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1 Supporting Information Novel Electrically-Conductive Porous PDMS/Carbon Nanofibre Composites for Deformable Strain-Sensors and Conductors Shuying Wu,, Jin Zhang, Raj B. Ladani, Anil R. Ravindran, Adrian P. Mouritz, Anthony J. Kinloch, and Chun H. Wang, * Sir Lawrence Wackett Aerospace Research Centre, School of Engineering, RMIT University, GPO Box 2476, Melbourne, VIC 3001, Australia School of Mechanical and Manufacturing Engineering, University of New South Wales, Sydney, NSW 2052, Australia Australian Future Fibres Research and Innovation Centre, Institute for Frontier Materials, Deakin University, VIC 3220, Australia Department of Mechanical Engineering, Imperial College London, London, SW7 2BX, UK * chun.h.wang@unsw.edu.au S-1

2 Stress (MPa) wt% 0.3 wt % 0.5 wt% 0.7 wt% 1.4 wt% 2.8 wt% Strain (%) Figure S1. The strain-stress curves for p-pdms/cnf nanocomposites containing different concentrations of CNFs. S-2

3 40 30 Specimen 1 Specimen 2 Specimen 3 R/R Strain (ε) 0.6 Figure S2. The relative resistance change versus strain under quasi-static loading from replicate specimens of p-pdms/cnf nanocomposites containing 0.1 wt% of CNFs. S-3

4 10 8 p-pdms/cnfs (0.3 wt%) 70% strain R/R Time (s) Figure S3. The relative resistance change over 10 cycles of loading-unloading (with a cyclic maximum applied strain of 70% and a minimum applied strain of 0%) of p-pdms/cnf nanocomposites containing 0.3 wt% of CNFs. S-4

5 Table S1. Summary of the sensing performance of recently reported strain sensors. Materials Stretchability (maximum operating strain) S-5 Gauge Factor Porous PDMS/CNFs 70% Linearity a Ref. Linear up to 70% b This work GA/PDMS 10% 61.3 Nonlinear (1) Conventional metallic strain gauge 5% 2 Linear (2) Silver nanowires/pdms 70% 2-14 Linear up to Graphene/nanocellulose paper 100% 7 Nonlinear (4) Fragmentized graphene foam/pdms 70% Linear (5) 40% Aligned CNTs-PDMS Two linear regions CNTs Ecoflex Linear (6) Graphene foam/pdms 16% 6.24 Nonlinear (7) Silver nanowires Ecoflex 50% 0.7 Linear (8) Graphene woven fabric/pdms 6% 1000 Nonlinear (9) Ultrathin graphene film/pdms 2% 1037 Nonlinear (10) Graphene-based thin film 1.8% 42 Linear (11) Pencil-trace graphite/flexible paper 0.6% Three linear regions Graphene/natural rubber 800% Linear up to 4% (13) Silver nanoparticle thin-film/pdms 20% 2.05 Not provided (14) ZnO piezoelectric fine-wires 1% 1250 Nonlinear (15) ZnO nanowires PDMS Linear (16) Carbon-black/PDMS composites 10% Two linear regions Silver nanowires PEDOT:PSS/PU 100% Nonlinear (18) a Linearity indicates, unless stated otherwise, being linear in R/R 0 versus L/L 0. b Linear up to 70% means, in the present work, linearity was seen in R/R 0 versus L/L 0 up to 20 to 30% strain but linearity in ln(r/r 0 ) versus ln(l/l 0 ) was recorded up to 70% strain. (3) (2) (12) (17)

