key challenges for the next generation of wearables...1 key challenges for the next generation of...

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1 Key challenges for the next generation of wearables Mohammad Amin Rezaei The material in this tutorial is based in part on IEEE Spectrum and my own research. For more information, please write to [email protected] © 2020 K. N. Toosi University of Technology 1.Introduction Wearable sensors have received considerable attention since they enable continuous physiological monitoring toward maintaining an optimal health status and assessing physical performance. Different wearable sensors have gained significant interest over the past few years. Wearable sensors can be defined as devices which can be worn by humans to track human health. Based on the advances in fabrication of sensors, wearable health sensors have been developed for several purposes. In this regard, various wearable sensors have been fabricated to recognize different disease. Wearable sensors can be divided to two main groups: (a) physical, and (b) electrochemical [1]. Wearable health monitoring systems are considered as the next generation of personal portable devices for telemedicine practice. These systems are based on monitoring different kinds of biological signals released by human beings through saliva, urine, breathing and epidemic skin perspiration. Scientists identified three engineering problems that must be tackled for an emerging class of biochemistry wearables: flexibility, power, and treatment delivery. In this report, the problems mentioned in the following sections are discussed, in the second section discussed material characteristics of this devices, third section introduce biofuel cell as power that said challenges and solution and section four, More advanced biochemistry wearables could also deliver drugs or chemicals themselves in addition to sensing, where one device would be capable of performing delivery the drug needed subcutaneously through microneedles that this section mentioned microneedles delivery strategies.

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  • 1

    Key challenges for the next generation of

    wearables

    Mohammad Amin Rezaei

    The material in this tutorial is based in part

    on IEEE Spectrum and my own research.

    For more information, please write to

    [email protected]

    © 2020 K. N. Toosi University of Technology

    1.Introduction

    Wearable sensors have received

    considerable attention since they enable

    continuous physiological monitoring

    toward maintaining an optimal health

    status and assessing physical

    performance. Different wearable sensors

    have gained significant interest over the

    past few years. Wearable sensors can be

    defined as devices which can be worn by

    humans to track human health. Based on

    the advances in fabrication of sensors,

    wearable health sensors have been

    developed for several purposes. In this

    regard, various wearable sensors have

    been fabricated to recognize different

    disease. Wearable sensors can be divided

    to two main groups: (a) physical, and (b)

    electrochemical [1].

    Wearable health monitoring systems

    are considered as the next generation of

    personal portable devices for

    telemedicine practice. These systems are

    based on monitoring different kinds of

    biological signals released by human

    beings through saliva, urine, breathing

    and epidemic skin perspiration.

    Scientists identified three engineering

    problems that must be tackled for an

    emerging class of biochemistry

    wearables: flexibility, power, and

    treatment delivery. In this report, the

    problems mentioned in the following

    sections are discussed, in the second

    section discussed material characteristics

    of this devices, third section introduce

    biofuel cell as power that said challenges

    and solution and section four, More

    advanced biochemistry wearables could

    also deliver drugs or chemicals

    themselves in addition to sensing, where

    one device would be capable of

    performing delivery the drug needed

    subcutaneously through microneedles

    that this section mentioned microneedles

    delivery strategies.

  • 2

    2. Desired features for wearable

    healthcare devices and Materials design

    strategies

    wearable healthcare devices design

    concepts have several ideal

    characteristics, e.g., stretchability,

    ultrathin, biocompatibility,

    biodegradability, and self-healing all of

    which will be highlighted in this section.

    2.1 Stretchability

    In recent years, the application of brittle

    and hard like metals and silicon in wearable

    device requiring large deformation has been

    limited. A stretchable sensor with high

    performance and elastic mechanical

    response is an ideal choice for the next

    generation of health care applications. Good

    tensile properties make the conformal

    contact between the device and the dynamic

    complex structure skin have high spatial and

    temporal resolution, which enhance

    collecting the signal from the skin interface.

    In the past decade, the rapid development of

    new concepts of structural design, new

    nanomaterials, manufacturing technology

    and applications have facilitated to great

    advances in stretchable electronic

    technology. At the device level, there are two

    main forms of retractable design, i.e.

    essentially retractable materials or through

    appropriate geometric layout of

    conventional materials.

    Recent advances in the development of

    stretchable materials have enabled many

    inherent stretchable devices to be realized.

