Life-Saving Threads: Advances in Textile-Based Analytical Devices

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Life-saving threads; advances in textile-based analytical devices Syamak Farajikhah, Joan Marc Cabot, Peter C. Innis, Brett Paull, and Gordon G. Wallace ACS Comb. Sci., Just Accepted Manuscript • DOI: 10.1021/acscombsci.8b00126 • Publication Date (Web): 14 Jan 2019 Downloaded from http://pubs.acs.org on January 15, 2019

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ACS Combinatorial Science

Life-saving threads; advances in textile-based analytical devices Syamak Farajikhah†, Joan M. Cabot‡, Peter C. Innis†,§,*, Brett Paull‡, Gordon Wallace†,§ †ARC

Centre of Excellence in Electromaterials Science (ACES), AIIM Facility, Innovation

campus, University of Wollongong NSW 2500, Australia ‡Australian

Centre for Research on Separation Science (ACROSS) and ARC Centre of

Excellence for Electromaterials Science (ACES), School of Natural Sciences, Faculty of Chemistry, University of Tasmania, TAS 7005, Australia §

Australian National Fabrication Facility – Materials Node, Innovation campus, University

of Wollongong NSW 2522, Australia. KEYWORDS: Fibre, textile, microfluidic, electrophoretic, separation

TABLE OF CONTENTS: ABSTRACT...............................................................................................................................2 INTRODUCTION......................................................................................................................2 FLOW CONTROL MECHANISMS IN μTADs.......................................................................4 Passive flow control mechanisms in μTADs .........................................................................7 Active flow control mechanisms in μTADs.........................................................................10 APPLICATIONS .....................................................................................................................12 EMERGING DIRECTIONS AND FUTURE TRENDS .........................................................23

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ABSTRACT

Novel approaches that incorporate electrofluidic and microfluidic technologies are reviewed to illustrate the translation of traditional enclosed structures into open and accessible textile based platforms. Through the utilisation of on-fibre and on-textile micro-fluidics, it is possible to invert the typical enclosed capillary column or microfluidic “chip” platform, to achieve surface accessible efficient separations and fluid handling, whilst maintaining a microfluidic environment. The open fibre/textile based fluidics approach immediately provides new possibilities to interrogate, manipulate, redirect, extract, characterise and quantify solutes and target species at any point in time during such processes as on-fibre electrodriven separations. This approach is revolutionary in its simplicity, and provides many potential advantages not otherwise afforded by the more traditional enclosed platforms.

INTRODUCTION

The spread of infectious diseases as well as acute debilitating illnesses, such as cancer, puts at risk the lives of millions of people around the world. As a consequence, there is an evergrowing need for development of low cost, rapid, portable and accurate diagnostic devices. Early detection and accurate diagnostics contributes significantly to prevention and increasing survivability rates, improved treatment outcomes, and ultimately reduced financial impacts 1– 7.

Through advances in detection techniques, public health has been greatly improved in recent

decades, however many of these technologies are unaffordable for developing countries. People in developing countries often unable to access new diagnostic technologies due to poverty and lack of sufficient infrastructure

6,8.

In response to this need, the World Health

Organization has prioritised the development of targeted “ASSURED” diagnostic devices that are not only affordable but sensitive, specific, user-friendly, rapid and robust, equipment free 2 ACS Paragon Plus Environment

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and deliverable to end user 6,8–10. The emergence of microfluidic technologies has had a great impact on diagnostics and public health. Microfluidic devices have a number of general advantageous characteristics, which can include the ability to process microscale solution volumes, rapid response rates, sample-in answer-out technology, simplicity, rapid prototyping and low-cost, and so will clearly play significant part in the development of next generation diagnostic technology 2,7,8,11. Portable and inexpensive microfluidic devices have attracted a lot of attention since they can potentially replace large expensive laboratory equipment and can provide in-situ, at-site and ‘at-person’ results. This exciting area of research has many potential applications in the development of diagnostic devices, including the integration of sensors offering the potential to provide real-time data on the interaction and exposure of the wearer to his/her environment, plus significant opportunities for personal health monitoring. Paper, textiles and more recently threads and fabrics have been demonstrated to have significant potential in providing affordable healthcare and environmental monitoring in microfluidic applications. Consequently, there has been an extensive interest in the development of minimally invasive, accurate, durable, user-friendly, and low cost diagnostic platforms12–21. Paper has been used as a substrate in analytical chemistries since early 1800s. Recently, its unique characteristics, such as power-free fluid transport via capillary action 6,22–24, as well as its flexibility, low cost, disposability and the ability to simply functionalize its surface chemistry makes this substrate highly appealing 22,23,25. Microfluidic paper analytical devices (µPAD) can be readily patterned and surface functionalized using inkjet, wax or screen printing approaches making µPAD’s affordable, equipment free and readable with naked eye. Significantly paper devices can be stable in many different environments and capable of capability of analysing multiple analytes using a single device 6,10,23,25. Essential to any µPAD is the need to define hydrophilic and hydrophobic regions on the paper substrate to create 3 ACS Paragon Plus Environment


