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  • 1.
    Parrilla, Marc
    et al.
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Chemistry, Applied Physical Chemistry.
    Cuartero, Maria
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Chemistry, Applied Physical Chemistry.
    Crespo, Gaston A.
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Chemistry, Applied Physical Chemistry.
    Wearable potentiometric ion sensors2019In: TrAC. Trends in analytical chemistry, ISSN 0165-9936, E-ISSN 1879-3142, Vol. 110, p. 303-320Article, review/survey (Refereed)
    Abstract [en]

    Wearable potentiometric ion sensors (WPISs) have become an exciting analytical platform that combines chemical, material and electronic efforts to supply physiological information during certain human activities. The real possibility of wearing an analytical device with diverse configurations-sweatband, patches, garments-without disturbing the welfare of the carrier has enabled potentiometric ion sensors both as health quality and sport performance controllers. Recent studies show a large involvement of WPISs in the following of critical biomarkers (timely or continuously), such as sodium, potassium, calcium, magnesium, ammonium and chloride, which are present at relatively high concentrations in sweat (similar to mM levels). Certainly, the non-invasive nature of WPISs and other significant features, e.g., simplicity and cost-effectiveness, have broadened new horizons in relation to applied analytical chemistry. This has been pointed out in the literature over the last decade with the predominance of two analytical outcomes: (i) the improvement of sport performance as a result of continuous detection of ions in sweat (health status of the individual) while decreasing physiological complications (injuries, muscle cramps, fatigue and dehydration) during practice; and (ii) advancements in clinical diagnostics and preventive medicine as a consequence of the monitoring of the health status of patients suffering from any kind of disorder. Beyond the undeniable importance of the integration of WPISs to satisfy current societal needs, the following crucial questions about misleading and missing analytical features need to be answered: To what extent is WPIS technology a reliable analytical tool for the quantification of ions? Is cross-validation the current bottleneck toward further progress? Which are the fundamental steps involving the ion-selective electrode side that would benefit WPIS outcomes? Why is sweat the main (and almost the only) biological fluid to be monitored by WPISs? What is the best sampling strategy to be incorporated into WPIS devices for on-body monitoring of sweat? Which precision limits should be considered to assure a reliable decision-making process? Accordingly, this review focuses on the progression of WPISs from an analytical perspective-merely our vision of the field-within the period between 2010 and 2018. An updated search using specific keywords (wearable, ion, potentiometry, sensor) provided 43 contributions, which are herein highlighted, with a sustainable acceleration over the last three years. Thus, this review describes the current state of WPIS technology, the construction of wearable all-solid-state potentiometric sensors, critical requirements of potentiometric sensors to be fulfilled in a wearable configuration and key features regarding the ideal implementation of WPISs as reliable messengers of physiological information in real scenarios.

  • 2.
    Parrilla, Marc
    et al.
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Chemistry, Applied Physical Chemistry.
    Cuartero, Maria
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Chemistry, Applied Physical Chemistry.
    Sanchez, Sara Padrell
    Karolinska Inst, Dept Clin Sci Intervent & Technol, K 57, SE-14186 Stockholm, Sweden.;Karolinska Univ Sjukhuset, Div Obstet & Gynecol, S-14186 Stockholm, Sweden..
    Rajabi, Mina
    KTH, School of Electrical Engineering and Computer Science (EECS), Micro and Nanosystems.
    Roxhed, Niclas
    KTH, School of Electrical Engineering and Computer Science (EECS), Micro and Nanosystems.
    Niklaus, Frank
    KTH, School of Electrical Engineering and Computer Science (EECS), Micro and Nanosystems.
    Crespo, Gaston A.
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Chemistry, Applied Physical Chemistry.
    Wearable All-Solid-State Potentiometric Microneedle Patch for Intradermal Potassium Detection2019In: Analytical Chemistry, ISSN 0003-2700, E-ISSN 1520-6882, Vol. 91, no 2, p. 1578-1586Article in journal (Refereed)
    Abstract [en]

