Highly Stretchable Sensor Based on Fluid Dynamics-Assisted Graphene Inks for Real-Time Monitoring of Sweat.

Graphene inks have recently attracted attention for the development of printed wearable and flexible electronics and sensors not only because of their high conductivity and low cost but also because they are suitable for high-speed printing. Although reliable and scalable printing technologies are well established, further improvement in graphene inks in terms of electrical conductivity, stretchability/flexibility, and mass production is necessary for sensors for real-time monitoring. Herein, highly stretchable and conductive graphene inks were prepared by an efficient and scalable fluid dynamics-assisted exfoliation of graphite and a mixing process with elastomeric Ecoflex. After printing inks onto textile substrates, the serpentine-patterned conductors exhibited high conductivity and stable resistance even under a mechanically stretched state (a strain of 150%). Electrochemical sensors that detect sodium ions were fabricated on this conducting platform. These sensors indicated high potentiometric sensing ability under different mechanical deformations. To demonstrate the on-body performance of the developed sensors, real-time monitoring of sodium-ion concentration in the sweat of a human subject was carried out during an indoor stationary cycling exercise.

Highly self-healable and flexible cable-type pH sensors for real-time monitoring of human fluids.

Development of sensing technology with wearable chemical sensors is realizing non-invasive, real-time monitoring healthcare and disease diagnostics. The advanced sensor devices should be compact and portable for use in limited space, easy to wear on human body, and low-cost for personalized healthcare markets. Here, we report a highly sensitive, flexible, and autonomously self-healable pH sensor cable developed by weaving together two carbon fiber thread electrodes coated with mechanically robust self-healing polymers. The pH sensor cable showed excellent electrochemical performances of sensitivity, repeatability, and durability. Spontaneous and autonomous sensor healing efficiency of the pH sensor cable was demonstrated by measuring sensitivity during four cycles of cutting and healing process. The pH sensor cable could measure pH in small volumes of real human fluid samples, including urine, saliva, and sweat, and the results were similar to those of a commercial pH meter. Taken together, successful real-time pH monitoring for human sweat was demonstrated by fabricating a wearable sensing system in which the pH sensor cable was knitted into a headband integrated with wireless electronics.

Preparation of ultrathin defect-free graphene sheets from graphite via fluidic delamination for solid-contact ion-to-electron transducers in potentiometric sensors.

In this study, ultrathin and defect-free graphene (Gr) sheets were prepared through a fluid dynamics-induced shear exfoliation method using graphite. The high hydrophobicity and surface area of Gr make it attractive as a solid-contact ion-to-electron transducer for potentiometric K+ sensors, in which the electrodes are fabricated through a screen-printing process. The electrochemical characterization demonstrates that Gr solid contact results in a high double-layer capacitance, potential stability, and strong resistance against water layer, gases, and light. The Gr-based K+ sensors showed a Nernstian slope of 53.53 mV/log[K+] within a linear concentration range of 10-1-10-4 M, a low detection limit of 10-4.28 M, a fast response time of ~8 s, good repeatability, and excellent long-term stability. Moreover, the Gr-based K+ sensors provided accurate ion concentrations in actual samples of human sweat and sports drinks.

Extremely Fast Self-Healable Bio-Based Supramolecular Polymer for Wearable Real-Time Sweat-Monitoring Sensor.

Sensors with autonomous self-healing properties offer enhanced durability, reliability, and stability. Although numerous self-healing polymers have been attempted, achieving sensors with fast and reversible recovery under ambient conditions with high mechanical toughness remains challenging. Here, a highly sensitive wearable sensor made of a robust bio-based supramolecular polymer that is capable of self-healing via hydrogen bonding is presented. The integration of carbon fiber thread into a self-healing polymer matrix provides a new toolset that can easily be knitted into textile items to fabricate wearable sensors that show impressive self-healing efficiency (>97.0%) after 30 s at room temperature for K+/Na+ sensing. The wearable sweat-sensor system-coupled with a wireless electronic circuit board capable of transferring data to a smart phone-successfully monitors electrolyte ions in human perspiration noninvasively in real time, even in the healed state during indoor exercise. Our smart sensors represent an important advance toward futuristic personalized healthcare applications.

Potentiometric performance of flexible pH sensor based on polyaniline nanofiber arrays.

