Supplementary Materials for

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1 advances.sciencemag.org/cgi/content/full/3/1/e16327/dc1 Supplementary Materials for Knitting and weaving artificial muscles Ali Maziz, Alessandro Concas, Alexandre Khaldi, Jonas Stålhand, Nils-Krister Persson, Edwin W. H. Jager The PDF file includes: Published 2 January 217, Sci. Adv. 3, e16327 (217) DOI: /sciadv fig. S1. Illustration of the two-step chemical-electrochemical combined CP synthesis used for the fabrication of the textile actuators. fig. S2. Schematic illustration of the three-electrode electrochemical cell. fig. S3. SEM-EDX measurements of the cross section of PEDOT-PPy coated Lyocell single yarn. fig. S4. Circumferential strain measurements of the PEDOT-PPy coated Lyocell single yarn. fig. S. Illustration of electrochemical cell configuration used for characterizing the textile actuators. fig. S6. Stress-strain measurements. fig. S7. Electromechanical characterizations of the elastane-based textile actuator. fig. S8. Current transient during the textile actuator life cycle test. fig. S9. Schematic illustration of the textiles constructions. fig. S1. Electromechanical characterizations of the copper-based fabric actuator. table S1. Effect of polyethylene glycol derivatives on the film thickness and electrical conductivity of the VPP PEDOT film. Other Supplementary Material for this manuscript includes the following: (available at advances.sciencemag.org/cgi/content/full/3/1/e16327/dc1) movie S1 (.mov format). A textuator unit drives a lever arm in a LEGO setup.

2 Two-step chemical-electrochemical combined PEDOT-PPy synthesis. The methodology for the fabrication of the textile-actuator is based on a two-step PEDOT- PPy combined chemical-electrochemical CPs synthesis The chemically synthesized PEDOT seed-layer forms a conductive electrode surface, allowing the following controllable electrochemical deposition of the functional, actuating PPy layer (fig. S1). (1) (2) Vapour-phase polymerization of EDOT Electrochemical synthesis of PPy Textile fabric PEDOT-coated textile PPy/PEDOT-coated textile fig. S1. Illustration of the two-step chemical-electrochemical combined CP synthesis used for the fabrication of the textile actuators. Influence polyethyleneglycol derivatives on PEDOT conductivity Table S1 shows the effect of the amount of polyethyleneglycol derivatives (PEGM and PEGDM) in the oxidative solution on the film thickness and electrical conductivity of VPP PEDOT film synthesized on glass substrate for 3min. table S1. Effect of polyethyleneglycol derivatives (at a 1:1 ratio) on the film thickness and electrical conductivity of VPP PEDOT film synthesized on glass substrate for 3 min.

3 Electrochemical synthesis of PPy. Potentiostat W CE R E F Py.1 M LiTFSI.1 M dissolved PC f ig. S2. Schematic illustration of the three-electrode electrochemical cell Scanning electron microscopy- Energy-dispersive X-ray spectroscopies (SEM-EDX) f ig. S3. (A) SEM image of PEDOT-PPy coated Lyocell-based yarn section (2. wt.% PEDOT and 2. wt.% PPy) and (B) the corresponding EDX (Energy-Dispersive X-ray spectroscopy). The light blue spots in Figure x represent the sulfur domains and illustrate the location of PEDOT (via sulfur atoms of thiophene moieties and dopant) and PPy (via dopant). The light pink spots illustrate the location of PPy domains (via nitrogen atoms of pyrrole moieties and dopant) The average electronic resistance per unit length of the conducting yarn is 126 Ω.cm which is relatively high and sufficient for use in actuators.

