skip to main content


Title: Highly Sensitive Wearable Sensor Based on (001)‐Orientated TiO 2 for Real‐Time Electrochemical Detection of Dopamine, Tyrosine, and Paracetamol
Abstract

The concentration of dopamine (DA) and tyrosine (Tyr) reflects the condition of patients with Parkinson's disease, whereas moderate paracetamol (PA) can help relieve their pain. Therefore, real‐time measurements of these bioanalytes have important clinical implications for patients with Parkinson's disease. However, previous sensors suffer from either limited sensitivity or complex fabrication and integration processes. This work introduces a simple and cost‐effective method to prepare high‐quality, flexible titanium dioxide (TiO2) thin films with highly reactive (001)‐facets. The as‐fabricated TiO2film supported by a carbon cloth electrode (i.e., TiO2–CC) allows excellent electrochemical specificity and sensitivity to DA (1.390 µA µM−1 cm−2), Tyr (0.126 µA µM−1 cm−2), and PA (0.0841 µA µM−1 cm−2). More importantly, accurate DA concentration in varied pH conditions can be obtained by decoupling them within a single differential pulse voltammetry measurement without additional sensing units. The TiO2–CC electrochemical sensor can be integrated into a smart diaper to detect the trace amount of DA or an integrated skin‐interfaced patch with microfluidic sampling and wireless transmission units for real‐time detection of the sweat Try and PA concentration. The wearable sensor based on TiO2–CC prepared by facile manufacturing methods holds great potential in the daily health monitoring and care of patients with neurological disorders.

 
more » « less
NSF-PAR ID:
10489891
Author(s) / Creator(s):
 ;  ;  ;  ;  ;  ;  ;  ;  
Publisher / Repository:
Wiley Blackwell (John Wiley & Sons)
Date Published:
Journal Name:
Small
ISSN:
1613-6810
Format(s):
Medium: X
Sponsoring Org:
National Science Foundation
More Like this
  1. Abstract

    Hydrogen sulfide (H2S) is a gaseous inflammatory mediator and important signaling molecule for maintaining gastrointestinal (GI) homeostasis. Excess intraluminal H2S in the GI tract has been implicated in inflammatory bowel disease and neurodegenerative disorders; however, the role of H2S in disease pathogenesis and progression is unclear. Herein, an electrochemical gas‐sensing ingestible capsule is developed to enable real‐time, wireless amperometric measurement of H2S in GI conditions. A gold (Au) three‐electrode sensor is modified with a Nafion solid‐polymer electrolyte (Nafion‐Au) to enhance selectivity toward H2S in humid environments. The Nafion‐Au sensor‐integrated capsule shows a linear current response in H2S concentration ranging from 0.21 to 4.5 ppm (R2= 0.954) with a normalized sensitivity of 12.4% ppm−1when evaluated in a benchtop setting. The sensor proves highly selective toward H2S in the presence of known interferent gases, such as hydrogen (H2), with a selectivity ratio of H2S:H2= 1340, as well as toward methane (CH4) and carbon dioxide (CO2). The packaged capsule demonstrates reliable wireless communication through abdominal tissue analogues, comparable to GI dielectric properties. Also, an assessment of sensor drift and threshold‐based notification is investigated, showing potential for in vivo application. Thus, the developed H2S capsule platform provides an analytical tool to uncover the complex biology‐modulating effects of intraluminal H2S.

     
    more » « less
  2. Abstract

    Although increasing efforts have been devoted to the development of non‐invasive wearable electrochemical sweat sensors for monitoring physiological and metabolic information, most of them still suffer from poor stability and specificity over time and fluctuating temperatures. This study reports the design and fabrication of a long‐term stable and highly sensitive flexible electrochemical sensor based on nanocomposite‐modified porous graphene by facile laser treatment for detecting biomarkers such as glucose in sweat. The laser‐reduced and patterned stable conductive nanocomposite on the porous graphene electrode provides the resulting glucose sensor with an excellent sensitivity of 1317.69 µA mm−1cm−2and an ultra‐low limit of detection of 0.079 µm. The sensor can also detect pH and exhibit extraordinary stability to maintain more than 91% sensitivity over 21 days in ambient conditions. Taken together with a temperature sensor based on the same material system, the dual glucose and pH sensor integrated with a flexible microfluidic sweat sampling network further results in accurate continuous on‐body glucose detection calibrated by the simultaneously measured pH and temperature. The low‐cost, highly sensitive, and long‐term stable platform could facilitate the early identification and continuous monitoring of different biomarkers for non‐invasive disease diagnosis and treatment evaluation.