    For instance, Bao et al. proposed a design

    concept for scalable semiconductor

    polymers, including the introduction of

    chemical groups to facilitate dynamic non-

    covalent crosslinked of conjugated polymers.

    The results show that the high field-effect

    mobility of the polymer can be recovered

    even under 100 % strain after 100 cycles.

    Figure 1.Schematic of the conjugated polymers under

    stretching and releasing

    The above research provides a general

    platform for integrating other intrinsically

    stretchable polymer materials and makes it

    possible to manufacture the next generation

    of stretchable wearable device.

    Another way to keep good strain-resistant

    conductivity and stretchability is to fabricate

    the conductive composites. Metal

    nanoparticales (NPs), nanowires (NWs),

    nanosheets and carbon nanotubes (CNTs)

    can be combined with stretchable

    elastomers. Cao et al. reported a composite

    ink consisting of adhesive rubber and soluble

    silver salts. This ink can be placed directly on

    a ballpoint pen and written on a stretchable

  • 3

    substrate, thus making stretchable sensors

    and interconnects with the wearable

    electronic devices. However, for intrinsically

    stretchable devices, a challenge is to find

    sealed, stretchable packaging materials.

    2.2 Ultrathin and conformality

    the traditional real-time monitoring

    equipment has some serious defects, such as

    rigid structure, high power consumption and

    limited function, which brings inconvenience

    to daily life and limits the medical

    application. An attractive way to solve these

    problems is to develop flexible biomedical

    sensors that provide conformal and ultra-

    sensitive properties for invisible links

    between humans and electronic devices. In

    this regard, a variety of concepts have been

    adopted to achieve large-scale and close

    contacts with conformal skin, including the

    development of active sensing matrices and

    the fabrication of ultra-thin, low modulus,

    light weight, flexible and stretchable

    membranes for conformal lamination on

    human skin surfaces. Among these, it is

    necessary to reduce the thickness of devices

    so as to make the electronic system more

    imperceptible, flexible and conformable,

    which is particularly conducive to the skin

    and implantable electronic products. Despite

    these advantages, the polymer properties

    and ultra-thin geometry of the substrates still

    pose enormous challenges to fabrication. In

    order to assist this process, rigid support

    substrates with sufficient adhesion are

    usually added to adapt to harsh

    microprocessing circumstances.

    However, after fabrication the stripping of

    ultra-thin and fragile polymer films from the

    supporting substrates will bring new

    problems to the integrity and performance

    maintenance of wearable systems.

    Therefore, in order to solve this problem,

    sacrificial layer can be lead-in between rigid

    support and polymer matrix. Then, the last

    layer of the sacrificial layer is removed by wet

    etching, and the flexible electronic system on

    the polymer substrate is obtained. For

    instance, Lee et al. studied an ultra-thin,

    comfortable, vibration-responsive e-skin

    that can detect skin acceleration, which is

    highly linear with the sound pressure of Ti/Cu

    film as a sacrificial layer. Compared with

    commercial speech recognition equipment,

    the device has higher sensitivity and flat

    frequency response in the speech frequency

    range, which can clearly recognize human

    speech in the presence of environmental

    noise or masks. Because of its low stiffness

    and ultra-thin structure, the device shows

    comfortable fit on the skin. Their research

    demonstrates great potential as the next

    generation of speech recognition devices for

    human-machine interface (HMI) and internet

    of things (IoT) applications, which need

    accurate voice information even in harsh

    acoustic environments.

  • 4

    Figure 2.(a) Schematic of the ultrathin vibration-

    responsive devices. (b) Optical image of the sensor

    attached on the neck skin.

    2.3. Biocompatibility and biodegradability

    In real-time medical applications, there is

    a need to be closely related to the biological

    interface, so it is hoped that wearable

    medical equipment will not cause additional

    health threats and comfort, and avoid

    restrictions on daily activities. The

    biocompatibility between human body and

    wearable sensors is the key to avoid

    triggering immune response. In general,

    compared with the matrix materials, active

    materials have higher risk. It is reported that

    due to the needle-like shape and small size of

    CNTs (carbon nanotubes), injecting large

    quantities of them into the lungs of mice can

    cause asbestos-like pathogenicity.