channels that may rely on delicate and time consuming patterning processes12–14,19,20. Paper also has other limitations such as low mechanical strength when wet and low efficiency of sample delivery due to loss of the solute out of the defined surface channels 26,27. Significantly, the developments in the µPAD approach are translatable to the emergent thread based technologies. An analogous concept to µPAD which is based upon textile threads has been reported by Li et al. 13 and Reches et al. such as flexibility,

12

in 2010. Threads benefit from some outstanding characteristics

high mechanical strength when wet, reusability, disposability,

independence of external power for fluid movement (due to capillary channels between fibres), ease of functionalization and low cost. Unlike µPADs, threads do not need hydrophobic barriers and can be easily converted into 3D structures or be integrated into wearable materials by traditional techniques such as knitting, weaving or sewing. These advantages make them an excellent candidate for microfluidic textile analytical devices (µTAD) 12,13,16,26–28; however, the uniformity of fluid movement in these may also influenced as a result of structural anisotropy resulting from the method of assembly in the textile architecture. Since the first demonstration of the µTAD approach, there has been a significant trend in utilising and studying the effect of different yarns and fabrics to form efficient µTAD structures and applications of these.

FLOW CONTROL MECHANISMS IN μTADs

Fluid flow in yarns and threads arise from wicking processes as a result of capillary forces generated within the gaps between directionally aligned fibres. This capillary action subsequently drives the fluid along the thread. The presence of waxes such as those composed of long fatty acid chains found on some natural fibres like cotton as well as contamination on synthetic fibres such as polyester have been observed to interfere with wicking in threads. The ability to enhance the wettability of yarns by surface modification and removal of waxes and/or 4 ACS Paragon Plus Environment

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contamination to increase in wicking by capillary action within a textile structure has also received significant attention12,13,28–31. Wicking properties of both natural and synthetic fibres can be improved by performing specific surface treatments to change their surface chemistry. Natural fibres like cotton, silk and wool are usually covered with a wax that contains fatty acid chains which may hinder or even stop liquid movement along threads (or fabrics). Plasma treatment and scouring in NaOH or Na2CO3 are common methods that have been used to remove waxes and improve wicking properties of natural fibres. Plasma treatment has also been widely used to enhance wicking properties of cotton fibres12,13,31–37, where the plasma treatment oxidizes the cotton surface and removes the wax; however, the plasma treatment process itself is typically non-permanent and studies to improve its durability has not been extensively explored. X-ray photoelectron spectroscopy (XPS) shows an increase in the surface concentration of oxygen, due to the generation of O-C-O, C=O, O-C=O and C-O on cotton, increasing the surface polarity which then leads to an improvement of wicking properties in cotton fibres13,31,36,37. Jeon et al.38 have also used plasma surface treatment to increase the wettability of wool fibres by degumming fatty acids on its surface where they observed that wool had different flowrates when treated with different plasma gases (O2, N2 and Ar) providing a degree of tunability that enabled flow control in micro-mixing devices. Alternatively, the

wettability of natural fibres can be

improved by boiling them14 or scouring them in NaOH or Na2CO329,39–49. NaOH and Na2CO3 is reported to attack aliphatic chains of the wax on the surface of cotton fibres, removing the wax and exposing the underlying cellulose structure which has negative charge and abundant hydroxyl (-OH) group functionality. Treatment with NaOH also increases O/C ratio which generally makes the fibre surface more hydrophilic29,42,45,46,49. The effect of surface treatment upon the wicking properties of cotton and wool fibres is shown in Figure 1.



