Supporting Information Easy to assemble PDMS/CNTs/PANI flexible supercapacitor with high energy-to-power density Raphael D. C. Balboni,a Guilherme K. Maron,a Mateus G. Masteghin,b Mehmet O. Tas,b Lucas S. Rodrigues,a Veridiana Gehrke,a José H. Alano,c Robson Andreazza,a Neftali L. V. Carreñoa and S. Ravi P. Silva*b Experimental All detailed information about calculation of areal and gravimetric specific capacitances, energy and power densities are described in detail, according to the following equations: For measurements in three-electrode configuration, the areal specific capacitances (Cspa) were calculated according to the equation (1). 𝐶𝑠𝑝𝑎 = 𝑖 𝑋 ∆𝑡 𝐴 𝑋 ∆𝑣 (1) Where 𝐶𝑠𝑝𝑎 is the areal specific capacitance, 𝐼 is the discharge current, ∆𝑡 is the discharge time, 𝐴 is the area of the electrode (0.49 cm-2) and ∆𝑉 is the potential range. The gravimetric specific capacitances (Cspg) were calculated according to equation (2). 𝐶𝑠𝑝𝑔 = 𝑖 𝑋 ∆𝑡 𝑚 𝑋 ∆𝑣 (2) Where m is the mass of polyaniline electrodeposited on the electrode. The gravimetric performances of the electrodes were based on the mass of PANI, since the mass of carbon nanotubes were difficult to reliably measure. Thus, the PDMS and the CNTs poorly contribute to the electrochemical performance of the device. For measurements performed in the flexible symmetric two-electrode supercapacitors, the Cspa and Cspg were calculated from GCD curves according to the equation (3) and equation (4), using the area of both electrodes (total of 0.98 cm2) and the mass of PANI of both electrodes, respectively. 𝐶𝑠𝑝𝑎 = 2𝐼 ∫ 𝑉𝑑𝑡 ∆𝑉 2 𝐴 (3) Where I is the current of charge/discharge, ∫Vdt is the area of the discharge curve after the IR drop, ∆V is the voltage window and A is the active area of the electrodes (0.98cm2) 𝐶𝑠𝑝𝑎 = 4𝐼 ∫ 𝑉𝑑𝑡 ∆𝑉 2 𝑚 (4) The areal and gravimetric energy densities were calculated from the GCD curves at different current densities, according to the equation (3) 𝐸𝑡 = 𝐶𝑠𝑝 × ∆𝑣 2 2 × 3.6 (5) Where 𝐸𝑡 is the energy density, Csp is the areal (or gravimetric) specific capacitance and ∆𝑉 is the potential range. The power density was calculated according to the equation (4) 𝑃𝑡 = 𝐸𝑡 × 3600 ∆𝑡 (6) Where 𝑃𝑡 is the power density, 𝐸𝑡 is the energy density and ∆𝑡 is the discharge time. For the cyclic voltammetry tests, the values of areal specific capacitances were obtained from the equation (5) 𝐶𝑠𝑝𝑎 = ∫ 2 𝑖𝑑𝑣/𝜈 ∆𝐸 𝐴 (7) Where idv is the area of the curve, 𝜈 is the scan rate, ∆𝐸 is the potential range and A is the area of a single electrode. Fig. S1 Contact angle measurements of PDMS, ACNTA/PDMS and ACNTA-PANI/PDMS Fig. S2 Gravimetric specific capacitance calculated from GCD curves for the ACNTA-PANI/PDMS measured in three-electrode configuration Fig. S3 Electrochemical performance of symmetric two-electrode ACNTA/PDMS supercapacitor. (a) CV curves at scan rates varying between 5 – 50 mV.s-1. (b) GCD curves at different current densities Fig. S4 Ragone plot showing the gravimetric energy and power densities calculated based on the mass of PANI Fig. S5 Illustration of the electrode’s fabrication process showing the steps between the initial Si/SiO2 wafer and the final supercapacitor electrode. The vertically aligned carbon nanotubes (VA-CNTs) are grown at the activated metal catalyst on the surface of the buried oxide, which later is drop-casted facing a mild-cured PDMS, concluding the transfer process. The PDMS+CNT electrode then undergoes a PANI electropolymerization finalizing the fabrication of the flexible SC device Fig. S6 