    Therefore, for future healthcare application

    of nanostructured materials, there is a great

    need for more in-depth understanding of

    immune response and a definition of

    exposure criteria under various

    circumstances, such as skin contact, intake,

    inhalation and injection. It is found that GaN

    has good biocompatibility and is an ideal

    choice for the application of high-speed

    electronic and optoelectronic devices. Many

    biocompatibility biosensors based on GaN

    are proposed. Recently, Rogers et al.

    proposed a silicon-based multifunctional

    brain sensor. The sensors for medical

    monitoring are completely biodegradable.

    Multiple immunohistochemical studies of

    brain tissue after implantation (2, 4 and 8

    weeks) showed that the sensor and its

    byproducts dissolved in intracranial space

    were biocompatible. This traditional

    semiconductor is biocompatible and can be

    used for biomedical implants and health

    monitoring. At the same time, a number of

    organic active substances, like

    polyethylenedioxythiophene (PEDOT) and

    polypyrrole (PPy), have been widely found to

    be biocompatible which can be used for

    monitoring cytoactive. Carbonized

    commodities such as tissues and cotton also

    have great potential in building

    biocompatible wearable sensors.

    Recently, biomaterials have been

    extensively studied as substrates and active

    components of various biocompatible

    electronic devices. The highly conductive

    carbon nanofibers films extracted from silk

    fabrics which were treated by simple thermal

    treatment without any chemical treatment

    were reported by Wang et al. This kind of

    carbon material has the characteristics of

    large production capacity, natural renewable

    resources, and is beneficial to the

    environment and human beings. Although

    the electronic performance of these devices

  • 5

    will require considerable optimization to be

    useful for wearable sensor applications, they

    show a promising biocompatibility route.

    Transient electronics technology is a new

    emerging technology in recent years. Its goal

    is to develop systems and equipment that

    can be absorbed by human organisms or

    environmental microorganisms at

    programmed speed. Biodegradable and

    Water-soluble materials are often

    investigated to be used in transient

    implantable devices. For example, Bao et al.

    designed and manufactured a highly

    sensitive flexible pressure sensor made

    entirely of biodegradable materials. The

    sensor has good sensing performance and

    can be used as a wearable medical device for

    continuous cardiovascular monitoring,

    including pulse signal acquisition of radial

    artery, carotid artery and human femur. This

    is the first step in sensor manufacturing.

    More complex and degradable sensors can

    be used in human biomedical applications to

    avoid further surgical intervention and

    reduce waste generation.

    Figure 3.(c) Illustration of the biodegradability healthcare

    sensing systems. (d) Photograph of the as-fabricated

    system.

    2.4. Self-healing

    At present, wearable healthcare device is

    often limited by robustness because its

    components are easily scratched and

    damaged on the human body, which may

    damage its function and reduce its

    perception performance. Ideal wearable

    equipment can not only retain its electronic

    function, but also heal itself after slight

    mechanical damage by restoring the

    electrical and mechanical characteristics.

    Very recently, great progress has been

    obtained in the development of self-healing

    chemistry, but only a few self-healing

    polymer systems have been used in

    electronic applications. Composite materials

    are commonly used as self-healing materials,

    which are filled with drug-loaded capsules or

    conductive particles. The composite

    hydrogel has strong and fast self-healing

    ability. The self-healing efficiency induced by

    reversible Ag-thiolate bond is as high as 93 %,

    which provides a good electromechanical

    performance in deep impression for the self-

    healing of hydrogels. In addition, by

    combining the conductive one dimensional

    network with the tensile self-healing

    polymer, nano-materials/ polymer

  • 6

    composites can reconstruct and restore the

    mechanical and conductive properties.

    Figure 4.Schematic illustrations of the self-healing

    mechanism for composite polymer matrix.

    2.5 Flexible substrates

    For traditional rigid medical sensors, glass,

    Si or SiO2 are used as substrates, which is not

    the key factor to determine the properties of

    the device. Yet, the substrate material is a

    key consideration in the development of

    wearable device structure. Low roughness

    and high mechanical flexibility are the high

    requirements of substrate materials.