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Figure 1. Improvement in wicking properties of yarns. (A) Cotton treated with plasma treatment32 and (B) Wool treated with I. Oxygen and II. Argon plasma. Pristine wool fibre and fibres treated for 0, 15, 30, 45 and 60 min, respectively from upside38 Plasma surface treatment has also been widely used by different groups to increase surface wettability and improve liquid movement of thread-based microfluidic devices made from polyester. This treatment increases surface polarity and removes surface contamination on the thread12,18,30,50–52. Furthermore, as shown in Table 1, Reches et al. demonstrated that plasma treatment significantly increases the wicking rate of different threads12.

Table 1. Increase in wicking rate after plasma treatment for different types of threads12 Thread

Wicking rate before treatment (cm/s)

Wicking rate after treatment (cm/s)

Rayon

0.29 ± 0.06

1.01 ± 0.69

Hemp

0.02 ± 0.01

0.55 ± 0.55

Nylon

0.03 ± 0.00

0.04 ± 0.01

Cotton

0.23 ± 0.04

1.89 ± 0.52

Polyester

0.13 ± 0.03

1.98 ± 0.79

Wool

Did not wick

2.20 ± 0.40

Did not wick

2.11 ± 0.30

Did not wick

1.91 ± 0.42

50% Cotton, 50% Acrylic Acrylic


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Natural silk

Did not wick

0.60 ± 0.21

In addition to research on the enhancement of the wettability of threads for microfluidics, others have suggested and utilised different mechanisms for flow control in μTADs.

Passive flow control mechanisms in μTADs

Fabricating μTADs have been demonstrated in several ways. In the simplest form hydrophilic threads are utilised to provide predefined paths for liquid movement. Initially, Reches et al. demonstrated different designs for thread-based microfluidics, such as cotton threads that were sewn through a hydrophobic substrate to incorporate an assayable zone into a bandage Figure 2A12. Using the same concept, other research groups have introduced the development of 3D thread-based microfluidic device by sewing hydrophilic threads into other substrates13,39. More sophisticated functions utilizing threads in microfluidic devices which expands upon the simple wicking approach have also been investigated. Li and co-workers have demonstrated the potential for not only fluid transport but also fibre based mixing by utilizing intertwined threads, Figure 2B13. In a similar approach, Safavieh et al. 32 employed a combination of knots with different topologies to provide control over mixing and splitting of the fluid in thread-based microfluidic devices, Figure 2C. Here they noted that varying the knot topology can change the fluid mixing ratio through changing the flow resistance in µTADs. More sophisticated methods of passive flow control in threads have been demonstrated by Ballerini et al37 where combinations of knots and glue, used to block wicking in parts of the thread, have been utilized to manipulate fluid movement. They demonstrated a range of threadbased operations including binary on/off style switches, fluid micro-selectors by sliding threads across blocked to unblocked regions, as well as micro-mixers as examples of the potential functions that can be utilized for designing complex yet low-cost µTADs. 7 ACS Paragon Plus Environment


While threads have shown promising results for μTAD applications, they commonly need to be suspended in the air or sewn onto or into a hydrophobic substrate. This approach results in a one dimensional fluid movement confined within the strand of a thread, and consequently limits scalability and the practicality of using thread-based microfluidics in wearable devices for applications such as point-of-care (POC) diagnostics. Fabric-based microfluidic devices, in contrast, are two dimensional in nature and provide a greater sampling zone, allowing a larger geometric area for the solute interaction and detection. However, due to the structural complexity of a fabric fluid movement within it maybe be far from uniform. Rather than sewing hydrophilic threads on a hydrophobic substrate, textile structures have the inherent ability to be fabricated with specific hydrophilic/hydrophobic contrast regions to provide a path for fluid movement. Bhandari et al. used hydrophilic and hydrophobic types of silk threads in a fabric to make a µTAD (Figure 2D)14 . Owen and co-workers have also demonstrated flow control by systematic changes in the placement of hydrophilic and hydrophobic threads within a fabric design53. In another work, Vatansever et al. used hydrophobic polypropylene and hydrophilic poly(ethylene terephthalate) yarns to create µTADs54. In a simpler approach, the introduction of hydrophilic/hydrophobic fluid paths within a textile structure other techniques including wax printing29,42,43,45,55–57 and photolithography have been utilized to create 2D and 3D µTADs with more complex structures. For instance, Liu et al. developed a µTAD using wax and carbon ink screen printing on a hydrophilic cotton substrate58,59. Baysal and co-workers have also developed µTADs using photolithography technique where they used a hydrophilic non-woven fabric as a base structure with physical barriers being incorporated into the structure using a hydrophobic photo-resist polymer51,60 (Figure 2F).


