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Materials Science in Additive Manufacturing                              Materials for 3D-printed electrodes



            PDMS surfactant in an oil environment to prepare liquid-  Increasing the content of ionic liquids is the primary
            liquid 3D printable ink [125] . With an electrical conductivity   approach to improving the electrical conductivity of
            of up to 301 S/m, the ink was formed by combining the   ionic gels, often accompanied by a sharp decrease in the
            light-curing hydrogel with ionic liquids that can enhance   mechanical properties of the gels [134,135] . Liquid leaks can
            its stretchable properties and conductivity. The viscosity   be toxic in the body, limiting the application of ionic
            of the ink and the concentration of PEDOT:PSS can be   gels [136-138] . Yao  et al. utilized granular amphiphilic ionic
            adjusted to within a certain range, increasing the versatility   particles to synthesize ionic gels, as shown in Figure 6B.
            of the ink in 3D printing technology. Zhou et al. reported   The  dissolved ionic  particles  increased  the  mechanical
            a phase-separated ink consisting of an electrical phase   properties of the ionic gels due to electronic interactions
            (PEDOT:PSS) and mechanical phase (hydrophilic PU),   or physical crosslinking, resulting in double-network
            which was prepared to obtain a bi-continuous conducting   ionic gels with high stretchability (>600%) and ultrahigh
                                                                                              2 [139]
            polymer hydrogel (BC-CPH). BC-CPH has high electrical   toughness (fracture energy >10  kJ/m )  . Zhang  et al.
            conductivity (over 11 S/cm), elongation (over 400%), and   used a phase separation strategy to improve the mechanical
            fracture toughness (over  3300  J/m ).  It can  be prepared   properties of the gels by doping lithium salt into the
                                        2
            as an all-hydrogel bioelectronic interface using extrusion   ionic gels [140] . The addition of lithium salts increased
            3D printing [126] . The viscosity of BC-CPH inks can also be   the electrical conductivity of the ionic gel and led to the
            adjusted to be used in electrostatic spinning technology   formation of a phase-separated microstructure within
            for long-term stable electrophysiological recording and   the ionic gel. Lithium ions establish lithium bonds with
            stimulation.                                       hydroxyl groups present on the polymer network, which
                                                               make up the rigid regions of the ionic gel and enhance the
              Despite the excellent properties of conductive polymers,
            the lack of stability still limits their application in daily life.   toughness of the ionic gel (mechanical strength in the range
                                                               of 2.29 to 5.19 MPa). The polymer chains and ionic liquid
            In future research, there is a need to explore strategies to   form the soft region of the ionic gel, which improves the
            improve the conductivity of existing CPs and focus on   elongation of the gel (>1000%). Through DLP 3D printing,
            ways to enhance their structural stability. At the same time,   this ionic gel can be fabricated into microcircuits with
            new types of conductive polymers with extended recycling   complex structures and microarrays for self-powered tactile
            life for flexible medical electrodes should be developed to   sensing, which has considerable potential for applications
            cater to a broader range of applications.          in the field of human-computer interaction [140]  (Figure 6C).
            5. Other materials                                   Hydrogels are moisturizing, flexible, and biocompatible
            In addition to the aforementioned materials, an increasing   materials. However, due to the lack of an effective energy
            number  of  novel  material  systems  are  being  employed   dissipation mechanism, hydrogels are prone to fracture or
            to 3D-print flexible medical electrodes, including ionic   breakage during  repeated stretching or  compression. To
            gels and composite hydrogels. In addition, conductive   satisfy the requirements for long-term applications of flexible
            polymer-doped elastomers possess continuous conductive   electrodes, hydrogels with excellent mechanical properties
                                                               (flexibility, resilience,  etc.) and high stability need to be
            phases  and  excellent  stretchability  and  transparency,   designed. Xiong et al. indicated that acrylated β-cyclodextrin
            attributes that facilitate more direct applications in flexible   could undergo precise host-guest recognition with bile acids
            and wearable electronics.
                                                               and form polymerizable pseudorotaxane by self-assembling
              Ionic gels are solid mixtures with ionic conductivity,   the two molecules [141] . Polymerizable pseudorotaxane can
            usually a mixture of polymeric organic polymers and   be mixed with photo-polymerizable acrylamide hydrogel
            ionic liquids [127-129] . The polymer molecular chains are   to obtain conductive polymerizable rotaxane hydrogels
            interconnected or entangled to form a spatial mesh   (PR-Gel), as shown in Figure 6D. The topological network
            structure, and the structural voids are filled with anions   of  pseudorotaxane  enhances  the  mechanical  properties
            and cations that act as a dispersing medium, giving the   of hydrogels, with a maximum tensile ratio of 830% and
            ionic gel a continuous conductive phase [130-132] . To enable   good flexibility in the temperature range of -20℃ to 60℃.
            ionic gels to be used in 3D printing technology, Huang   Furthermore, this method improved the poor fatigue
            et  al. designed a self-regulating ink consisting of poly   resistance of the hydrogel, and no significant hysteresis was
            (ionic liquid) networks, ionic liquid monomers, and   observed after 500 cycles at 300% strain. This report utilizes
            free ionic liquid. By adjusting the ratio, the rheological   DLP 3D printing to fabricate PR-Gel into flexible sensors
            properties of the ink can be modified, and the printability   with complex geometries that can better adapt to the surface
            of the ionic gel can be increased to realize efficient DIW   structure of the human body and can be used for real-time
            printing (Figure 6A) [133] .                       monitoring of human electrocardiographic signals [141] .


            Volume 2 Issue 4 (2023)                         9                       https://doi.org/10.36922/msam.2084
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