    Generally, metal foils, rubber and elastic

    polymers are extensively choose as

    substrates because of their great mechanical

    elasticity, good chemical resistance and

    thermal stability. Many commercial

    polymers and elastomers can be used as

    substrates for flexible and stretchable

    electronic products. PDMS

    (polydimethylsiloxane) is a commercial

    silicon elastomer with good processability,

    hydrophobic, non-flammable, non-toxic and

    high tensile strength (up to 1000 %). It has

    been used in wearable sensors, prostheses

    and microfluids. The inherent flexibility and

    expansibility of PDMS make the

    corresponding devices respond well to

    compression strains, tension and torsion. In

    addition, the extensibility of PDMS can be

    improved by geometric structure to meet the

    application requirements of coplanar

    devices. Therefore, PDMS matrix has good

    biocompatibility, soft, curved and extensible

    skin surface, which is suitable for biological

    health applications. The sensitivity of

    microstructured thin films is much higher

    than that of unstructured elastomer thin

    films, and can be adjusted by different

    microstructures. These advantages expand

    its applicability as a large area substrate for

    wearable sensing systems. In certain

    specially appointed applications, some other

    substrates like Ecoflex or PU may also be

    beneficial. Although silicon elastomer films

    have been widely used as substrates for

    wearable sensing systems, they still face

    some key challenges: (1) Compare with

    silicon wafers commonly used in electronic

    industry, the surface quality of silicon

    elastomers is difficult for integrated

    technique; (2) The problem of long-term

    stability of silicon elastomer is widespread

    due to their high permeability; (3) The poor

    thermal stability of the silicon elastomer

    seriously limits the preparation temperature

    of the electrode.

    In addition to synthetic substrates, some

    natural materials have also been opened for

    manufacture of wearable system substrates.

    Biomaterial is the largest material system in

  • 7

    nature. It has good biocompatibility,

    biodegradability, versatility, sustainability

    and low cost. Fibers and textiles are ideal for

    wearable sensing systems because they are

    supposed to be the closest natural materials

    to human skin. For instance, natural silks are

    not only an abundant and attractive

    biomaterial, but also satisfy the mechanical

    requirements of irregular deformation.[2]

    3.Power

    As the demand for wearable sensors

    grows, so too does the demand for relevant

    power sources. Wearable sensors are

    increasingly becoming “energy-hungry” in

    order to meet the increasing demands of

    detecting multiple parameters

    simultaneously, performing complex data

    analysis, communicating with other sensors,

    devices and data transmission. The scientific

    community that has interest in solving this

    issue has broadly focused on three aspects –

    develop low-power energy efficient devices,

    compact, energy dense wearable power

    sources and adaptive algorithms for

    intelligent, low-power consuming

    electronics. Advances in the field of wearable

    energy devices have not been able to cope

    with the speed at which wearable sensor

    technology has progressed. Limitation

    caused by inefficient wearable power

    sources is a common roadblock for effective

    adaptation of wearable sensors. It is thus

    imperative to develop wearable power

    sources that are in the vicinity of the target

    wearable electronic device in order to

    obviate the need for long wires and ease of

    complete device integration with the body.

    In this regard, several avenues, such as

    wearable batteries, supercapacitors, solar

    cells, biofuel cells, thermoelectric, and

    piezoelectric/triboelectric, have been

    explored by researchers to realize wearable

    power devices. In biochemical wearable

    batteries refer to biofuel cells.

    3.1 biofuel cells challenges

    Biofuel cells that harvest biochemical

    energy using biological components

    represent an attractive “green” alternative

    for various wearable and implantable

    applications. Biofluids, such as sweat, tears,

    interstitial fluid and blood, are rich with

    metabolites that can be exploited as fuels by

    wearable biofuel cells to generate usable

    electrical energy. Moreover, biofuel cells act

    as selfpowered sensors and hence these

    systems mandate lower energy

    requirements as compared to conventional

    chemical sensors. This is attractive for

    wearable applications where energy supply

    is usually a critical challenge. Although, these

    attributes sound striking, today’s wearable

    biofuel cells face several daunting challenges

    that hamper their use as viable energy

    sources for various wearable applications. To

    begin with, enzymes that convert the fuels

    into energy are quite labile and lose their

    catalytic properties in presence of harsh

    conditions that may be encountered in

  • 8

    wearable electronics, e.g. varying

    temperature, humidity, or presence of

    certain chemical species. The operational

    lifespan of the wearable biofuel cells is also

    short compared to the energy demands of

    the wearable electronics. In addition,

    continuous reproducible flow of high

    concentration of biofuel to the wearable

    biofuel cells is not possible, since the flow of

    these biofuels is regulated by the human

    physiology. Thus, continuous generation of

    constant power is quite challenging. Also, the

    power generated by these devices is low with

    the output voltage changing gradually with

    time. Furthermore, wearable biofuel cells

    must possess stretchability to endure

    mechanical deformations common for

    wearables applications. Developing body

    compliant stretchable biofuel cells which

    protect the enzymes and other chemical

    reagents from degrading/leaching under

    changing conditions is certainly a challenge.

