Electronic Supplementary Information All-inkjet-printed .

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Electronic Supplementary Material (ESI) for Energy & Environmental Science.This journal is The Royal Society of Chemistry 2016Electronic Supplementary InformationAll-inkjet-printed, solid-state flexible supercapacitors on paperKeun-Ho Choi,a JongTae Yoo,ab Chang Kee Leec and Sang-Young Leea*aDepartmentof Energy Engineering, School of Energy and Chemical Engineering, UlsanNational Institute of Science and Technology (UNIST), Ulsan, 689-798, South Korea. E-mail:syleek@unist.ac.kr; Tel: 82-52-217-2948bSchoolof Energy and Chemical Engineering, Ulsan National Institute of Science andTechnology (UNIST), Ulsan, 689-798, South Korea.cKoreaPackaging Center, Korea Institute of Industrial Technology, Bucheon, Gyeonggi-do,421-742, South Korea.1

Fig. S1. Schematics and SEM images of the stepwise fabrication procedure of the CNFnanomat-based primer layer: (a) A4 paper, (b) inkjet-printed (wet-state) CNF layer depositedon A4 paper, (c) inkjet-printed CNF nanomat deposited onto A4 paper. The highly developednanoporous structure was generated after the solvent exchange between ethanol/acetonemixture and water.Fig. S2. 3D laser scanning microscope images of: (a) A4 paper (wetting substrate, Ra(surface roughness) 4.8 m) and (b) PET film (non-wetting substrate, Ra 0.2 m).Fig. S3. Viscosity of the electrode (SWNT/AC) inks as a function of shear rate, before/aftercentrifugation (at 10,000 rpm for 1 h).Fig. S4. SEM images of the Ag NWs: (a) before and (b) after sonication-driven scission.Fig. S5. Viscosity of Ag NW inks (containing short NWs, after sonication-driven scission) asa function of shear rate.Fig. S6. SEM images of a control sample (Ag NWs without SWNTs): (a) before and (b) afterUV irradiation.Fig. S7. FT-IR spectra showing the change of characteristic peaks assigned to C C doublebonds of ETPTA, before/after the UV crosslinking reaction.2

Fig. S8. Linear sweep voltammetry (LSV) profile of [BMIM][BF4]/ETPTA mixture (afterremoval of the residual water).Fig. S9. TGA profile (dynamic mode, heating rate 10 oC min-1 under nitrogen atmosphere)of the inkjet-printed ([BMIM][BF4]/ETPTA) solid-state electrolyte.Fig. S10. Effect of scan rates ( 1 - 200 mV s-1) on: (a) CV profiles and (b) coulombicefficiency of the inkjet-printed SC.Fig. S11. Ragone plot (i.e., specific energy density [Wh kg-1] vs. specific power density [Wkg-1]) of the inkjet-printed SC.Fig. S12. (a) Galvanostatic charge-discharge (GCD) profiles (at current density 0.2 mA cm2)of the inkjet-printed SCs showing IR drop. Galvanostatic GCD profiles (at current densities 1.0 – 10.0 mA cm-2) of the inkjet-printed SCs (b) with Ag NWs and (c) without Ag NWs.Fig. S13. Schematics and photographs of the inkjet-printed SCs: (a) 5 cells connected inseries and (b) 5 cells connected in parallel.Fig. S14. (a) Schematic of the inkjet-printed, letter (“BATTERY”)-shaped SC that wasseamlessly connected with the inkjet-printed electrical circuit. (b) Charge/discharge profilesof the inkjet-printed, letter (“BATTERY”)-shaped SC.Fig. S15. (a) Schematic of the inkjet-printed, traditional Korean “Taegeuk” symbol-like SCthat was aesthetically unitized with inkjet-printed electric circuit and other patterns. (b)Charge/discharge profiles of the inkjet-printed, “Taegeuk” symbol-like SC.3

Fig. S16. A schematic of the inkjet-printed SCs that were seamlessly connected via theinkjet-printed electric circuits to LED lamps in the inkjet-printed Korea map.Fig. S17. Photographs of the (a) temperature sensor and (b) Arduino board.Fig. S18. Video clips showing the operation of: (a) a blue LED lamp in the smart cup (forcold water ( 10 oC)) and (b) a red LED lamp in the smart cup (for hot water ( 80 oC)).4

