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1 Supporting Information for Novel Flexible Transparent Conductive Films with Enhanced Chemical and Electro- Mechanical Sustainability: TiO 2 Nanosheet-Ag Nanowire Hybrid Hiesang Sohn, 1,2 * Seyun Kim, 1 Weonho Shin, 2 Jong Min Lee, 2 Hyangsook Lee, 3 Dong-Jin Yun, 3 Kyoung-Seok Moon, 2 In Taek Han, 2 Chan Kwak 2 and Seong-Ju Hwang 4 1 Department of Chemical Engineering, Kwangwoon University, 20 Kwangwoon-Ro, Nowon- Gu, Seoul 01897, Korea 2 Inorganic Materials Laboratory, Materials Center, Samsung Advanced Institute of Technology, Samsung Electronics, 130 Samsung-ro, Yeongtong-gu, Suwon, , Korea 3 Analytical Engineering Group, Platform Technology Laboratory, Samsung Advanced Institute of Technology, Samsung Electronics, 130 Samsung-ro, Yeongtong-gu, Suwon, , Korea 4 Department of Chemistry and Nanoscience, Ewha Womans University, Seoul, 03760, Korea S-1
2 Corresponding Author: Hiesang Sohn, Tel: Address: Figure S1. (a) Digital photograph of TiO 2 nanosheet (NS) colloidal solution (left: Tyndall phenomenon observed in our TiO 2 NS solution, right: large scale production of TiO 2 NS solution in a scale of 300 ml) (b) UV-Vis spectra of TiO 2 NS. S-2
3 Figure S2. (a) Digital photograph of RuO 2 NS colloidal solution (b) UV-Vis spectra of RuO 2 NS (c) AFM image of RuO 2 NS for the measurement of NS thickness. S-3
4 Figure S3. Atomic force microscope (AFM) image of Ag NW (a) plane view, (b) 3D constructed image of (b), (c) AFM image analysis for the measurement of Ag NW thickness. Figure S4. (a) TEM images of TiO 2 NS deposited on Cu TEM grid, (b) magnified image of TiO 2 NS in (a), (c) high-resolution TEM images of TiO 2 NS obtained from (b) (inset: SAED diffraction pattern). S-4
5 Figure S5. (a) AFM images of TiO 2 NS (b) AFM image analysis for the measurement of TiO 2 NS thickness. Figure S6. Schematic illustration on the effect of nanopressing on the TCF based on (a) Ag NW and (b) Ag NW-TiO 2 NS hybrid. S-5
6 Figure S7. Electronic images for RuO2 NS: TEM images for (a) dispersed RuO2 NS; (b) RuO2 NS (cross-section view); (c) SEM images of RuO2 NS deposited on PC substrate; (d) SEM images for RuO2 NS-Ag NW hybrid prepared on PC substrate. Figure S8. Change of sheet resistance (Rs) and transmittance (TT) with time for ZnO NS (a) Change of sheet resistance (b) change of optical transmittance. S-6
7 Figure S9. Comparison of resistivity change ( R/R 0 ) of various conductors (Ag NW and RuO 2 NS-Ag NW and TiO 2 NS-Ag NW hybrid) measured after 200K bending cycles at 6.7% strain. S-7
8 Figure S10. Plot of optical transmittance (%) vs. sheet resistance (R s, ohm/sq.) in comparison of previous studies and this work (Ag NW-TiO 2 NS hybrid TCF). Figure S11. Plot of bending strain (ε, %) vs. fractional resistivity change ( R/R 0 ) at various bending cycles (<1K, ~10K, ~40K, ~200K) in comparison of previous studies and this work (Ag NW/TiO 2 NS hybrid). (R1) (R2) Park, J. H.; Lee, D. Y.; Kim, Y.-H.; Kim, J. K.; Lee, J. H.; Park, J. H.; Lee, T.-W.; Cho, J. H. Flexible and Transparent Metallic Grid Electrodes Prepared by Evaporative Assembly. ACS Appl. Mater. Interfaces 2014, 6, Hsiao, S.-T.; Tien, H.-W.; Liao, W.-H.; Wang, Y.-S.; Li, S.-M.; MMa, C.-C.; Yu, Y.- H.; Chuang, W.-P. A Highly Electrically Conductive Graphene-Silver Nanowire Hybrid Nanomaterial for Transparent Conductive Films. J. Mater. Chem. C 2014, 2, S-8