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While fluid moves in µTADs due to capillary wicking, the flow rate achievable dependent upon several factors such as surface functional groups, thread and fabrics internal structures and waxes or impurities on textile threads and fabrics. This can be further enhanced by gravityassisted fluid movement which has been used by Agustini et al. to achieve higher fluid flow rates in µTADs27,61 (Figure 2E). However, fluid movement due to simple wicking or gravity cannot really be described as precise or controllable, hence using active flow control mechanisms (by utilising an external force) have been investigated.

Figure 2. (A) array of cotton threads sewn through a bandage12, (B) Fluid mixing by twisting threads. The top and the middle threads that transport cyan and yellow liquids are twisted and sleeved inside a heat shrink tube; the bottom thread that transports magenta liquid is not twisted with the other two threads and passes through the mixing zone from outside of the heat shrink tube13, (c) A web made of yarns and knots operating as a serial dilutor32, (D) A fabric chip comprising hydrophilic (white) and hydrophobic (gold) silk fibres, a green die 9 ACS Paragon Plus Environment


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was deposited and spread on one of hydrophilic parts14, (E) Gravity-assisted fluid movement in μTADs62 and (F) Schematic of μTAD fabrication using photolithography technique51

Active flow control mechanisms in μTADs

Although wicking is a simple and effective method for the movement of liquids, thereby potentially eliminating the need for an external pump to move fluids in μTAD structures, several research groups have adopted a complementary approach that exploits the control of fluids and solutes using electroosmosis (applied potential). Over past three decades, three common capillary based electrophoretic techniques, namely capillary zone electrophoresis (CZE), isotachophoresis (ITP) and capillary electrochromotography (CEC), have been developed as powerful separation methods for charged solutes. These techniques have demonstrated utility for the separation of inorganic and organic ions as well as charged biomolecules of various sizes, up to and including proteins. Electrophoretic based separation techniques, including CZE, ITP and CEC, have been demonstrated to achieve high efficiency and outstanding selectivity that is well beyond what is achievable with current standard liquid chromatographic methods. However, the small inner diameters of the capillaries used, as well as the very limited sample loading capacity, hinders post-capillary detection in each of these techniques. A fundamental disadvantage of capillary based separation is that it is not feasible to access to the solute within the capillary during the actual separation process, where the detection of separated solutes only occurs at a single point within the capillary column, or indeed at the exit of the capillary63,64. The utilisation of fibre, thread or textile based substrates instead of capillaries can potentially eliminate this fundamental disadvantage.

The

Lin

research group has carried out electrophoretic separation on μTADs18,20,30 (Figure 3A). In these devices polyester threads were utilised for the electrophoresis separation and electrochemical 10 ACS Paragon Plus Environment

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detection of mixed ion samples30, BUN18 and glucose20 in whole human blood by applying 300-500 V cm-1 using a buffer solution of 1.0 mM of MES (2-(N-morpholino) ethanesulfonic acid) at pH 5. Narahari et al. developed a scalable fabric platform made of cotton fabric, to hold large volumes of an aqueous buffer, with a nylon- or polyester-based fabric as a separation substrate. The textile device was demonstrated to be capable of electrophoretic separation of small molecules and protein solutes using an applied potential of 35V cm-1 with glycine−NaOH electrolyte at pH 8.5819 (Figure 3B). Recently, more complex electrophoretic separation and selective movement of solutes in a branched μTAD were demonstrated by Cabot et al65 where they demonstrated electrophoretic separation of fluorescein and rhodamine B dyes solute using nylon as a thread substrate, while applying 200 V cm-1 in using 2.5 mM Tris/CHES buffer at pH 8.5 (Figure 3C). Recently, Ramesan and co-workers have proposed that surface acoustic wave can also be used as an external power source to precisely move fluid in μTADs66. In this approach they demonstrated tunable fluid movement by utilising surface acoustic wave in a network of cotton threads. In the approach they also demonstrated the serial dilution of two different synthetic food dyes in thread network embedded in a transparent hydrogel (Figure 3D).