    A concoction of these challenges currently

    impedes the utilization of wearable biofuel

    cells to directly power electronic devices.

    3.2 solution

    By properly addressing the challenges facing

    wearable biofuel cells, these devices could

    become a viable energy source for on-body

    applications. A handful of researchers are

    attempting to address the issue involved in

    developing soft, stretchable biofuel cells by

    combining advances in materials science. For

    example, our group recently demonstrated a

    highly stretchable glucose biofuel cell that

    could be repeatedly stretched by 300%

    without much effect on its power generation

    ability (Figure 5). Similarly, Ogawa et al

    demonstrated a stretchable textile-based

    biofuel cell that could be repeatedly

    stretched by 50% with the small impact on

    the power output (20-30% loss). Similar

    efforts must be made to develop body-

    compliant biofuel cells. The problem of long-

    term stability of wearable biofuel cells under

    diverse conditions could be addressed by

    incorporating enzyme stabilizing agents or

    nano/microsized hybrid materials and by

    providing biocompatible microenvironments

    to the immobilized enzyme. Researchers

    could also look into developing multi-fuel

    biofuel cells, complete oxidation of fuels and

    rechargeable biofuel cells to address the

    issue of continuous supply of energy. At the

    same time, researchers should leverage

  • 9

    nanomaterials to further enhance the power

    conversion efficiency of the biofuel cells.[3]

    Figure 5.highly stretchable biofuel cells

    4. Treatment delivery

    4.1 Microneedles: delivery strategies

    Microneedle arrays (MN) are minimally

    invasive devices that by-pass the SC barrier,

    thus accessing the skin microcirculation and

    achieving systemic delivery by the

    transdermal route. MN (50– 900 µm in

    height, up to 2000 MN cm2) in various

    geometries and materials (silicon, metal,

    polymer) are produced using

    microfabrication techniques. MN are applied

    to the skin surface and painlessly pierce the

    epidermis, creating microscopic aqueous

    pores through which drugs diffuse to the

    dermal microcirculation. MN are long

    enough to penetrate to the dermis, but are

    short and narrow enough to avoid

    stimulation of dermal nerves or puncture of

    dermal blood vessels.

    Solid MNs are normally employed in the

    so-called ‘poke with patch’ approach. Solid

    MN are applied to the skin and then

    removed, creating transient aqueous

    microchannels are created in the stratum

    corneum. Subsequently, a conventional drug

    formulation (transdermal patch, solution,

    cream or gel) is applied, creating an external

    drug reservoir (Fig. 6A). Permeation through

    these microchannels occurs via passive

    diffusion. The main limitation of this

    approach is the requirement for a two-step

    application process, which may lead to

    practicality issues for patients. The materials

    used to produce solid MN are typically

    silicon, metals and polymers.

    Coated MNs are prepared by coating solid

    MN with a drug formulation prior to skin

    application. After insertion of coated MN

    arrays into the skin, the coated drug

    formulation will be dissolved and deposited

    in the skin (Fig. 6B). This delivery strategy is

    typically referred to as ‘coat and poke’.

    Coated MNs have been employed for the

    rapid cutaneous delivery of macromolecules,

    such as vaccines, proteins, peptides and DNA

    to the skin. This type of MN allows a simple

    one-step application process, but its main

    limitation is the restricted amount of drug

    that can be coated onto the finite surface

  • 10

    area of the MN structures. Accordingly, the

    use of coated MNs is restricted to potent

    molecules/drugs. Various techniques have

    been developed to efficiently coat the

    individual MN shafts in MN arrays.

    The third type of MN are dissolving MNs.

    They are made by micro-moulding soluble

    matrices, generally a biocompatible polymer

    or sugar, including the active substance. The

    skin insertion of the array is followed by

    dissolution of the MNs tips upon contact with

    skin interstitial fluid. The drug cargo is then

    released over time (Fig. 6C). The release

    kinetics of the drug depends upon the

    constituent polymers’ dissolution rate.