9 (R3) (R4) (R5) (R6) (R7) (R8) (R9) Ho, X.; Lu, H.; Liu, W.; Tey, J. N.; Cheng, C. K.; Kok, E.; Wei, J. Electrical and Optical Properties of Hybrid Transparent Electrodes That Use Metal Grids and Graphene Films. J. Mater. Res. 2013, 28, a) Qiu, T.; Luo, B.; Liang, M.; Ning, J.; Wang, B.; Li, X.; Zhi, L. Hydrogen Reduced Graphene Oxide/Metal Grid Hybrid Film: Towards High Performance Transparent Conductive Electrode for Flexible Electrochromic Devices. Carbon 2015, 81, ; b) Dou, L.; Cui, F.; Yu, Y.; Khanarian, G.; Eaton, S. W.; Yang, Q.; Resasco, J.; Schildknecht, C.; Schierle-Arndt, K.; Yang, P. Solution-Processed Copper/Reduced- Graphene-Oxide Core/Shell Nanowire Transparent Conductors. ACS Nano 2016, 10, ; c) Yang, J.; Zhao, Y.; Song, L.; Liu, J.; Liu, L.; Zeng, B. Graphene/Metallic Network Hybrid Structure for High Performance Transparent Electrode. Technical Digest th Inter. Vac. Nanoelectron. Conference. Lai, Y.-T.; Tai, N.-H. One-Step Process for High-Performance, Adhesive, Flexible Transparent Conductive Films Based on p Type Reduced Graphene Oxides and Silver Nanowires. ACS Appl. Mater. Interfaces 2015, 7, Lee, D.; Lee, H.; Ahn, Y.; Jeong, Y.; Lee, D.-Y.; Lee, Y. Highly Stable and Flexible Silver Nanowire-Graphene Hybrid Transparent Conducting Electrodes for Emerging Optoelectronic Devices. Nanoscale 2013, 5, Lee, D.; Lee, H.; Ahn, Y.; Lee, Y. High-Performance Flexible Transparent Conductive Film based on Graphene/AgNW/Graphene Sandwich Structure. Carbon 2015, 81, Liu, Y.; Chang, Q.; Huang, L. Transparent, Flexible Conducting Graphene Hybrid Films with a Subpercolating Network of Silver Nanowires. J. Mater. Chem. C 2013, 1, Moon, I. K.; Kim, J. I.; Lee, H.; Hur, K.; Kim, W. C.; Lee, H. 2D Graphene Oxide Nanosheets as an Adhesive Over-Coating Layer for Flexible Transparent Conductive Electrodes. Sci. Rep. 2013, 3, (R10) Kim, J.; Lim, J. W.; Mota, F. M.; Lee, J.-E.; Boppella, R.; Lim, K. Y.; Kim, K.; Choi, W. K.; Kim, D. H. Reduced Graphene Oxide Wrapped Core-Shell Metal Nanowires as Promising Flexible Transparent Conductive Electrodes with Enhanced Stability. Nanoscale 2016, 8, (R11) Liang, J.; Li, L.; Tong, K.; Ren, Z.; Hu, W.; Niu, X.; Chen, Y.; Pei, Q. Silver Nanowire Percolation Network Soldered with Graphene Oxide at Room Temperature and Its Application for Fully Stretchable Polymer Light-Emitting Diodes. ACS Nano 2014, 8, (R12) Sun, Q.; Lee, S. J.; Kang, H.; Gim, Y.; Park, H. S.; Cho, J. H. Positively-charged Reduced Graphene Oxide as an Adhesion Promoter for Highly-stable Silver Nanowire Film. Nanoscale 2015, 7, S-9
