpha (TNF-α), and interleukin-6 (IL-6) in human biological samples for diagnosis of cytokine syndrome. Using fluorescent CDs and MIP technology, the dPAD exhibits high selectivity and sensitivity. Detection is based on fluorescence quenching of CDs achieved through the interaction of the target analytes with the MIP layer on the paper substrate. Quantitative analysis is easily accomplished by measuring the distance length of quenched fluorescence with a traditional ruler and naked eye readout enabling rapid diagnosis of cytokine syndrome and the underlying infection. Our sensor demonstrated linear ranges of 2.50-24.0 pg mL-1 (R2 = 0.9974), 0.25-3.20 pg mL-1 (R2 = 0.9985), and 1.50-16.0 pg mL-1 (R2 = 0.9966) with detection limits (LODs) of 2.50, 0.25, and 1.50 pg mL-1 for CRP, TNF-α, and IL-6, respectively. This sensor also demonstrated remarkable selectivity compared to a sensor employing a non-imprinted polymer (NIP), and precision with the highest relative standard deviation (RSD) of 5.14%. The sensor is more accessible compared to prior methods relying on expensive reagents and instruments and complex fabrication methods. Furthermore, the assay provided notable accuracy for monitoring these biomarkers in various human samples with recovery percentages ranging between 99.22% and 103.58%. By integrating microfluidic systems, nanosensing, and MIPs technology, our developed dPADs hold significant potential as a cost-effective and user-friendly analytical method for point-of-care diagnostics (POC) of cytokine-related disorders. This concept can be further extended to developing diagnostic devices for other biomarkers.

Ultrasensitive electrochemical sensor for detection of salivary cortisol in stress conditions.

A natural stress response induces elevated cortisol levels in biological fluids, such as saliva. While current sensor technologies can detect cortisol in real time, their sensitivity and reliability for human subjects have not been assured. This is due to relatively low concentrations of salivary cortisol, which fluctuate throughout the day and vary significantly between individuals. To address these challenges, we present an improved electrochemical biosensor leveraging graphene's exceptional conductivity and physicochemical properties. A 1-pyrenebutyric acid N-hydroxysuccinimide ester (PBASE-NHS)-modified commercial graphene foam (GF) electrode is presented to realize an ultra-sensitive biosensor for cortisol detection directly in human saliva. The biosensor fabrication process entails the attachment of anti-cortisol monoclonal antibodies (mAb-cort) onto a PBASE-NHS/GF electrode through noncovalent immobilization on the vertically stratified graphene foam electrode surface. This unique immobilization strategy preserves graphene's structural integrity and electrical conductivity while facilitating antibody immobilization. The binding of cortisol to immobilized mAb-cort is read out via differential pulse voltammetry using ferri/ferro redox reactions. The immunosensor demonstrates an exceptional dynamic range of 1.0 fg mL-1 to 10,000 pg mL-1 (R2 = 0.9914) with a detection limit of 0.24 fg mL-1 (n = 3) for cortisol. Furthermore, we have established the reliability of cortisol sensors in monitoring human saliva. We have also performed multiple modes of validation, one against the established enzyme-linked immunosorbent assay (ELISA) and a second by a third-party service Salimetric on 16 student volunteers exposed to different stress levels, showing excellent correlation (r = 0.9961). These findings suggest the potential for using mAb-cort/PBASE-NHS/GF-based cortisol electrodes for monitoring salivary cortisol in the general population.

Soft Injectable Sutures for Dose-Controlled and Continuous Drug Delivery.

Transdermal drug delivery offers a promising alternative to traditional methods such as oral ingestion and hypodermic injection. Hypodermic injections are painful, while oral ingestion requires higher doses due to enzymatic degradation and poor absorption. While microneedles address the pain issue, they are limited to delivering small amounts of drugs and can be impractical due to peeling off with motion and sweat. Herein, this work proposes soft injectables using drug-carrying sutures for painless and localized sustained delivery in the dermis. These sutures can remain in place during delivery and are suitable for all skin types. Surgical sutures can also serve as open capillary microfluidic channels carrying drug from a wearable drug reservoir to enable long-term (weeks to months) transdermal drug delivery. The experiments focus on delivering 5-fluorouracil (5-FU), a cancer drug, and rhodamine B, a drug model. A fixed-length suture of 60 cm delivers 0.43 mg of 5-flurouracil in 15 min. The experiments also demonstrate a continuous drug delivery of rhodamine B for over 8 weeks at a rate of 0.0195 mL h-1 . The results highlight that soft injectable sutures are promising candidates for long-term sustained delivery of varying quantities of drugs over weeks period compared to hypodermic injection, oral ingestion, or microneedles.