Fig. S1. Schematics and SEM images of the stepwise fabrication procedure of the CNFnanomat-based primer layer: (a) A4 paper, (b) inkjet-printed (wet-state) CNF layer depositedon A4 paper, (c) inkjet-printed CNF nanomat deposited onto A4 paper. The highly developednanoporous structure was generated after the solvent exchange between ethanol/acetonemixture and water.5

Fig. S2. 3D laser scanning microscope images of: (a) A4 paper (wetting substrate, Ra(surface roughness) 4.8 m) and (b) PET film (non-wetting substrate, Ra 0.2 m).6

80Before CentrifugationAfter CentrifugationViscosity (cP)604020012345678910Shear Rate (s-1)Fig. S3. Viscosity of the electrode (SWNT/AC) inks as a function of shear rate, before/aftercentrifugation (at 10,000 rpm for 1 h).7

Fig. S4. SEM images of the Ag NWs: (a) before and (b) after sonication-driven scission.8

Viscosity (cP)102Ag NW Ink10110010-112345678910Shear Rate (s-1)Fig. S5. Viscosity of Ag NW inks (containing short NWs, after sonication-driven scission) asa function of shear rate.9

Fig. S6. SEM images of a control sample (Ag NWs without SWNTs): (a) before and (b) afterUV irradiation.10

Fig. S7. FT-IR spectra showing the change of characteristic peaks assigned to C C doublebonds of ETPTA, before/after UV crosslinking reaction.11

Current Density (mA cm-2)0.20.10.0-0.1-0.2-4-3-2-10123Voltage (V vs. Pt/Pt )Fig. S8. Linear sweep voltammetry (LSV) profile of [BMIM][BF4]/ETPTA mixture (afterremoval of the residual water).12

Fig. S9. TGA profile (dynamic mode, heating rate 10 oC min-1 under nitrogen atmosphere)of the inkjet-printed ([BMIM][BF4]/ETPTA) solid-state electrolyte.13

Fig. S10. Effect of scan rates ( 1 - 200 mV s-1) on: (a) CV profiles and (b) coulombicefficiency of the inkjet-printed SC.14

Specific Energy (Wh kg-1)103102Inkjet-printed supercapacitor (this work)Thin-film supercapacitor (Ref. 34)Thin-film supercapacitor (Ref. 37)10110010-1 110102103104105Specific Power (W kg-1)Fig. S11. Ragone plot (i.e., specific energy density [Wh kg-1] vs. specific power density [Wkg-1]) of the inkjet-printed SC.15

Fig. S12. (a) Galvanostatic charge-discharge (GCD) profiles (at current density 0.2 mA cm2) of the inkjet-printed SCs showing IR drop. Galvanostatic GCD profiles (at current densities 1.0 – 10.0 mA cm-2) of the inkjet-printed SCs (b) with Ag NWs and (c) without Ag NWs.16

Fig. S13. Schematics and photographs of the inkjet-printed SCs: (a) 5 cells connected inseries and (b) 5 cells connected in parallel.17

Fig. S14. (a) Schematic of the inkjet-printed, letter (“BATTERY”)-shaped SC that wasseamlessly connected with the inkjet-printed electrical circuit. (b) Charge/discharge profilesof the inkjet-printed, letter (“BATTERY”)-shaped SC.18

Fig. S15. (a) Schematic of the inkjet-printed, traditional Korean “Taegeuk” symbol-like SCthat was aesthetically unitized with the inkjet-printed electric circuit and other patterns. (b)Charge/discharge profiles of the inkjet-printed, “Taegeuk” symbol-like SC.19

Fig. S16. Schematic of the inkjet-printed SCs that were seamlessly connected via the inkjetprinted electric circuits to LED lamps in the inkjet-printed Korea map.20

Fig. S17. Photographs of the (a) temperature sensor and (b) Arduino board.21

Fig. S18. Video clips showing the operation of: (a) a blue LED lamp in the smart cup (forcold water ( 10 oC)) and (b) a red LED lamp in the smart cup (for hot water ( 80 oC)).22

inkjet-printed electric circuits to LED lamps in the inkjet-printed Korea map. Fig. S17. Photographs of the (a) temperature sensor and (b) Arduino board. Fig. S18. Video clips showing the operation of: (a) a blue LED lamp in the smart cup (for cold water ( 10 oC)) and (b) a red LED lamp in the smart cup (for hot water ( 80 oC)).

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