10 (R13) Hwang, B.; Park, M.; Kim, T.; Han, S. M. Effect of RGO deposition on chemical and mechanical reliability of Ag nanowire flexible transparent electrode. RSC Adv. 2016, 6, (R14) Qiu, T.; Luo, B.; Liang, M.; Ning, J.; Wang, B.; Li, X.; Zhi, L. Hydrogen reduced graphene oxide/metal grid hybrid film: towards high performance transparent conductive electrode for flexible electrochromic devices. Carbon 2015, 81, (R15) Wang, B.-Y.; Lee, E.-S.; Oh, Y.-J.; Kang, H. W. A silver nanowire mesh overcoated protection layer with graphene oxide as a transparent electrode for flexible organic solar cells. RSC Adv. 2017, 7, (R16) Dong, H.; Wu, Z.; Jiang, Y.; Liu, W.; Li, X.; Jiao, B.; Abbas, W.; Hou, X. A Flexible and Thin Graphene/Silver Nanowires/Polymer Hybrid Transparent Electrode for Optoelectronic Devices. ACS Appl. Mater. Interfaces 2016, 8, (R17) Kim, S.; Kim, S. Y.; Kim, J.; Kim, J. H. Highly Reliable AgNW/PEDOT:PSS Hybrid Films: Efficient Methods for Enhancing Transparency and Lowering Resistance and Haziness. J. Mater. Chem. C 2014, 2, (R18) Chu, C. R.; Lee, C.; Koo, J.; Lee, H. M. Fabrication of Sintering-free Flexible Copper Nanowire/Polymer Composite Transparent Electrodes with Enhanced Chemical and Mechanical Stability. Nano Res. 2016, 9, (R19) Yun, H. J.; Kim, S. J.; Hwang, J. H.; Shim, Y. S.; Jung, S.-G.; Park, Y. W.; Ju, B.-K. Silver Nanowire-IZO-Conducting Polymer Hybrids for Flexible and Transparent Conductive Electrodes for Organic Light-Emitting Diodes. Sci. Rep. 2016, 6, (R20) Zou, J.; Yip, H.-L.; Hau, S. K.; Jen, A. K.-Y. Metal Grid/Conducting Polymer Hybrid Transparent Electrode for Inverted Polymer Solar Cells. Appl. Phys. Lett. 2010, 96, (R21) Im, H.-G.; Jung, S.-H.; Jin, J.; Lee, D.; Lee, J.; Lee, D.; Lee, J.-Y.; Kim, I.-D.; Bae, B.-S. Flexible Transparent Conducting Hybrid Film Using a Surface-Embedded Copper Nanowire Network: A Highly Oxidation-Resistant Copper Nanowire Electrode for Flexible Optoelectronics. ACS Nano 2014, 8, (R22) Kang, H.; Jung, S.; Jeong, S.; Kim, G.; Lee, K. Polymer-metal hybrid transparent electrodes for flexible electronics. Nature Commun. 2015, 6, (R23) Narayanan, S.; Hajzus, J. R.; Treacy, C. E.; Bockstaller, M. R.; Porter, L. M. Polymer Embedded Silver-Nanowire Network Structures - A Platform for the Facile Fabrication of Flexible Transparent Conductors. ECS J. Solid State Sci. Tech. 2014, 3, P363-P369. (R24) Xiong, W.; Liu, H.; Chen, Y.; Zheng, M.; Zhao, Y.; Kong, X.; Wang, Y.; Zhang, X.; Kong, X.; Wang, P.; Jiang, L. Highly Conductive, Air-Stable Silver Nanowire@Iongel Composite Films toward Flexible Transparent Electrodes. Adv. Mater. 2016, 28, S-10
11 (R25) Liu, Y.-S.; Feng, J.; Ou, X.-L.; Cui, H.-F.; Xu, M.; Sun, H.-B. Ultrasmooth, highly conductive and transparent PEDOT:PSS/silver nanowire composite electrode for flexible organic light-emitting devices. Org. Electron. 2016, 31, (R26) Hwang, B.; An, C.-H.; Becker, S. Highly robust Ag nanowire flexible transparent electrode with UV-curable polyurethane-based overcoating layer. Mater. Des. 2017, 129, (R27) Tokuno, T.; Nogi, M.; Jiu, J.; Suganuma, K. Hybrid Transparent Electrodes of Silver Nanowires and Carbon Nanotubes: a Low-temperature Solution Process. Nanoscale Res. Lett. 2012, 7, (R28) Jing, M.-X.; Han, C.; Li, M.; Shen, X.