Gold Nanomaterial-Based Microfluidic Paper Analytical Device for Simultaneous Quantification of Gram-Negative Bacteria and Nitrite Ions in Water Samples.

This study presents a rapid microfluidic paper-based analytical device (µPAD) capable of simultaneously monitoring Gram-negative bacteria and nitrite ions (NO2-) for water quality monitoring. We utilize gold nanoparticles (AuNPs) functionalized with polymyxin molecules (AuNPs@polymyxin) to cause color change due to aggregation for the detection of Gram-negative bacteria, and antiaggregation in the presence of o-phenylenediamine (OPD) for NO2- detection. In this study, Escherichia coli (E. coli) serves as the model of a Gram-negative bacterium. Using the developed µPADs, the color changes resulting from aggregation and antiaggregation reactions are measured using a smartphone application. The linear detection ranges from 5.0 × 102 to 5.0 × 105 CFU/mL (R2 = 0.9961) for E. coli and 0.20 to 2.0 µmol/L (R2 = 0.995) for NO2-. The detection limits were determined as 2.0 × 102 CFU/mL for E. coli and 0.18 µmol/L for NO2-. Notably, the newly developed assay exhibited high selectivity with no interference from Gram-positive bacteria. Additionally, we obtained acceptable recovery for monitoring E. coli and NO2- in drinking water samples with no significant difference between our method and a commercial assay by t test validation. The sensor was also employed for assessing the quality of the pond and environmental water source. Notably, this approach can also be applied to human urine samples with satisfactory accuracy. Furthermore, the assay's stability is extended due to its reliance on AuNPs rather than reagents like antibodies and enzymes, reducing costs and ensuring long-term viability. Our cost-effective µPADs therefore provide a real-time analysis of both contaminants, making them suitable for assessing water quality in resource-limited settings.

Smart sensing flexible sutures for glucose monitoring in house sparrows.

There is a need for flexible chemical sensors for the ecological and physiological research of avian species such as house sparrows (Passer domesticus). Current methods in this field are invasive and require multiple physical interactions with the birds. Emerging research in flexible bioelectronics can enable realization of implantable devices that are mechanically compliant with the underlying tissues for continuous real-time sensing in situ. However, challenges still remain in forming an intimate flexible interface. One of the promising flexible bioelectronic platforms for tissue-embedded sensing is based on functionalizing surgical sutures or threads. Threads have three-dimensional flexibility, high surface-area-to-volume ratio, inherent wicking properties, and are easily functionalizable using reel-to-reel dip coating. Threads are ideal as they are lightweight, therefore, would not interfere with flight motion and would only require minimal interaction with the bird. However, the challenge remains in achieving a highly conductive yet flexible electrode for electrochemical sensing using materials such as gold. In this study, we address this issue through novel gold deposition directly on thread substrate followed by enzyme immobilization to realize flexible electrochemical glucose biosensors on medical-grade sutures. These sensors were calibrated and tested in a range that is wide enough to include the expected range of glucose concentration in house sparrows (0-8.55 mM). Glucose monitoring in house sparrows will provide insights into energy metabolism and regulation during stress responses. In addition, the stability, repeatability, and selectivity of the sensor were tested with final validation in a real bird. Our innovative gold-coated, thread-based flexible electrochemical glucose sensor can also be used in other small and large animals. This can also be extended to monitoring other metabolites in future.

Ingestible pH sensing device for gastrointestinal health monitoring based on thread-based electrochemical sensors.