Figure 3. (A) A schematic showing the experimental setup for the electrophoretic separation on threads67, (B) Dye migration and separation in prototype devices. Anionic Yellow deposited at the start position migrates the fabric strip and toward (applied field= 35 V cm-1 in 1× glycine−NaOH)19, (C) Microscopy images of controlled protein delivery by electrophoresis on a nylon thread (scale bars 2 mm)65 and (D)Time series images showing transport and mixing of two coloured solutions, yellow and blue, due to surface acoustic wave applied at the point α66. APPLICATIONS

A range of applications have been reported utilising simple fluid wicking through to more complicated microfluidic textile-based separation platforms. Both threads and fabrics have been applied to a areas such as bacteria isolation and quantification65, chemotaxis studies for cell culture systems66, immunoassay36, blood typing50, chemical synthesis68, bioanalysis69, and the determination of nucleic acids48, protein48, glucose61, drugs27 , small ions30 and metals57. These applications are also subsequently dependent upon the ability to interrogate and detect the solute of interest at the surface of the fibre, yarn or textile structure. Since different 12 ACS Paragon Plus Environment

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platforms, techniques, analyte and conditions have been used, it is difficult to make a meaningful comparison between the varied approaches. However, due to the design flexibility of fabrics, which facilitates easily incorporation of different threads and electrodes within the substrate, the µTADs textile approach has clear advantages.

Despite its relatively low sensitivity detection, colorimetric has been one of the most utilized due to its simplicity and robustness. For instance, different research groups have performed colorimetric detection of glucose12,49,70, pH71 or proteins55 as reliable and cost-effective methods utilising μTADs. Bhandari et al. used a patterned silk fabric to make a µTAD for use in an immunoassay for colourimetric detection of Rabbit IgG utilising silk thread treated with gold nanoparticles conjugated with Goat Anti-Rabbit IgG (Figure 4A)

14.

Baysal and co-

workers have also developed flexible and disposable µTADs utilising photolithography techniques on Evolon® (polyester/nylon) nonwoven substrates. They demonstrated semiquantitative colourimetric detection of the lactate level in simulated sweat solution suggesting a wearable sensor to monitor athlete’s physical status during exercise by functionalising the detection reservoir using lactate oxidase and peroxidase enzymes51. They further demonstrated the biosensor for colourimetric detection of H2O2 using horseradish peroxidase enzyme and 2,2’-azino-bis(3-ethylbenzthiazoline-6-sulfonic acid) and diammonium salt functionalised reservoirs60. Wu et al. also developed a µTAD utilising photolithography on cotton fabrics to perform colorimetric assays of glucose and bovine serum albumin in artificial urine samples using potassium iodide, trehalose and glucose oxidase–horseradish peroxidase reagents for functionalisation of detection reserviors49. Curto and co-workers have also demonstrated a wearable, flexible and electronic-free µTADs for real-time monitoring of sweat pH (Figure 4B). In this study, a nonwoven textile was used to drive sweat from the sensing area through the channels filled with ionogel/dye mixtures. The combination of colours of different channels 13 ACS Paragon Plus Environment


at a particular pH then formed a particular colour pattern detectable through standard image processing and analysis techniques71. In other research, Vatansever et al. have demonstrated pH-selective fluid movement on μTADs54 (Figure 4C). They locally modified the surface of polyester part in a polyester/polypropylene fabric with an epoxide-containing polymer followed by grafting patterns of poly(acrylic acid) and poly(2-vinyl pyridine) as different pHsensitive polymers. They then demonstrated that liquid transport in the modified fabric is defined by pH-response of the grafted polymers. Recently, Sateanchok et al. developed a costeffective method for colorimetric detection of antioxidant on a device composed of cotton threads for sample delivery and functionalized papers immobilized with reagents. The contact point of thread and paper serves as a reactor and colourimetric detection can be made using a mobile phone camera. Assays for total phenolic content and antioxidant capacity using FolinCiocalteu and DPPH reagents, respectively, were demonstrated using the proposed μTAD72. Choi et al. also reported using polysiloxanes in thread-based microfluidics to tune the fluid movement through the thread. Then they introduced a μTAD with manipulated fluid flow to calorimetrically detect the concentration of Salmonella enterica serotype Enteritidis in phosphate buffered saline, spiked milk, juice and lettuce employing cotton threads functionalized with gold nanoparticle-anti-S. Enteritidis mouse monoclona conjugates73.