    Therefore, controlled drug delivery is

    achievable by adjusting the polymeric

    composition of the MN array, or by

    modification of the MN fabrication process.

    Hollow MNs allows the delivery of a

    particular medication into the skin via the

    injection of a fluid formulation through the

    inserted hollow needles (Fig. 6D). This type of

    MNs allows continuous delivery of molecules

    across the skin through the MN bore using

    different methods: diffusion or pressure- or

    electrically driven flow. Such systems are

    possibly capable of delivering larger amounts

    of drug substances in comparison to solid,

    coated and dissolving MNs. Hollow MNs are

    made from a range of materials, including

    silicon and metal, glass, polymers and

    ceramic. The main limitations of hollow MNs

    are the potential for clogging of the needle

    openings with tissue during skin insertion

    and the flow resistance, due to dense dermal

    tissue compressed around the MN tips

    during insertion. The first limitation can

    possibly be overcome by using an alternative

    design to locate the bore-opening at the side

    of the MN tip. Partial needle retraction

    following insertion may also enhance fluid

    infusion, due to relaxation of the compressed

    tissue around the tips. However, use of liquid

    drug formulations will require a suitable,

    possibly complex, reservoir and liquid

    formulations are notoriously unstable,

    particularly at the elevated ambient

    temperatures found in the developing world.

    relatively new type of MN arrays are

    prepared from hydrogelforming matrices.

    Such systems were first described recently by

    Donnelly et al. This novel strategy involves

    integrated systems consisting of crosslinked

    drug-free polymeric MN projecting from a

    solid baseplate to which a patch-type drug

    reservoir is attached. After application of the

    MN array to the skin, the inserted needle tips

    rapidly take up interstitial fluid from the

    tissue, thus inducing diffusion of the drug

    from the patch through the swollen

    microprojections (Fig. 6E). These systems are

    manufactured using aqueous blends of

    specific polymeric materials, namely

    poly(methyl vinyl ether-co-maleic acid)

    crosslinked by esterification using

    poly(ethyleneglycol). Garland et al. showed

    that drug delivery can be tailored by

    modulating the crosslink density of the

  • 11

    hydrogel matrix. Importantly, hydrogel-

    forming MNs are removed intact from skin,

    leaving no measurable polymer residue

    behind. However, they are sufficiently

    softened to preclude reinsertion, thus

    further reducing the risk of transmission of

    infection. Other polymers that can be used to

    prepare hydrogel-forming MNs are chitosan,

    PLGA and poly(vinyl alcohol). With these

    alternative polymer systems, however, the

    drug is included inside the hydrogel-forming

    MN patch rather than in an external patch,

    thus limiting the quantity of drug that can be

    delivered.

    Figure 6. A schematic representation of five different MN types used to facilitate drug delivery transdermally. (A)

    Solid MNs for increasing the permeability of a drug formulation by creating micro-holes across the skin. (B)

    Coated MNs for rapid dissolution of the coated drug into the skin. (C) Dissolvable MNs for rapid or controlled

    release of the drug incorporated within the microneedles. (D) Hollow MNs used to puncture the skin and enable

    release of a liquid drug following active infusion or diffusion of the formulation through the needle bores. (E)

    Hydrogel-forming MNs take up interstitial fluids from the tissue, inducing diffusion of the drug located in a patch

    through the swollen microprojections.

  • 12

    References

    [1] Nasiri, Sara, and Mohammad Reza Khosravani. "Progress and challenges in

    fabrication of wearable sensors for health monitoring." Sensors and Actuators A:

    Physical (2020): 112105.

    [2] Lou, Zheng, et al. "Reviews of wearable healthcare systems: Materials, devices and

    system integration." Materials Science and Engineering: R: Reports 140 (2020): 100523.

    [3] Bandodkar, Amay J., Itthipon Jeerapan, and Joseph Wang. "Wearable chemical

    sensors: Present challenges and future prospects." Acs Sensors 1.5 (2016): 464-482.

    [4] Larraneta, Eneko, et al. "Microneedle arrays as transdermal and intradermal drug

    delivery systems: Materials science, manufacture and commercial development."

    Materials Science and Engineering: R: Reports 104 (2016): 1-32.