There exists a strong correlation between the pH levels of the gastrointestinal (GI) tract and GI diseases such as inflammatory bowel disease (IBS), ulcerative colitis, and pancreatis. Existing methods for diagnosing many GI diseases predominantly rely on invasive, expensive, and time-consuming techniques such as colonoscopy and endoscopy. In this study, an autonomous ingestible smart biosensing system in a pill format with integrated pH sensors is reported. The smart sensing pills will measure the pH profile as they transit through the GI tract. The data is then downloaded from the pills after they are collected from the feces. The sensor is based on electrodeposited PANI on carbon-coated conductive threads providing high pH sensitivity. Engineering innovations allowed integration of thread-based sensors on 3D-printed pill surfaces with front-end readout electronics, memory, and microcontroller assembled on mm-size circular printed circuit boards. The entire smart sensing pill possesses an overall length of 22.1 mm and an outer diameter of 9 mm. The modular biosensing system allows integration of thread-based biosensors to monitor other biomarkers in GI tract that mitigates the complex sensor fabrication process as well as overall pill assembly.

Highly Sensitive Photothermal Microfluidic Thread-Based Duplex Immunosensor for Point-of-Care Monitoring.

Herein, we successfully developed a thread-based analytical device (µTAD) for simultaneous immunosensing of two biomolecules with attomolar sensitivity by using a photothermal effect. A photothermal effect exploits a strong light-to-heat energy conversion of plasmonic metallic nanoparticles at localized surface plasmon resonance. The key innovation is to utilize the cotton thread to realize this sensor and the use of chitosan modification for enhancing the microfluidic properties, for improving the efficiency of photothermal conversion, and for sensor stability. The developed µTAD sensor consists of (i) a sample zone, (ii) a conjugation zone coated with gold nanoparticles bound with an antibody (AuNPs-Ab2), and (iii) a test zone immobilized with a capture antibody (anti-Ab1). The prepared µTAD is assembled in a custom three-dimensional (3D) printed device which holds the laser for illumination and the thermometer for readout. The 3D-printed supportive device enhances signal response by focusing light and localizing the heat generated. For proof of concept, simultaneous sensing of two key stress and inflammation biomarkers, namely, cortisol and interleukin-6 (IL-6), are monitored using this technique. Under optimization, this device exhibited a detection linear range of 2.0-14.0 ag/mL (R2 = 0.9988) and 30.0-360.0 fg/mL (R2 = 0.9942) with a detection limit (LOD) of 1.40 ag/mL (∼3.86 amol/L) and 20.0 fg/mL (∼950.0 amol/L) for cortisol and IL-6, respectively. Furthermore, the analysis of both biomolecules in human samples indicated recoveries in the range of 98.8%-102.88% with the highest relative standard deviation being 3.49%, offering great accuracy and precision. These results are the highest reported sensitivity for these analytes using an immunoassay method. Our PT-µTAD strategy is therefore a promising approach for detecting biomolecules in resource-limited point-of-care settings.

Tunable Radio Frequency Antenna Based on Phase Change Materials.

In conventional communication systems, dedicated tunable circuit elements are used to realize different functions and achieve performance metrics. For example, tuning the center frequency or the input impedance of an antenna in a radio frequency (RF) system is performed by complex impedance-matching circuits. In this paper, the antenna utilizes the temperature-induced irreversible mechanical deformation of a shape memory alloy (SMA) as a natural way to tune the antenna's shape and configuration, thereby providing inherent tunability without bulky circuit elements. This paradigm of material programming for impedance tuning of an SMA-based antenna is validated by both numerical simulation and measurements.

Nanomaterials integrated with microfluidic paper-based analytical devices for enzyme-free glucose quantification.

