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International Journal of Bioprinting             3D printable conductive composite inks for biocompatible electrodes


            distribution and percolation threshold concentration.   rapidly increased with the GO concentration >2 vol% to
            Pidcock et al. dispersed MWCNT into gellan gum (GG) ,   the printable range and showed shear-thinning behavior.
                                                        [52]
            which is a linear, anionic polysaccharide and has been   The research team hypothesized that some GO flakes
            approved by both the US Food and Drug Administration   roll up at high concentrations, enhancing their elastic
            and the  European Union for medical  usage . The   properties by forming strong network. The GO ink showed
                                                   [62]
            biocompatible property of GG allows the use of wearable or   conductivity of around 100 S/m with and without additional
            transplantable strain gauges. The research team dispersed   components such as F127. Similarly, Shi et al. formulated
            the ink at the ratio of 1:10-1–5:10-1 (indicating 1 mg/mL   aqueous ink with electrochemically derived GO (EGO)
            of MWNT and 0.1–0.5 mg/mL of GG) and 2:10-1–2:10-15   and polydimethylsiloxane (PDMS) submicrobeads . The
                                                                                                       [66]
            (indicating 1–15 mg/mL of MWNT and one-fifth of GG)   PDMS/EGO ink showed shear-thinning behavior, proven
            with ultrasonication and analyzed the viscosity and the   by viscosity decrease with shear rate, and complex modulus.
            conductivity. The viscosity of 2:10-1 is comparable to that   Due to its thixotropic and viscoelastic properties, ink can be
            of water (~1 mPa∙s) at all shear rates. The viscosity of   printed with a small inner nozzle diameter (50 µm). After
            2:10-15 at a low shear rate is 1000 mPa∙s, which is more   the annealing process, EGO deoxygenated and covered
            than twice higher than that of 4 mg/mL GG. However, the   the PDMS submicrobeads, increasing the conductivity
            viscosity decreases to around 200 mPa∙s at a high shear rate,   (0.06  S/m for 0.83 vol%).
            similar to that of 4 mg/mL GG. This observation supports
            the enhancement of shear-thinning behavior with the   4.3. MXene-based printing ink
            introduction of filler. The strain gauge with a gauge factor   After the introduction of  graphene, the potential of 2D
            value of around 15 can be fabricated using the ink.  materials has caught the attention of research community.
              Pedrotty  et al. mixed SWCNTs in nanofibrillated   A novel  2D  material  called  MXene  is  fabricated  from
            cellulose with the surfactant Pluronic F127 at a   the MAX phase, composed of Mn+1AXn, where M is a
            concentration of 1.9  wt% . The complex modulus NFC/  transition metal, A is an A group (mostly IIIA and IVA
                                [63]
                                                                                                  [74]
            SWCNT ink implied elastic behavior (tan  δ < 1) below   group) element, X is C and/or N, and n = 1,2,3 . The A layer
            100 Pa and viscous behavior (tan δ > 1) over 100 Pa, proving   can be etched out using an acid such as hydrofluoric acid,
            shear-thinning behavior for extrusion-based printing. The   leaving the Mn+1Xn layer. MXenes show extraordinary
            decrease in viscosity in response to the shear rate verifies   mechanical and electrical properties. Among various
            this property. The conductivity of the NFC/SWCNT   types of MXenes, Ti C Tx, where Tx represents the surface
                                                                                 2
                                                                               3
            was around 43 S/m. The NFC/SWCNT ink is printed on   terminators (e.g. OH, O , or F), is known to be non-
                                                                                   2
                                                                   [75]
            biocompatible BNC film and attached to the ventricle   toxic . Boularaoui et al. used low-concentration GelMA
            incision; the conductive patch proved the ability to restore   hydrogels as a polymer, and Ti C Tx MXene as a filler
                                                                                           2
                                                                                         3
                                                                                          [67]
            the conductive velocity of the heart.              to create a conductive composite . The ink containing
                                                               0.05 mg/mL MXene showed high cell viability after day 7,
            4.2.2. Graphene-based printing ink                 although the cell viability of 0.1 mg/mL MXene dropped
            Graphene is a single layer of carbon sheet with high   on day  7. The ink showed shear-thinning behavior with a
            conductivity and mechanical properties. Jakus  et al.   slight increase in viscosity at a low shear rate as expected.
            fabricated a 3D printable  graphene (3DG) composite by   The conductivity of  the  ink was  around  0.65 S/m  and
            combining 75  wt%  graphene  flakes with  biocompatible   0.94 S/m at 0.05 mg/mL and 0.1 mg/mL, respectively,
            and biodegradable polylactide-co-glycolide (PLG) .   which is comparable to the conductivity of the electroactive
                                                        [64]
            The solvent was evaporated in a sonicating bath until the   tissues  (0.4 – 0.9   S/m).  Orangi  et al. dispersed Ti C Tx
                                                                                                         3
                                                                                                           2
            viscosity  reached  30 Pa∙s.  The 3DG  showed  high fidelity   MXene and super absorbent polymer beads with DI water
                                                                                              [73]
            that could stack >700 hundred layers and conductivity   and 3D-printed micro-supercapacitors . The ink showed
            of >800 S/m after annealing. However, the hydrophobic   shear-thinning behavior and the storage modulus larger
            property of  graphene hinders its biomedical and   than the loss modulus (tan δ < 1), making the ink printable
            implantation applications. Therefore,  graphene oxide   and sustaining the structure without additive at room
            (GO), oxidized graphene that includes oxygen functional   temperature. The printed structure exhibited outstanding
            groups, or reduced graphene oxide (rGO), which is redoxed   areal capacitances and maximum energy density due to the
            GO for its desired properties is used instead. García-  high electrical conductivity of MXene.
            Tuñón et  al. generated a water-based paste with GO and   5. Electrode integrated cell culture platform
            various materials (e.g., polymers, ceramics, and steel) .
                                                        [65]
            GO suspension showed shear-thinning behavior when   The extrusion-based printing technology facilitates the
            diluted in water at 0.1 – 0.6 vol%. The storage modulus   embedding of the electrode inside the base polymer


            Volume 9 Issue 1 (2023)                        293                      https://doi.org/10.18063/ijb.v9i1.643
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