4 Weight percent of PEDOT and PPy calculation. The weight percent of PEDOT and PPy was determined by weighing the textile samples in a dry state before and after the two-step chemical-electrochemical coating and calculated with the following relationships. h =,.%=, 1 Circumferential strain measurements of the single yarn. Circumferential strain measurement of the S-yarn was recorded using a Mitutoyo LSM-1H contactless Laser Scan Micrometer (LSM), controlled by a display unit (Mitutoyo LSM-61) and the output signal was fed to the potentiostat ( f ig. S4A). The S-yarn was submerged in a three-electrode electrochemical cell containing LiTFSI (.1 M) dissolved in propylene carbonate. Gold coated polyethylene (PET) substrate was used as counter electrode and a Ag/Ag+ non-aqueous reference electrode. The Ag/Ag + reference electrode is commonly employed in non-aqueous electrochemical studies. The Ag/Ag + reference electrode is made by placing a clean silver wire into an electrolyte containing silver ion i.e. Silver nitrate (AgNO 3 ). The electrolyte in the reference compartment is.1 M AgNO 3,.1 M tetrabutylammonium perchlorate (TBAP)/ acetonitrile CH 3 CN). Typical other polar or dipolar aprotic solvents such dimethylformamide (DMF), dimethylsulfoxide (DMSO) and propylene carbonate (PC) can be also used instead of CH 3 CN. An alternating potential of -1. V and.v was employed to reduce and oxidise the PEDOT- PPy and the circumferential strain (radial expansion) was measured ( fig. S4B). The circumferential strain set-up and measurement procedures are described in more detail in references (33, 3).

5 A Laser Source PPy-coated S-Yarn Cross-section L L PPy Actuated in.1m LiTFSI in PC Laser Detector B (i) 238 Fibre diameter Fibre diameter (µm) (ii) Applied potential (V),6,4,2 6 -, ,4 -,6 -,8-1 -1,2 Applied potential (V) (iii),,3,1 -, ,3 -,

6 f ig. S4. Circumferential strain measurements of the S-yarn. (A) Illustration of experimental set-up for circumferential strain measurement with a laser scanning micrometer (LSM).(B). Displacement (i), applied potential (ii) and current (iii) during charging and discharging of PEDOT-PPy coated S-yarn between -1 V and. V, 1s half period. The PPy-PEDOT layer expands during reduction and contracts during oxidation. Isometric force and isotonic strain measurements. f ig. S. Illustration of electrochemical cell configuration used for characterizing the. textile-actuators.

7 . Tensile strength results A 2 3 B Stress (MPa) 1 1 Stress (MPa) Strain (%) Strain (%) C Stress (MPa) Strain (%) f ig. S6. Stress strain curves (A) single Lyocell yarn (.2 mm in diameter), (B) Single Elastan yarn (.2 mm in diameter) and (C) Single stainless steel wire AISI 34 (.1mm in diameter) Electromechanical characterizations of the elastan based textile-actuator Elastane knitted fabric Elastane S-yarn Strain (%) f ig. S7. Isotonic strain ( L/L ) versus time for Elastan based S-yarn and knitted fabric (L*w= 2mm*mm) during activation between. V and -1 V for 8s. The knitted fabric was 1:1 rib knitwear. PPy coating same as for the Lyocell yarns and fabrics.

8 Current transient during the textile actuator life cycle test A 2 1- cycles B cycles C cylces D cylces f ig. S8. The current versus time for the 12 T-yarn weave life cycle test. (A) 1- first cycles. (B) 1-1 first cycles. (C) cycles and (D) Textiles constructions f ig. S9. Schematic illustration of (A) plain knitted and (B) weave constructions.

9 Copper-based fabric actuator f ig. S1. (A) Three knitted Cu fabrics, from the top to the bottom: an uncoated Cu fabric; a PPy-coated fabric connected with Al wires and a PPy-coated Cu fabric connected with Cu wires. (B) Actuation of a knitted PPy-coated Cu fabric. The voltage has been switched between -1 V and V every 4 s. the average displacement was equal to 96 μm. The displacement was measured using a model laser displacement sensor (optoncdt 17- by Micro-epsilon) connected to a PC.