Planar Supercapacitors with Buckled Carbon Nanotube. /Mn-Mo Mixed Oxide Electrodes and Air-Stable Organic Electrolyte

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1 [ Supporting Information ] Skin-Like, Dynamically Stretchale, Planar Supercapacitors with Buckled Caron Nanotue /Mn-Mo Mixed Oxide Electrodes and Air-Stale Organic Electrolyte Geumee Lee, Jung Wook Kim, Heun Park, Jae Yoon Lee, Hanchan Lee, Changhoon Song, Sang Woo Jin, Kayeon Keum, Chul-Ho Lee, and Jeong Sook Ha *,, KU-KIST Graduate School of Converging Science and Technology, Korea University, 145 Anam-ro, Seonguk-gu, Seoul, 2841, Repulic of Korea Department of Chemical and Biological Engineering, Korea University, 145 Anam-ro, Seonguk-gu, Seoul, 2841, Repulic of Korea Corresponding author * jeongsha@korea.ac.kr (Jeong Sook Ha) 1

2 a Stress (MPa) Nonporous Porous Transmittance (%) Nonporous Porous Contact angle ( o ) c Porous Nonporous Strain (%) Wavelength (nm) Figure S1. Comparison of porous and nonporous elastomeric sustrates. (a) Strain-stress curves. () Transmittance spectra. (c) Water contact angles. a Figure S2. (a) A schematic illustration for measuring the resistance change of the uckled electrode. () Definition of applied strain onto a uckled electrode. 2

3 2 mm 3 mm 12 mm 2 mm 8 mm 8 mm 5% 3 mm 12 mm Width 33 µm Interspace 2 µm Biaxial Stretching Width 5 µm Interspace 3 µm Figure S3. Dimensions of a SPS efore and after 5% iaxial stretching. a d = 5 mm Figure S4. Photographs of a SPS (a) wrapped around a glass rod with a diameter of 5 mm and () a stretched SPS. Inset indicates the thickness of a porous sustrate, ~27 μm. 3

4 a cycle 9 cycles 18 cycles 27 cycles 36 cycles 2 mvs cycle 9 cycles 18 cycles 27 cycles 36 cycles 2 mvs Figure S5. CV curves during 36 electrodeposition cycles in 2 mm MnSO 4 solutions (a) with and () without 2 mm Na 2MoO 4 at a scan rate of 2 mvs mm MoO mm Mn 2+ /2 mm MoO mvs Figure S6. CV curves for the 36 th electrodeposition cycle taken in 2 mm Na 2MoO 4 (lack) and 2 mm MnSO 4/2 mm Na 2MoO 4 (red) solutions, respectively. 4

5 9 cycles 18 cycles 54 cycles 72 cycles Figure S7. SEM images of Mn/Mo mixed oxide electrodes created with various numer of deposition cycle. All scale ars are 2 µm. Loading mass ( gcm -2 ) Deposition cycle F(kHz) Figure S8. The loading masses of Mn/Mo mixed oxide as a function of the numer of deposition cycles. 5

6 Areal capacitance (mfcm -2 ) Scan rate (mvs -1 ) 9 cls 18 cls 36 cls 54 cls 72 cls Figure S9. Dependence of areal capacitances on the scan rate from 1 to 3 mvs -1 for the Mn/Mo mixed oxide prepared with various deposition cycles mvs -1 Figure S1. CV curves taken for four different Mn/Mo mixed oxide electrodes at a scan rate of 5 mvs -1. 6

7 Areal capacitance (mfcm -2 ) a Vs -1.3 Vs -1.5 Vs -1.1 Vs -1.2 Vs -1.3 Vs Time (s).1 macm -2.3 macm -2.5 macm -2.7 macm macm -2 c -Z Im ( ) Z Im ( ) khz to.1 Hz Z re ( ) Z re ( ) Figure S11. Pseudocapacitive ehavior of a Mn/Mo@MWCNT composite electrode via threeelectrode measurements in.5 M Na 2SO 4. (a) CV curves at various scan rates of.1-.3 Vs -1. () GCD curves at current densities from.1 to 1. macm -2. (c) Nyquist plot taken over the frequency range of 5 khz-.1 Hz. a c MWCNT Mn/Mo@MWCNT 5 mvs macm -2 MWCNT Mn/Mo@MWCNT Time (s) MWCNT Mn/Mo@MWCNT Figure S12. Electrochemical performance of MWCNT (lack) and Mn/Mo@MWCNT (red) electrodes via three-electrode measurements in.5 M Na 2SO 4. (a) CV curves at a scan rate of 5 mvs -1. () GCD curves at a current density of.1 macm -2. (c) Areal capacitance as a function of current density from.1 to 1. macm -2. 7

8 5 4 Initial 1 month 2 months 4 months -Z Im (k ) ESR ( ) Elapsed time (month) Re (k ) Figure S13. Nyquist plots of a symmetric planar cell (Au/GPE/Au) with elapsed time in amient air for 4 months. The inset shows the change in the equivalent series resistance (ESR) ADN SN Intentisy (a.u.) LiTFSI PMMA GPE Raman shift (cm -1 ) Figure S14. Raman spectra in the frequency region of 6-16 cm -1 taken from adiponitrile (ADN), succinonitrile (SN), lithium is(trifluoromethanesulfonyl)imide (LiTFSI), poly(methylmethacrylate) (PMMA) and gel polymer electrolyte (GPE). 8

9 Voltage (V) macm macm -2.5 macm Time (hr) Figure S15. Self-discharge curves of a SPS with Mn/Mo@MWCNT electrodes and ADN/SN/LiTFSI/PMMA electrolyte. Normalized capacitance (C/C ) Elapsed time (d) Figure S16. Capacitance retention of a SPS with elapsed time in amient air. 9

10 a w/ PMMA w/o PMMA Gel Liquid Figure S17. Photographs taken from the organic electrolyte on a sustrate made with and without PMMA. (a) Before and () after tilting the sustrate. 1

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