Shayan Mehraeen

Electropolymerized polypyrrole (PPy) is considered as one of the promising polymers for use in ionic-electroactive or conducting polymer (CP) actuators. Its electromechanical properties surpass those of other prominent CPs such as poly(3,4-ethylenedioxythiophene) polystyrene sulfonate (PEDOT/PSS) or polyaniline. However, freestanding and linear contracting actuator fibers made solely of electropolymerized PPy are not available yet. This work therefore targets the development of all-CP-based actuator fibers: electromechanically active PPy is electropolymerized on the surface of wet-spun, also electromechanically active PEDOT/PSS fibers. The thickness of the PPy fiber sheath is varied by using different electropolymerization durations. Mechanical and actuation properties of the different PEDOT/PPy core-sheath actuator fibers are investigated via tensile tests and isotonic actuation strain and isometric actuation force measurements, respectively. The fiber actuators show high tensile stability in both dry and aqueous conditions, rendering them highly suitable for actuation in aqueous electrolyte media. Regarding linear, untwisted, and uncoiled CP fiber actuators, the presented actuation measurements demonstrate to the best of our knowledge the highest reported linear contractile actuation strains of up to 2.2% in electrolytes and remarkable tensile actuation stresses of 1.64 MPa, as well as a high long-term cyclic actuation stability using varying actuation durations. This renders the fibers as a highly promising material, particularly with regard to their further structural textile processing for use in actuating wearables or soft robots.

Like skeletal muscles having a fibrous structure, conducting polymers can actuate upon electrical stimulation and can be shaped into fibers. Through textile assembly strategies of such fibers, complex actuating architectures are possible. However, state‐of‐the‐art strategies using short pieces of yarn, which compel manual integration, are not fully taking advantage of textiles. To manufacture actuating textiles that best exploit textile properties like softness and pliability, and to enable production upscaling, a production of continuous, actuating fibers is presented here. These fibers are produced from commercial polyamide 6/6 filaments by first continuously dip‐coating in a modified commercial poly(3,4−ethylenedioxythiophene):poly(styrene sulfonate) (PEDOT:PSS) dispersion before the electropolymerization of polypyrrole (PPy), where the fibers are withdrawn continuously through an electrolyte solution containing the pyrrole monomer. By employing a cyclic dip‐coating with individual viscosity, drying temperature, and withdrawal speed for each layer, and by adjusting the tension, speed, and applied potential of the electropolymerization, their isotonic strain is enhanced threefold. Their specific tension, at 400 µN tex⁻¹, reaches slightly higher than human skeletal muscle fibers. Furthermore, these continuous actuating fibers produced on the meter are processable in an industrial knitting machine. This study anchors the development of textile muscle fibers for future textile muscles.

Poly(3,4‐ethylenedioxythiophene) (PEDOT), an inherently electrically conductive or conjugated polymer (CP), exhibits the potential to play a significant role in the development of innovative fiber materials for use in smart textiles, such as wearables. Furthermore, these fibers can function as artificial muscles in the emerging field of interactive fiber rubber composites. This study introduces a straightforward and efficient method for creating PEDOT‐based, biomimetic, fiber‐shaped, linearly contracting ionic electroactive polymer actuators. To achieve this, a wet‐spinning technique is presented, which enables a continuous production of PEDOT:polystyrene sulfate (PSS) fibers at high production rates of 34 m h⁻¹, an additional fiber washing step and a sulfuric acid posttreatment step to increase the fibers conductivity. The fibers provide a high conductivity of 1028 S cm⁻¹, maximum tensile strength reaching 182 MPa, and a maximum elongation of 24%. When utilized as CP actuators in an aqueous sodium dodecylbenzenesulfonate electrolyte medium, the fibers demonstrate a repeatable maximum isometric contractile force of 1.64 mN and repeatable linear contractile strain up to 0.56%. Furthermore, a high level of cyclic long‐term actuation stability can be demonstrated. Notably, these contractile strains are, to the best of knowledge, the highest reported values for pristine PEDOT:PSS fibers.

Electronic textiles (E‐textiles) are made using various materials including carbon nanotubes, graphene, and graphene oxide. Among the materials here, e‐textiles are fabricated with reduced graphene oxide (rGO) coating on commercial textiles. rGO‐based yarns are prepared for e‐textiles by a simple dip coating method with subsequent non‐toxic reduction. To enhance the conductivity, the rGO yarns are coated with poly(3,4‐ethylene dioxythiophene): poly(styrenesulfonic acid) (PEDOT) followed by electrochemical polymerization of polypyrrole (PPy) as the electromechanically active layer, resulting in textile actuators. The rGO‐based yarn actuators are characterized in terms of both isotonic displacement and isometric developed forces, as well as electron microscopy and resistance measurements. Furthermore, it is demonstrated that both viscose rotor spun (VR) and viscose multifilament (VM) yarns can be used for yarn actuators. The resulting VM‐based yarn actuators exhibit high strain (0.58%) in NaDBS electrolytes. These conducting yarns can also be integrated into textiles and fabrics of various forms to create smart e‐textiles and wearable devices.