In this study, nanomaterials capable of enzyme-free glucose quantification and colorimetric readout are integrated into a microfluidic paper-based analytical devices (µPADs). Gold nanoparticles (AuNPs) and silver nanoparticles (AgNPs) were utilized as a peroxidase-like nanozyme and a colorimetric probe to achieve glucose monitoring. In this developed device, glucose is oxidized by AuNPs to generate hydrogen peroxide (H2O2), which flows in the paper microchannels toward detection zones. H2O2 then etches the immobilized AgNPs to induce a color change. The intensity of color change is easily monitored using a smartphone application. Following method optimization, we obtained a linear range from 0.50 to 10.0 mmol L-1 (R2 = 0.9921) and a detection limit (LOD) of 340.0 µmol L-1. This falls in the clinically relevant range for glucose monitoring and diabetes diagnosis in humans. In addition, the total analysis time is just 20 min, which is significantly less than the same experiment performed in the solution phase. Also, our method is markedly selective; other substrates do not interfere. The recovery test in human control samples was in the range of 98.47-102.34% and the highest relative standard deviation (RSD) was 3.58%. The enzyme-free approach for glucose sensing is highly desirable for diabetes diagnosis as it replaces the more expensive enzyme with cheaper nanomaterials. Furthermore, since nanomaterials are more environmentally stable compared to enzymes, it has the potential for widespread deployment as point-of-care diagnostics (POC) in resource-limited settings.

Temperature Sensing Shape Morphing Antenna (ShMoA).

Devices that can morph their functions on demand provide a rich yet unexplored paradigm for the next generation of electronic devices and sensors. For example, an antenna that can morph its shape can be used to adapt communication to different wireless standards or improve wireless signal reception. We utilize temperature-sensitive shape memory alloys (SMA) to realize a shape morphing antenna (ShMoA). In the designed architecture, multiple conjoined shape memory alloy sections form the antenna. The shape morphing of this antenna is achieved through temperature control. Different temperature threshold levels are used for programming the shape. Besides its conventional use for RF applications, ShMoA can serve as a multi-level temperature sensor, analogous to thermoreceptors in an insect antenna. ShMoA essentially combines the function of temperature sensing, embedded computing for detection of threshold crossings, and radio frequency readout, all in the single construct of a shape-morphing antenna (ShMoA) without the need for any battery or peripheral electronics. The ShMoA can be employed as bio-inspired wireless temperature sensing antennae on mobile robotic flies, insects, drones and other robots. It can also be deployed as programmable antennas for multi-standard wireless communication.

Recent progress in electrospun nanomaterials for wearables.

Wearables have garnered significant attention in recent years not only as consumer electronics for entertainment, communications, and commerce but also for real-time continuous health monitoring. This has been spurred by advances in flexible sensors, transistors, energy storage, and harvesting devices to replace the traditional, bulky, and rigid electronic devices. However, engineering smart wearables that can seamlessly integrate with the human body is a daunting task. Some of the key material attributes that are challenging to meet are skin conformability, breathability, and biocompatibility while providing tunability of its mechanical, electrical, and chemical properties. Electrospinning has emerged as a versatile platform that can potentially address these challenges by fabricating nanofibers with tunable properties from a polymer base. In this article, we review advances in wearable electronic devices and systems that are developed using electrospinning. We cover various applications in multiple fields including healthcare, biomedicine, and energy. We review the ability to tune the electrical, physiochemical, and mechanical properties of the nanofibers underlying these applications and illustrate strategies that enable integration of these nanofibers with human skin.

Hard polymeric porous microneedles on stretchable substrate for transdermal drug delivery.

Microneedles offer a convenient transdermal delivery route with potential for long term sustained release of drugs. However current microneedle technologies may not have the mechanical properties for reliable and stable penetration (e.g. hydrogel microneedles). Moreover, it is also challenging to realize microneedle arrays with large size and high flexibility. There is also an inherent upper limit to the amount and kind of drugs that can be loaded in the microneedles. In this paper, we present a new class of polymeric porous microneedles made from biocompatible and photo-curable resin that address these challenges. The microneedles are unique in their ability to load solid drug formulation in concentrated form. We demonstrate the loading and release of solid formulation of anesthetic and non-steroidal anti-inflammatory drugs, namely Lidocaine and Ibuprofen. Paper also demonstrates realization of large area (6 × 20 cm2) flexible and stretchable microneedle patches capable of drug delivery on any body part. Penetration studies were performed in an ex vivo porcine model supplemented through rigorous compression tests to ensure the robustness and rigidity of the microneedles. Detailed release profiles of the microneedle patches were shown in an in vitro skin model. Results show promise for large area transdermal delivery of solid drug formulations using these porous microneedles.

Ingestible pH Sensing Capsule with Thread-Based Electrochemical Sensors.