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Figure 4. (A) Direct immunoassay on the fabric chip. The upper part is a cut strip before testing. Test and control lines are labeled as T and C14, (B) wearable micro-fluidic system for monitoring sweat pH71 and (C) Selective fluid transport by using pH sensitive μTAD54. A number of approaches have been used to increase the sensitivity of the detection methods in µTADs. Some examples include the use of surface functionalised threads or surfaces with bound and functionalised nanoparticles47, patterned electrodes74, electrophoretic separations18 as well as other detection systems such as electrochemical detection61,67, SERS75, fluorescence65 or electrochemiluminescence58. Metallic electrodes and metal-coated fibres have been incorporated into the textile substrates to develop fabric-based electrophoretic platforms for protein separation19. Alternatively, Robinson et al. treated fabric samples with silver nanoparticles (AgNPs) to develop a low cost Surface-enhanced Raman scattering (SERS) wearable sensors for monitoring biomarkers or environmental pollutants75. Recently, the Marcolino Junior research group developed a cost effective and non-invasive method for determination of glucose level by measuring glucose level in tear by carrying out microflow injection analysis (μFIA) on an integrated µTAD 15 ACS Paragon Plus Environment


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composed of a simple poly(toluidine blue O)-glucose oxidase (GOx) amperometric biosensor with low cost cotton threads61 (Figure 5A). They also combined electrochemical biosensors and threads to detect phenol in tap water62. A range of 2D and 3D µTADs to perform colorimetric bioassays for qualitative measurements or using in combination with electrochemical detections have been demonstrated29,42,43,45,55–57. Liu et al. developed µTADs using wax and carbon ink screen printing on cotton fabrics58 and threads59for wireless electrochemiluminescence providing improved sensitivity and selectivity for the detection of H2O2 and tri-n-propylamine (TPA). Recently, Agustini and co-workers also reported a costeffective and green method for solvent-free chromatographic separation of ascorbic acid (AA) and dopamine (DA) on thread-based microfluidics based on an ion exchange mechanism carrying out simultaneous electrochemical detection of AA and DA at a gold sputter coated thread76. The Lin research group has reported a thread-based microfluidic system for electrophoretic separation and subsequent electrochemical detection of inorganic ions samples such as Cl-, BrI- 30 and blood urea nitrogen (BUN) in whole blood 18. BUN was detected by the incorporation of an enzyme-doped thread to direct electrochemical detection of BUN and glucose in serum 20

(Figure 5B). Narahari et al. has also demonstrated a µTAD for separation of human albumin

and human IgG19 (Figure 5C). Recently, Cabot et al. demonstrated the selective movement of proteins in branching structures and fluorescent dye separations on µTADs

utilizing

electrophoresis technique65. Additionally, they demonstrated the use of joining nylon, silk and cotton, via simple knotting, to create a unique ability to physically concentrate fluorescent dyes within different locations by chromatographic interaction. An application of this approach was demonstrated by trapping and detecting bacteria cells from urine as a potential diagnostic platform for urinary tract infection, proving the cell survival after the on-fibre electrophoretic concentration (Figure 5D). 16 ACS Paragon Plus Environment

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Banerjee and co-workers demonstrated other applications for µTADs by synthesizing ferric hydroxide and 2,4-dichloro-N-(2-morpholinoethyl) benzamide in thread reactors, as well as using threads as microchannel for chemical sensing68. A summary of the reported µTAD applications to date are shown in Table 2. Reports are organised based on textile structures, methods of making path for fluid movement, fluid movement mechanisms and finally proposed applications for μTADs.

Figure 5. (A) Glucose determination using µFIA on an integrated biosensor and µTAD61, (B) Experimental setup for the developed thread-based capillary electrophoresis-electrochemical detection system to detect directly the BUN and glucose in serum20, (C) quantitative measurement of electrophoretic focusing of bovine albumin conjugated to Naphthol Blue (Blue BA) electromigrated on a polyester fabric strip19 and (D) fluorescent microscopy photographs for electrophoresis trapping of stained bacterial cells for determination of urinary tract infection in urine sample65.


