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As recent developments in noninvasive biosensors spearhead the thrust toward personalized health and fitness monitoring, there is a need for high throughput, cost-effective fabrication of flexible sensing components. Toward this goal, we present roll-to-roll (R2R) gravure printed electrodes that are robust under a range of electrochemical sensing applications. We use inks and electrode morphologies designed for electrochemical and mechanical stability, achieving devices with uniform redox kinetics printed on 150 m flexible substrate rolls. We show that these electrodes can be functionalized into consistently high performing sensors for detecting ions, metabolites, heavy metals, and other small molecules in noninvasively accessed biofluids, including sensors for real-time, in situperspiration monitoring during exercise. This development of robust and versatile R2R gravure printed electrodes represents a key translational step in enabling large-scale, low-cost fabrication of disposable wearable sensors for personalized health monitoring applications.

Homeostasis of ionized calcium in biofluids is critical for human biological functions and organ systems. Measurement of ionized calcium for clinical applications is not easily accessible due to its strict procedures and dependence on pH. pH balance in body fluids greatly affects metabolic reactions and biological transport systems. Here, we demonstrate a wearable electrochemical device for continuous monitoring of ionized calcium and pH of body fluids using a disposable and flexible array of Ca2+and pH sensors that interfaces with a flexible printed circuit board. This platform enables real-time quantitative analysis of these sensing elements in body fluids such as sweat, urine, and tears. Accuracy of Ca2+concentration and pH measured by the wearable sensors is validated through inductively coupled plasma-mass spectrometry technique and a commercial pH meter, respectively. Our results show that the wearable sensors have high repeatability and selectivity to the target ions. Real-time on-body assessment of sweat is also performed, and our results indicate that calcium concentration increases with decreasing pH. This platform can be used in noninvasive continuous analysis of ionized calcium and pH in body fluids for disease diagnosis such as primary hyperparathyroidism and kidney stones.