-Q. High Performance of Carbon Nanotubes/Silver Nanowires-PET Hybrid Flexible Transparent Conductive Films via Facile Pressing-Transfer Technique. Nano. Res. Lett. 2014, 9, (R29) Xu, X.; Zhou, J.; Jiang, L.; Lubineau, G.; Ng, T.; Ooi, B. S.; Liao, H.-Y.; Shen, C.; Chen, L.; Zhu, J. Y.; Highly Transparent, Low-Haze, Hybrid Cellulose Nanopaper as Electrodes for Flexible Electronics. Nanoscale 2016, 8, (R30) Lee, P.; Ham, J.; Lee, J.; Hong, S.; Han, S.; Suh, Y. D.; Lee, S. E.; Yeo, J.; Lee, S. S.; Lee, D.; Ko, S. H. Highly Stretchable or Transparent Conductor Fabrication by a Hierarchical Multiscale Hybrid Nanocomposite. Adv. Funct. Mater. 2014, 24, (R31) Pillai, S. K. R.; Wang, J.; Wang, Y.; Sk, M. M.; Prakoso, A. B.; Chan-Park, R. M. B. Totally embedded hybrid thin films of carbon nanotubes and silver nanowires as flat homogenous flexible transparent conductors. Sci. Rep. 2016, 6, (R32) Huang, G.-W.; Xiao, H.-M.; Fu, S.-Y. Paper-based silver-nanowire electronic circuits with outstanding electrical conductivity and extreme bending stability. Nanoscale 2014, 6, (R33) Hwang, B.; Li, X.; Kim, S. H.; Lim, S. Effect of carbon nanotube addition on mechanical reliability of Ag nanowire network. Mater. Lett. 2017, 198, (R34) Hwang, B.; An, Y.; Lee, H.; Lee, E.; Becker, S.; Kim, Y.-H.; Kim, H. Highly Flexible and Transparent Ag Nanowire Electrode Encapsulated with Ultra-Thin Al 2 O 3 : Thermal, Ambient, and Mechanical Stabilities. Sci. Rep. 2017, 7, (R35) Wang, C.-T.; Ting, C.-C.; Kao, P.-C.; Li, S.-R.; Chu, S.-Y. Enhanced optical, electrical, and mechanical characteristics of ZnO/Ag grids/zno flexible transparent electrodes. J. Appl. Phys. 2017, 122, (R36) Han, J.; Yuan, S.; Liu, L.; Qiu, X.; Gong, H.; Yang, X.; Li, C.; Hao, Y.; Cao, B. Fully indium-free flexible Ag nanowires/zno:f composite transparent conductive electrodes with high haze. J. Mater. Chem. A 2015, 3, (R37) Im, H.-G.; Jeong, S.; Jin, J.; Lee, J.; Youn, D.-Y.; Koo, W.-T.; Kang, S.-B.; Kim, H.- J.; Jang, J.; Lee, D.; Kim, H.-K.; Kim, I.-D.; Lee, J.-Y.; Bae, B.-S. Hybrid crystalline- S-11
12 ITO/metal nanowire mesh transparent electrodes and their application for highly flexible perovskite solar cells. NPG Asia Mater. 2016, 8, e282-e289. (R38) Kim, A.; Won, Y.; Woo, K.; Kim, C.-H.; Moon, J. Highly Transparent Low Resistance ZnO/Ag Nanowire/ZnO Composite Electrode for Thin Film Solar Cells. ACS Nano 2013, 7, (R39) Huang, Q.; Shen, W.; Fang, X.; Chen, G.; Yang, Y.; Huang, J.; Tan, R.; Song, W. Highly Thermostable, Flexible, Transparent, and Conductive Films on Polyimide Substrate with an AZO/AgNW/AZO Structure. ACS Appl. Mater. Interfaces 2015, 7, (R40) Xu, Q.; Shen, W.; Huang, Q.; Yang, Y.; Tan, R.; Zhu, K.; Dai, N.; Song, W. Flexible transparent conductive films on PET substrates with an AZO/AgNW/AZO sandwich structure. J. Mater. Chem. C 2014, 2, (R41) Chang, J.-H.; Chiang, K.-M.; Kang, H.-W.; Chi, W.-J.; Chang, J.-H.; Wu, C.-I.; Lin, H.-W. Solution-Processed Molybdenum Oxide Treated Silver Nanowire Network: A Highly Conductive Transparent Conducting Electrode with Superior Mechanical and Hole Injection Properties. Nanoscale 2015, 7, S-12
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