     
    more » « less
  3. Abstract

    Wearable health monitoring has garnered considerable interest from the healthcare industry as an evolutionary alternative to standard practices with the ability to provide rapid, off‐site diagnosis and patient‐monitoring. In particular, sweat‐based wearable biosensors offer a noninvasive route to continuously monitor a variety of biomarkers for a range of physiological conditions. Both the accessibility and wealth of information of sweat make it an ideal target for noninvasive devices that can aid in early diagnosis of disease or to monitor athletic performance. Here, the integration of ammonium (NH4+) and calcium (Ca2+) ion‐selective membranes with a poly(3,4‐ethylenedioxythiophene):poly(styrenesulfonate)‐based (PEDOT:PSS) organic electrochemical transistor (OECT) for multiplexed sensing of NH4+and Ca2+in sweat with high sensitivity and selectivity is reported for the first time. The presented wearable sweat sensor is designed by combining a flexible and stretchable styrene‐ethylene‐butene‐styrene substrate with a laser‐patterned microcapillary channel array for direct sweat acquisition and delivery to the ion‐selective OECT. The resulting dermal sensor exhibits a wide working range between 0.01 × 10−3and 100 × 10−3m, well within the physiological levels of NH4+and Ca2+in sweat. The integrated devices are successfully implemented with both ex situ measurements and on human subjects with real‐time analysis using a wearable sensor assembly.

     
    more » « less
  4. The simple synthesis of a Ni–TiO2nanocomposite supported on Vulcan carbon (XC–72 R) for the electrooxidation reaction of glucose is reported. Four transition metal weight ratios were synthesized and characterized. Cyclic voltammetry studies in 0.1 M NaOH demonstrate that the four metal catalysts can effectively oxidize 1 mM glucose, with the 3:1 (60%) Ni to Ti nanocomposite yielding the highest current. The 60% Ni–TiO2/XC72R catalyst was used to construct an enzyme–less, chronoamperometric sensor for glucose detection in an alkaline medium. Using 50μM aliquots of glucose at a potential of +0.7 V (vs Hg/HgO), the sensor responded rapidly (<3 s), provided a sensitivity of 3300μA mM−1cm−2, detection limits of 144 nM (Signal/Noise = 3), and excellent selectivity and reproducibility. The glucose aliquot concentrations were then increased to 1 mM to mimic physiological blood conditions of 1–20 mM. At a potential of +0.7 V (vs Hg/HgO), the sensor continued to respond rapidly (<1 s), showed a sensitivity of 273.7μA mM−1cm−2, detection limits of 3.13μM (S/N = 3), and excellent selectivity and reproducibility. The catalyst also exhibited an ideal anti–poisoning capability to free chloride ions and negligible signals towards other interfering species.

     
    more » « less
  5. Abstract

    Significant optical absorption in the blue–green spectral range, high intralayer carrier mobility, and band alignment suitable for water splitting suggest tin disulfide (SnS2) as a candidate material for photo‐electrochemical applications. In this work, vertically aligned SnS2nanoflakes are synthesized directly on transparent conductive substrates using a scalable close space sublimation (CSS) method. Detailed characterization by time‐resolved terahertz and time‐resolved photoluminescence spectroscopies reveals a high intrinsic carrier mobility of 330 cm2V−1s−1and photoexcited carrier lifetimes of 1.3 ns in these nanoflakes, resulting in a long vertical diffusion length of ≈1 µm. The highest photo‐electrochemical performance is achieved by growing SnS2nanoflakes with heights that are between this diffusion length and the optical absorption depth of ≈2 µm, which balances the competing requirements of charge transport and light absorption. Moreover, the unique stepped morphology of these CSS‐grown nanoflakes improves photocurrent by exposing multiple edge sites in every nanoflake. The optimized vertical SnS2nanoflake photoanodes produce record photocurrents of 4.5 mA cm−2for oxidation of a sulfite hole scavenger and 2.6 mA cm−2for water oxidation without any hole scavenger, both at 1.23 VRHEin neutral electrolyte under simulated AM1.5G sunlight, and stable photocurrents for iodide oxidation in acidic electrolyte.

     
    more » « less