Smart textiles combine the features of conventional textiles with promising properties of smart materials such as electromechanically active polymers, resulting in textile actuators. Textile actuators comprise of individual yarn actuators, so understanding their electro‐chemo‐mechanical behavior is of great importance. Herein, this study investigates the effect of inherent structural and mechanical properties of commercial yarns, that form the core of the yarn actuators, on the linear actuation of the conducting‐polymer‐based yarn actuators. Commercial yarns were coated with poly(3,4‐ethylenedioxythiophene)‐poly(styrenesulfonate) (PEDOT:PSS) to make them conductive. Then polypyrrole (PPy) that provides the electromechanical actuation is electropolymerized on the yarn surface under controlled conditions. The linear actuation of the yarn actuators is investigated in aqueous electrolyte under isotonic and isometric conditions. The yarn actuators generated an isotonic strain up to 0.99% and isometric force of 95 mN. The isometric strain achieved in this work is more than tenfold and threefold greater than the previously reported yarn actuators. The isometric actuation force shows an increase of nearly 11‐fold over our previous results. Finally, a qualitative mechanical model is introduced to describe the actuation behavior of yarn actuators. The strain and force created by the yarn actuators make them promising candidates for wearable actuator technologies.

Electrochemical devices as conducting polymer‐based actuators or textile actuators often use layers of different conducting polymers. Although research has been performed on such devices, it is still not very clear how the different layers affect each other. Here we attempt to clarify such influence on yarn actuators using electrochemical methods. Different electrochemical methods as cyclic voltammetry, chronoamperometry or chronopotentiometry were used to electropolymerize polypyrrole on top of a poly(3,4‐ethylenedioxythiophene) polystyrene sulfonate (PEDOT:PSS) coated textile yarns by using different applied electrochemical conditions (potentials/currents). Thus, we found that selecting suitable conditions (as an applied potential of +0.8 V) for such electropolymerization is key to obtain a polypyrrole of high quality. Besides, we show that the underlying layer of PEDOT:PSS has an influence on such electropolymerization conditions and can be subjected to parallel redox reactions as oxidation or electrochemical degradation that influence the electropolymerized polypyrrole.

The pursuit of a promising replacement candidate for graphite as a Li-ion battery anode, which can satisfy both engineering criteria and market needs has been the target of researchers for more than two decades. In this work, we have investigated the synergistic effect of nitrogen-doped reduced graphene oxide (NrGO) and nanotubular TiO ₂ to achieve high rate capabilities with high discharge capacities through a simple, one-step and scalable method. First, nanotubes of hydrogen titanate were hydrothermally grown on the surface of NrGO sheets, and then converted to a mixed phase of TiO ₂ -B and anatase (TB) by thermal annealing. Specific surface area, thermal gravimetric, structural and morphological characterizations were performed on the synthesized product. Electrochemical properties were investigated by cyclic voltammetry and cyclic charge/discharge tests. The prepared anode showed high discharge capacity of 150 mAh g ⁻¹ at 1 C current rate after 50 cycles. The promising capacity of synthesized NrGO-TB was attributed to the unique and novel microstructure of NrGO-TB in which long nanotubes of TiO ₂ have been grown on the surface of NrGO sheets. Such architecture synergistically reduces the solid-state diffusion distance of Li ⁺ and increases the electronic conductivity of the anode.

Polyaniline nanofibers have shown promising electrical and electrochemical properties which make them prominent candidates in the development of smart systems employing sensors and actuators. Their electrochemical actuation potential is demonstrated in this study. A trilayer composite actuator based on polyaniline nanofibers was designed and fabricated. Cross-linked polyvinyl alcohol was sandwiched between two polyaniline nanofibrous electrodes as ion-containing electrolyte gel. First, electrochemical behavior of a single electrode was studied, showing reversible redox peak pairs in 1 M HCl using a cyclic voltammetry technique. High aspect ratio polyaniline nanofibers create a porous network which facilitates ion diffusion and thus accelerates redox reactions. Bending displacement of the prepared trilayer actuator was then tested and reported under an AC potential stimulation as low as 0.5 V in a variety of frequencies from 50 to 1000 mHz, both inside 1 M HCl solution and in air. Decay of performance of the composite actuator in air is investigated and it is reported that tip displacement in a solution was stable and repeatable for 1000 s in all selected frequencies.

Successful performance of biocompatible hybrid systems in various biomedical applications such as wound healing patches, and scaffolds for stem cell preparation have been reported. However, relatively poor structural properties and further bacterial infection have been the major drawbacks for their commercialization. In order to improve the antimicrobial property of such structures, transition metals have been previously added to the media. However, the potential risk of metal pollution as well as hardship of processing has put this approach into obsolescence. Herein the ternary polyvinyl alcohol/reduced graphene oxide/polyaniline fibrous nanocomposites, as substitute for transition metal-containing nanocomposites, were prepared via electrospinning. The mats' structural properties (e.g. rheological, morphological, electrical and mechanical properties) and their antibacterial properties against E. coli bacteria cultures after two different treatments (including thermal and acid doping approaches) were systematically investigated. It was shown that in addition to significant structural improvement, an over 80% antibacterial property enhancement in treated mats in comparison to pristine PVA fibers were achieved. Finally the interaction and main effect analyses were used for suggesting the optimum antibacterial specimen conditions.