We report potentiometric performance of a polyaniline nanofiber array-based pH sensor fabricated by combining a dilute chemical polymerization and low-cost and simple screen printing process. The pH sensor had a two-electrode configuration consisting of polyaniline nanofiber array sensing electrode and Ag/AgCl reference electrode. Measurement of electromotive force between sensing and reference electrodes provided various electrochemical properties of pH sensors. The pH sensor show excellent sensor performances of sensitivity of 62.4 mV/pH, repeatability of 97.9% retention, response time of 12.8 s, and durability of 3.0 mV/h. The pH sensor could also measure pH changes as the milk is spoiled, which is similar to those of a commercial pH meter. The pH sensors were highly flexible, and thus can measure the fruit decay on the curved surface of an apple. This flexible and miniature pH sensor opens new opportunities for monitoring of water, product process, human health, and chemical (or bio) reactions even using small volumes of samples.

Fabrication of newspaper-based potentiometric platforms for flexible and disposable ion sensors.

Paper-based materials have attracted a great deal of attention in sensor applications because they are readily available, biodegradable, inexpensive, and mechanically flexible. Although paper-based sensors have been developed, but important obstacles remian, which include the retention of chemical and mechanical stabilities when paper is wetted. Herein, we develop a simple and scalable process for fabrication of newspaper-based platforms by coating of parylene C and patterning of metal layers. As-prepared parylene C-coated newspaper (PC-paper) provides low-cost, disposable, and mechanically and chemically stable electrochemical platforms for the development of potentiometric ion sensors for the detection of electrolyte cations, such as, H+ and K+. The pH and K+ sensors produced show near ideal Nernstian sensitivity, good repeatability, good ion selectivity, and low potential drift. These disposable, flexible ion sensors based on PC-paper platforms could provide new opportunities for the development of point-of-care testing sensors, for diagnostics, healthcare, and environment testing.

High performance flexible pH sensor based on polyaniline nanopillar array electrode.

Flexible pH sensor technologies have attracted a great deal of attention in many applications, such as, wearable health care devices and monitors for chemical and biological processes. Here, we fabricated flexible and thin pH sensors using a two electrode configuration comprised of a polyaniline nanopillar (PAN) array working electrode and an Ag/AgCl reference electrode. In order to provide nanostructure, soft lithography using a polymeric blend was employed to create a flexible nanopillar backbone film. Polyaniline-sensing materials were deposited on a patterned-nanopillar array by electrochemical deposition. The pH sensors produced exhibited a near-Nernstian response (∼60.3mV/pH), which was maintained in a bent state. In addition, pH sensors showed other excellent sensor performances in terms of response time, reversibility, repeatability, selectivity, and stability.

Fabrication of Flexible, Redoxable, and Conductive Nanopillar Arrays with Enhanced Electrochemical Performance.

Highly ordered and flexible nanopillar arrays have received considerable interest for many applications of electrochemical devices because of their unique mechanical and structural properties. Here, we report on highly ordered polyoxometalate (POM)-doped polypyrrole (Ppy) nanopillar arrays produced by soft lithography and subsequent electrodeposition. As-prepared POM-Ppy/nanopillar films show superior electrochemical performances for pseudocapacitor and enzymeless electrochemical sensor applications and good mechanical properties, which allowed them to be easily bent and twisted. Regarding electrochemical characteristics for pseudocapacitive electrodes, the POM-Ppy/nanopillar electrodes are capable of delivering high areal capacitance of 77.0 mF cm(-2), high rate performance, and good cycle life of ∼100% retention over 3500 cycles even when bent. Moreover, the study suggests that the POM-Ppy/nanopillar electrodes have an excellent electrocatalytic activity toward hydrogen.

Nanopillar films with polyoxometalate-doped polyaniline for electrochemical detection of hydrogen peroxide.

Design and fabrication of electrodes is key in the development of electrochemical sensors with superior electrochemical performances. Herein, an enzymeless electrochemical sensor is developed for detection of hydrogen peroxide based on the use of highly ordered polyoxometalate (POM)-doped polyaniline (PANI) nanopillar films. The electrodeposition technique enables the entrapment of POMs into PANI during electropolymerization to produce thin coatings of POM-PANI. Electrochemical investigations of the POM-PANI/nanopillar electrode showed well-defined multiple pairs of redox peaks and rapid electron transfer. The nanopillar structure facilitated the diffusion of the electrolyte and thus, enhanced the redox reaction. In particular, the POM-PANI/nanopillar electrode was incorporated into a flow injection biosensor and it demonstrates its electrocatalytic activity to detect hydrogen peroxide with high sensitivity, rapid response time, and low detection limit.