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Table 2. Applications reported for textile-based microfluidic devices Textile structure

Method of making fluid path

Fluid movement mechanism

Application Design of the thread-based devices incorporating pins as electrodes77

Thread

Introducing functionalized thread substrates as disposable, low-cost-per-test diagnostics, for routine SERS spectroscopy34 Calorimetrically detecting of 𝑁𝑂2― to show the potential of producing low-cost portable diagnostics13 A new type of manufacturing process for the development of particle-like arrays for a multiplexed bioassay platform using individually functionalized thread strands was introduced36 Electrochemical sensing of physical and chemical markers both In vivo and In vitro78

Nil

Wicking

Blood plasma separation41 Detection of protein, nitrite and ketones and glucose in artificial urine. And alkaline phosphatase in artificial blood plasma12 Visual detection of lung cancer related biomarker, i.e. human ferritin antigen using carbon nanotubes reporters79 Electrochemical detection of human ferritin using gold nanorod reporters80 Room temperature DNA detection device44 Human ferritin detection47 A novel enhanced dry-reagent cotton thread device for Squamous cell carcinoma antigen detection based on two kinds of gold nanoparticles and a novel room temperature DNA detection device by using adenosine based molecular beacon probe were introduced48


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Highly sensitive detection of human hemoglobin81 Colorimetric assessment of acetylcholinesterase activity82 ABO and Rh/D blood typing50 Blood typing52 Effect of different plasma treatments and treatment times on wettability of wool fibres. A simple microfluidic device was designed to do micro-mixing38 Creating patterns on the Poly(methyl methacrylate) chip with gold electrodes and integrated into polymer-based microfluidic channels to create functionalized microfluidic systems69 Detection of three target molecules in serum was performed to demonstrate a multiplexed assay as well as singleplex assay33 Describes a semiquantitative method for analytical detection by measuring the length of colour change on indicator treated threads using a ruler31 The effect of the surface morphologies of silk and cotton fibers on the separation properties for the application of blood typing based on the principal of chromatographic elution35 Cost-effective assays for antioxidant with a mobile phone detector72 Colorimetric detection of Salmonella enterica serotype Enteritidis in phosphate buffered saline73. Simultaneous determination of acetaminophen and diclofenac by exploring of the multiple pulse amperometry detection modes27 Gravityassisted

Amperometric determination of estriol83 Electrochemical detection of naproxen84 Amperometric detection of tear glucose 61 Electrochemical detection of phenol in tap water62



Green chromatographic separation and electrochemical detection of DA and AA76 Electrophores

Blood urea nitrogen and glucose detection in human whole blood20 Separation and detection of mixed ion samples and bio- samples 30

is

Capillary electrophoresis electrochemical detection of blood urea nitrogen in whole blood18 Constructing passive microfluidic systems32

Wicking

Performing chemical synthesis and sensing and bovine serum albumin detection and quantification of glucose present a human blood plasma 68 sequential determination of Cu(II) and Zn(II)40 Colorimetric assessing of glucose in artificial urine70 Introduction of a rapid, low-cost and sensitive biosensor for Infectious bronchitis virus detection by using molybdenum disulphide85.

Knots and twists Gravityassisted Electrophores is

Controlled protein delivery, electrophoretic separation and isolation of solutes65 Knotting to link different thread materials, providing the ability to physically concentrate solutes by chromatographic interaction. Application of trapping and detection of bacteria cells for urinary tract infection65

Surface acoustic wave Knots, twists and adhesives

Quantitative assays of hydrogen peroxide and glucose46

Wicking

Tunable acoustically driving fluid in a thread network and a thread network embedded in hydrogel.66

Various mechanisms of flow control in yarns were shown and discussed37


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Wax masking

Wicking

Detection of different electro-active compounds86

Making channels using hollow spun fibres

Wicking

Demonstration of the potential of using hollow or liquid core fibres as microfluidic channels87.

Simultaneous quantifying small concentrations of multiple biomarkers of disease using 2D and 3D microfluidic devices55 Quantitatively determination of human chorionic gonadotropin42 Wicking Wax patterning

Bovine Serum Albumin detection in artificial urine29 Glucose determination in different sample resources56 Determination of lactate concentration in saliva samples43 Quantitative colorimetric detection of glucose or bovine serum albumin in artificial urine45

Fabrics

Developing a µTAD for wireless elechrochemiluminescese detection of TriPropylamine and H2O258 Gravityassisted

Wax patterning to create a µTAD for detection of Cr(III) in water57 Colorimetric assays of glucose and protein in artificial urine 49

Photolith ographic patterning

Wicking

Hydrophi

Wicking

Detecting lactate in sweat51 An enzyme biosensor based on colorimetric detection of hydrogen peroxide was reported60 Real-time chemical analysis of sweat composition, in particular pH88



lic threads on hydrophobic fabric

Applicability toward facilitated and controlled biofluid removal, such as skin surfaces experiencing heavy perspiration was demonstrated39 Electrophores is