Illustration of the flexible two-electrode supercapacitor assembly Fig. S7 Scheme illustrating the electrochemical measurements under different bending angles Table S1 Comparison of areal and gravimetric specific capacitances of this work measured in two and three-electrode configurations with various similar materials for flexible supercapacitor application. Sample Measurement Current density Scan rate configuration ACNTA-PANI/PDMS Three-electrode 1 mA.cm-2 - Csp Csp Ref (mF.cm-2) (F.g-1) 408 265 This work ACNTA-PANI/PDMS Two- electrode 0.2 mA.cm-2 - 40.6 This 51.6 work Ti3C2Tx/CF Three-electrode - 10 mV.s-1 RuO2/CF Three-electrode - 10 mV.s-1 Three-electrode A.g-1 a-MWCNT/PANI PANI/VACNTs PANI/MWCNT/PDMS Three-electrode 0.25 5 Three-electrode A.g-1 - 5 401 1 - 388 1 - - 201 2 - - 415 3 mV.s-1 481 - 4 mV.s-1 88 - 5 Activated CC Three-electrode - CNT@graphene@PANI/PDMS Three-electrode 0.4 mA - 588.7 - 6 VACNT-SS – TiO2 Two-electrode 1.67 mA.cm-2 - 16.24 - 7 PPy(DBS)/CNTs/PDMS Two-electrode - 100 mV.s-1 3.6 - 8 graphene/MoS2 Two-electrode 0.3 mA - 70 - 9 Two-electrode A.g-1 - - 233 10 - - 10.67 11 - 159 4 MWCNT/PANI CNT/MoS2/PDMS PANI/MWCNT/PDMS MWCNTs-PANI-PDMS Two-electrode 1 0.1 mA.cm-2 Two-electrode Two-electrode 0.2 10 5 mV.s-1 mA.cm-2 - CNT – PANI - PDMS Two-electrode 1 SWCNT-PDMS Two-electrode 1 A.g-1 - 3D-G/PANI/pdms Two-electrode 1 A.g-1 G-PANI Two-electrode NRG//PANI MOF/PANI 44.13 A.g-1 12 308.4 13 - 54 12 - - 140 14 0.1 mA.cm-2 - 23 - 15 Two-electrode 0.25 mA.cm-2 - 14.5 - 16 Two-electrode mA.cm-2 - 28.1 - 17 0.1 Table S2 Parameters obtained from the equivalent electric circuit from EIS measurements. Sample Rs C1 R1 (ohm.cm-2) (mF.cm-2) (ohm.cm-2) W C2 ACNTA/PDMS 214 6.99 209.7 7.2 1.04 ACNTA-PANI/PDMS 153.3 8.34 72.46 5.5 20.23 (mF.cm-2) References 1 Q. Jiang, N. Kurra, M. Alhabeb, Y. Gogotsi and H. N. Alshareef, Adv. Energy Mater., 2018, 8, 1–10. 2 S. Y. Lee, J. Il Kim and S. J. Park, Energy, 2014, 78, 298–303. 3 S. Hussain, E. Kovacevic, R. Amade, J. Berndt, C. Pattyn, A. Dias, C. Boulmer-Leborgne, M. R. Ammar and E. BertranSerra, Electrochim. Acta, 2018, 268, 218–225. 4 M. Yu, Y. Zhang, Y. Zeng, M. S. Balogun, K. Mai, Z. Zhang, X. Lu and Y. Tong, Adv. Mater., 2014, 26, 4724–4729. 5 G. Wang, H. Wang, X. Lu, Y. Ling, M. Yu, T. Zhai, Y. Tong and Y. Li, Adv. Mater., 2014, 26, 2676–2682. 6 X. Liang, L. Zhao, Q. Wang, Y. Ma and D. Zhang, Nanoscale, 2018, 10, 22329–22334. 7 P. Avasthi, A. Kumar and V. Balakrishnan, ACS Appl. Nano Mater., 2019, 2, 1484–1495. 8 R. Zhang, K. Yan, A. Palumbo, J. Xu, S. Fu and E.-H. Yang, Nanotechnology, 2019, 30, 95401. 9 N. Li, T. Lv, Y. Yao, H. Li, K. Liu and T. Chen, J. Mater. Chem. A, 2017, 5, 3267–3273. 10 H. Lin, L. Li, J. Ren, Z. Cai, L. Qiu, Z. Yang and H. Peng, Sci. Rep., 2013, 3, 1–6. 11 T. Lv, Y. Yao, N. Li and T. Chen, Angew. Chemie - Int. Ed., 2016, 55, 9191–9195. 12 L. Li, Z. Lou, W. Han, D. Chen, K. Jiang and G. Shen, Adv. Mater. Technol., , DOI:10.1002/admt.201600282. 13 X. Chen, H. Lin, P. Chen, G. Guan, J. Deng and H. Peng, Adv. Mater., 2014, 26, 4444–4449. 14 K. Li, Y. Huang, J. Liu, M. Sarfraz, P. O. Agboola, I. Shakir and Y. Xu, J. Mater. Chem. A, 2018, 6, 1802–1808. 15 X. Zang, X. Li, M. Zhu, X. Li, Z. Zhen, Y. He, K. Wang, J. Wei, F. Kang and H. Zhu, Nanoscale, 2015, 7, 7318–7322. 16 L. Zhang, X. Qing, Z. Chen, J. Wang, G. Yang, Y. Qian, D. Liu, C. Chen, L. Wang and W. Lei, ACS Appl. Energy Mater., 2020, 3, 6845–6852. 17 A. P. M. Udayan, O. Sadak and S. Gunasekaran, ACS Appl. Energy Mater., 2020, 3, 12368–12377.