    A new analytical all-solid-state platform for intradermal potentiometric detection of potassium in interstitial fluid is presented here. Solid microneedles are modified with different coatings and polymeric membranes to prepare both the potassium-selective electrode and reference electrode needed for the potentiometric readout. These microneedle-based electrodes are fixed in an epidermal patch suitable for insertion into the skin. The analytical performances observed for the potentiometric cell (Nernstian slope, limit of detection of 10(-4.9) potassium activity, linear range of 10(-4.2) to 10(-1.1), drift of 0.35 +/- 0.28 mV h(-1)), together with a fast response time, adequate selectivity, and excellent reproducibility and repeatability, are appropriate for potassium analysis in interstitial fluid within both clinical and harmful levels. The potentiometric response is maintained after several insertions into animal skin, confirming the resiliency of the microneedle-based sensor. Ex vivo tests based on the intradermal detection of potassium in chicken and porcine skin demonstrate that the microneedle patch is suitable for monitoring potassium changes inside the skin. In addition, the dimensions of the microneedles modified with the corresponding layers necessary to enhance robustness and provide sensing capabilities (1000 mu m length, 45 degrees tip angle, 15 mu m thickness in the tip, and 435 mu m in the base) agree with the required ranges for a painless insertion into the skin. In vitro cytotoxicity experiments showed that the patch can be used for at least 24 h without any side effect for the skin cells. Overall, the developed concept constitutes important progress in the intradermal analysis of ions related to an electrolyte imbalance in humans, which is relevant for the control of certain types of diseases.

  • 3.
    Parrilla, Marc
    et al.
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Chemistry, Applied Physical Chemistry.
    Ortiz-Gomez, Inmaculada
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Chemistry. Univ Granada, Fac Sci, Dept Analyt Chem, Campus Fuentenueva, E-18071 Granada, Spain..
    Canovas, Rocio
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Chemistry.
    Salinas-Castillo, Alfonso
    Univ Granada, Fac Sci, Dept Analyt Chem, Campus Fuentenueva, E-18071 Granada, Spain..
    Cuartero, Maria
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Chemistry, Applied Physical Chemistry.
    Crespo, Gaston A.
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Chemistry, Applied Physical Chemistry.
    Wearable Potentiometric Ion Patch for On-Body Electrolyte Monitoring in Sweat: Toward a Validation Strategy to Ensure Physiological Relevance2019In: Analytical Chemistry, ISSN 0003-2700, E-ISSN 1520-6882, Vol. 91, no 13, p. 8644-8651Article in journal (Refereed)
    Abstract [en]

    Herein, the reproducibility and a double validation of on-body measurements provided by new wearable potentiometric ion sensors (WPISs) is presented. Sweat collected during sport practice was first analyzed using the developed device, the pH-meter, and ion chromatography (IC) prior to onbody measurements (off-site validation). Subsequently, the accuracy of onbody measurements accomplished by the WPISs was evaluated by comparison with pH-meter readings and IC after collecting sweat (every 10-12.5 min) during sport practice. The developed device contains sensors for pH, Cl-, K+, and Na+ that are embedded in a flexible sampling cell for sweat analysis. The electrode array was fabricated employing MWCNTs (as an ion-to-electron transducer) and stretchable materials that have been exhaustively characterized in terms of analytical performance, presenting Nernstian slopes within the expected physiological range of each ion analyte (Cl-, 10-100 mM; 10-10 mM; and Na+, 10- 100 mM and pH, 4.5-7.5), drift suitable for midterm exercise practice (0.3 +/- 0.2 mV h(-1)), fast response time, adequate selectivity for sweat measurements, and excellent reversibility. Besides that, the designed sampling cell avoids any sweat contamination and evaporation issues while supplying a passive sweat flow encompassing specifically the individual's perspiration. The interpretation of ion concentration profiles may permit the identification of personal dynamic patterns in sweat composition while practicing sport.

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