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.

Highlights: Ultrathin and defect-free graphene ink is prepared through a high-throughput fluid dynamics process, resulting in a high exfoliation yield (53.5%) and a high concentration (47.5 mg mL⁻¹). A screen-printed graphene conductor exhibits a high electrical conductivity of 1.49 × 10⁴ S m⁻¹ and good mechanical flexibility. An electrochemical sodium ion sensor based on graphene ink exhibits an excellent potentiometric sensing performance in a mechanically bent state. Real-time monitoring of sodium ion concentration in sweat is demonstrated. Conductive inks based on graphene materials have received significant attention for the fabrication of a wide range of printed and flexible devices. However, the application of graphene fillers is limited by their restricted mass production and the low concentration of their suspensions. In this study, a highly concentrated and conductive ink based on defect-free graphene was developed by a scalable fluid dynamics process. A high shear exfoliation and mixing process enabled the production of graphene at a high concentration of 47.5 mg mL⁻¹ for graphene ink. The screen-printed graphene conductor exhibits a high electrical conductivity of 1.49 × 10⁴ S m⁻¹ and maintains high conductivity under mechanical bending, compressing, and fatigue tests. Based on the as-prepared graphene ink, a printed electrochemical sodium ion (Na⁺) sensor that shows high potentiometric sensing performance was fabricated. Further, by integrating a wireless electronic module, a prototype Na⁺-sensing watch is demonstrated for the real-time monitoring of the sodium ion concentration in human sweat during the indoor exercise of a volunteer. The scalable and efficient procedure for the preparation of graphene ink presented in this work is very promising for the low-cost, reproducible, and large-scale printing of flexible and wearable electronic devices.

Endonucleases have recently widely used in molecular diagnostics. Here, we report a strategy to exploit the properties of Argonaute (Ago) proteins for molecular diagnostics by introducing an artificial nucleic acid circuit with Ago protein (ANCA) method. The ANCA is designed to perform a continuous autocatalytic reaction through cross-catalytic cleavage of the Ago protein, enabling one-step, amplification-free, and isothermal DNA detection. Using the ANCA method, carbapenemase-producing Klebsiella pneumoniae (CPKP) are successfully detected without DNA extraction and amplification steps. In addition, we demonstrate the detection of carbapenem-resistant bacteria in human urine and blood samples using the method. We also demonstrate the direct identification of CPKP swabbed from surfaces using the ANCA method in conjunction with a three-dimensional nanopillar structure. Finally, the ANCA method is applied to detect CPKP in rectal swab specimens from infected patients, achieving sensitivity and specificity of 100% and 100%, respectively. The developed method can contribute to simple, rapid and accurate diagnosis of CPKP, which can help prevent nosocomial infections.