Hydrophi lic/hydropho bic threads patterning

Separation of small molecule as well as macromolecule (protein) solutes19 Immunoassay14

Wicking

Making microfluidic fibre channels with switchable water transport54 Flow control by systematic change in fabric design.53

Hydrophi lic patterning of a hydrophobic substrate

Nil

Wicking

Presenting patterned fabric allowed selective permeation of water-based reagents through the hydrophilic regions89

Wicking

A wearable, electronic-free and flexible microfluidic system based on ionic liquid polymer gels for monitoring in real-time the pH of the sweat generated during an exercise period was presented71 Low cost SERS substrates75


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EMERGING DIRECTIONS AND FUTURE TRENDS

Very recently, due to the characteristics of thread and fabrics along with their potential biocompatibility, applications of µTADs have been expanded into bio-related studies. Ramesan and co-workers have demonstrated serial dilution in thread network embedded in a transparent hydrogel that mimics in vivo tissue microenvironment using surface acoustic wave (Figure 6A)66. Mostafalu et al. also used a surface modified threads capable of sensing electrochemically to develop an integrated µTAD platform used to measure both physical (strain and temperature), and chemical (pH and glucose) properties both in vivo and in vitro78. Functionalized filaments composed of cellulose nanofibrils conjugated with antihuman haemoglobin (anti-Hb) antibodies have also been utilised to detect haemoglobin with high sensitivity and low levels of nonspecific adsorption81 (Figure 6B). Our group has also recently introduced low-cost µTADs utilizing novel 3D printed supporting platform along with commercial threads. Possibility of controlled protein delivery, electrophoresis isolation and separation of biomolecules and bacteria cells has also been also demonstrated65 (Figure 6C).

ACS Paragon Plus Environment

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Figure 6. (A) Acoustically-driven fluid into a thread network embedded in transparent hydrogel66, (B) pH-sensing system communicating with a smart phone via a Bluetooth platform78. and (c) The use of knotting to link different thread materials to trap bacteria for urinary tract infection65 Textile-based microfluidics is a relatively recent and elegantly simple technology and provides significant opportunities for the development of ASSURED6 analytical devices. A present textilebased microfluidics have been emerged to tackle the cost issue of the chip-based microfluidics, however to the best of our knowledge none of them have been commercialized. To-date most research groups have explored simple fluid wicking in this area and only a few reports are available on the true potential of using controlled electrophoretic systems in textile-based microfluidics. Although fluid can be transported in textile-based microfluidics by simple wicking, in order to obtain controllable devices with precise fluid control, a driving force other than simple capillary action or ‘wicking’ is required. Electric fields have the potential to be used to move, pre-


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concentrate and separate solutes within fluids. In this instance the fluid is held as a surface layer upon a thread or fibre, where both electroosmotic force and solute electroosmotic migration can take place in a controlled manner. More significantly, separations that are achievable in capillaries systems can be simulated on the surface of fibres using close environmental control. A huge potential exists to exploit the separation potential of electrophoresis in multiple dimensions, either upon single threads in simple mono-directional arrangements, or multidimensional and woven fluidic designs, incorporating multiple types of interconnected fibres with different arrangements. Moreover, modified fibres, or functionalized composite fibres can potentially be used for ‘on-fibre’ trapping, isolation and derivatization. By understanding of the fundamental underlying principles of the nature and role of the fibre material in the electrophoretic separations, together with its impact upon the efficiency of ambient ionization, this technology has the capacity to provide solutions to the analysis of small molecules to large biomolecules, and even whole cells. The approaches in this review indicate that there is a potential to develop new analytical platforms for ‘on-fibre’ detection. Whereby the open textile or fibre format permits a degree of accessibility to extract or detect the solute species as they are separated across the surface in a manner not available in classical chromatographic or capillary based analytical techniques.

AUTHOR INFORMATION Corresponding Author *[email protected] Author Contributions The manuscript was written through contributions of all authors. All authors have given approval to the final version of the manuscript.


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ACKNOWLEDGMENT The authors acknowledge funding support from the Australian Research Council Centre of Excellence Scheme (CE 140100012) and the Australian National Fabrication Facility (ANFF) Materials Node under the National Collaborative Research Infrastructure Strategy providing nano and micro-fabrication facilities for Australia’s researchers. REFERENCES (1)

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Life-Saving Threads: Advances in Textile-Based Analytical Devices

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