Existing techniques for diagnosing gastrointestinal disorders in stomach, small and large intestines, and colon depend on biopsy, endoscopy or colonoscopy methods which are invasive, expensive and time-consuming. In fact, such methods also lack the ability to access large parts of the small intestine. In this article, we demonstrate a smart ingestible biosensing capsule that is capable of monitoring pH activity in small and large intestines. pH is a known biomarker for several gastrointestinal disorders such as inflammatory bowel disease. Functionalized threads utilized as pH sensing mechanism are integrated with front-end readout electronics and 3D-printed case. This paper demonstrates a modular sensing system design that alleviates the sensor fabrication difficulties as well as the overall assembly of the ingestible capsule.

Flexible thread-based electrochemical sensors for oxygen monitoring.

Oxygen plays a key role in human physiology and is abnormally modulated in various disease pathologies making its in situ monitoring quite important. Most oxygen sensors are not able to measure oxygen levels deep inside the tissue or have mismatched electrode-tissue interfaces. In this study we developed a flexible thread-based oxygen sensor that combines the unique advantages of minimal invasiveness and superior flexibility offering the possibility for tissue integration. The sensor is featured by a simple and low-cost fabrication approach which allows for measuring the overall oxygen concentration either over a large surface area or locally at any spot in any three-dimensional environment with high spatial accuracy and high sensitivity. The sensor can sensitively detect dissolved oxygen levels within the physiological range of tissue oxygenation. The sensor's performance is insensitive to pH variation from 5.8 to 8.0. The sensor shows good repeatability and stability over a period of one week in phosphate buffered saline. In addition, the signal variation is less than 10% after hundreds of cycles of physical bending. Using a hydrogel-based tissue model the sensor has been shown to probe dissolved oxygen levels at different spatial locations inside a tissue-like environment.

Head motion classification using thread-based sensor and machine learning algorithm.

Human machine interfaces that can track head motion will result in advances in physical rehabilitation, improved augmented reality/virtual reality systems, and aid in the study of human behavior. This paper presents a head position monitoring and classification system using thin flexible strain sensing threads placed on the neck of an individual. A wireless circuit module consisting of impedance readout circuitry and a Bluetooth module records and transmits strain information to a computer. A data processing algorithm for motion recognition provides near real-time quantification of head position. Incoming data is filtered, normalized and divided into data segments. A set of features is extracted from each data segment and employed as input to nine classifiers including Support Vector Machine, Naive Bayes and KNN for position prediction. A testing accuracy of around 92% was achieved for a set of nine head orientations. Results indicate that this human machine interface platform is accurate, flexible, easy to use, and cost effective.

Influence of Hydrogen Bond Donor Identity and Intentional Water Addition on the Properties of Gelatin-Supported Deep Eutectic Solvent Gels.

Deep eutectic solvent (DES) gel electrolytes have recently emerged as promising alternatives to ionic liquid- or water-based gels for "ionic skin" sensor applications. Researchers have also been exploring the effects that varying amounts of water may have on the local hydrogen bonding environment within a few model DES systems. In this study, the physical properties and ionic conductivities of biopolymer (gelatin)-supported gels featuring two established DESs and three DES/water mixture formulations are investigated and compared. The DES/water mixtures are formed by combining choline chloride with one of three organic hydrogen bond donors (HBDs), ethylene glycol, glycerol, or 1,2-propanediol, in a 1:2 molar ratio, together with a controlled amount of water, 25 mol % (approximately 5-6 wt % water). For the same fixed gelatin content (20 wt %), DES/water mixture gel Young's modulus values are found to be tunable based on the organic HBD identity, increasing 6-fold from 7 (1,2-propanediol) to 42 (glycerol) kPa. Furthermore, large differences are observed in the resulting gel properties when water has been intentionally added to well-studied DESs. Coformulation with water is found to increase ethylene glycol-based DES gel toughness, measured via tensile testing, from 23 to 68 kJ/m3 while simultaneously boosting gel room temperature ionic conductivity from 3.3 to 5.2 mS/cm. These results highlight the multiple roles that controlled amounts of water in DES can play within gelatin-supported DES/mixture gel electrolytes, such as influencing gelatin self-assembly and reducing local viscosity to promote facile ion transport.