6 References (1) Wu, S.; Ladani, R. B.; Zhang, J.; Ghorbani, K.; Zhang, X.; Mouritz, A. P.; Kinloch, A. J.; Wang, C. H. Strain Sensors with Adjustable Sensitivity by Tailoring the Microstructure of Graphene Aerogel/PDMS Nanocomposites. ACS Appl. Mater. Interfaces 2016, 8, (2) Yamada, T.; Hayamizu, Y.; Yamamoto, Y.; Yomogida, Y.; Izadi-Najafabadi, A.; Futaba, D. N.; Hata, K. A Stretchable Carbon Nanotube Strain Sensor for Human-Motion Detection. Nat. Nanotechnol. 2011, 6, (3) Amjadi, M.; Pichitpajongkit, A.; Lee, S.; Ryu, S.; Park, I. Highly Stretchable and Sensitive Strain Sensor Based on Silver Nanowire-Elastomer Nanocomposite. ACS Nano 2014, 8, (4) Yan, C. Y.; Wang, J. X.; Kang, W. B.; Cui, M. Q.; Wang, X.; Foo, C. Y.; Chee, K. J.; Lee, P. S. Highly Stretchable Piezoresistive Graphene-Nanocellulose Nanopaper for Strain Sensors. Adv. Mater. 2014, 26, (5) Jeong, Y. R.; Park, H.; Jin, S. W.; Hong, S. Y.; Lee, S.-S.; Ha, J. S. Highly Stretchable and Sensitive Strain Sensors Using Fragmentized Graphene Foam. Adv. Funct. Mater. 2015, 25, (6) Hwang, S.; Jeong, S. H. Stretchable Carbon Nanotube Conductors and Their Applications. Korean J. Chem. Eng. 2016, 33, (7) Xu, R.; Lu, Y.; Jiang, C.; Chen, J.; Mao, P.; Gao, G.; Zhang, L.; Wu, S. Facile Fabrication of Three- Dimensional Graphene Foam/Poly(dimethylsiloxane) Composites and Their Potential Application as Strain Sensor. ACS Appl. Mater. Interfaces 2014, 6, (8) Yao, S.; Zhu, Y. Wearable Multifunctional Sensors Using Printed Stretchable Conductors Made of Silver Nanowires. Nanoscale 2014, 6, (9) Li, X.; Zhang, R. J.; Yu, W. J.; Wang, K. L.; Wei, J. Q.; Wu, D. H.; Cao, A. Y.; Li, Z. H.; Cheng, Y.; Zheng, Q. S.; Ruoff, R. S.; Zhu, H. W. Stretchable and Highly Sensitive Graphene-on-Polymer Strain Sensors. Sci. Rep. 2012, 2, 6. (10) Li, X.; Yang, T.; Yang, Y.; Zhu, J.; Li, L.; Alam, F. E.; Li, X.; Wang, K.; Cheng, H.; Lin, C.-T.; Fang, Y.; Zhu, H. Large-Area Ultrathin Graphene Films by Single-Step Marangoni Self-Assembly for Highly Sensitive Strain Sensing Application. Adv. Funct. Mater. 2016, 26, (11) Hempel, M.; Nezich, D.; Kong, J.; Hofmann, M. A Novel Class of Strain Gauges Based on Layered Percolative Films of 2D Materials. Nano Lett. 2012, 12, (12) Liao, X.; Liao, Q.; Yan, X.; Liang, Q.; Si, H.; Li, M.; Wu, H.; Cao, S.; Zhang, Y. Flexible and Highly Sensitive Strain Sensors Fabricated by Pencil Drawn for Wearable Monitor. Adv. Funct. Mater. 2015, (13) Boland, C. S.; Khan, U.; Backes, C.; O Neill, A.; McCauley, J.; Duane, S.; Shanker, R.; Liu, Y.; Jurewicz, I.; Dalton, A. B.; Coleman, J. N. Sensitive, High-Strain, High-Rate Bodily Motion Sensors Based on Graphene Rubber Composites. ACS Nano 2014, 8, (14) Lee, J.; Kim, S.; Lee, J.; Yang, D.; Park, B. C.; Ryu, S.; Park, I. A Stretchable Strain Sensor Based on a Metal Nanoparticle Thin Film for Human Motion Detection. Nanoscale 2014, 6, (15) Zhou, J.; Gu, Y.; Fei, P.; Mai, W.; Gao, Y.; Yang, R.; Bao, G.; Wang, Z. L. Flexible Piezotronic Strain Sensor. Nano Lett. 2008, 8, (16) Xiao, X.; Yuan, L. Y.; Zhong, J. W.; Ding, T. P.; Liu, Y.; Cai, Z. X.; Rong, Y. G.; Han, H. W.; Zhou, J.; Wang, Z. L. High-Strain Sensors Based on ZnO Nanowire/Polystyrene Hybridized Flexible Films. Adv. Mater. 2011, 23, (17) Kong, J.-H.; Jang, N.-S.; Kim, S.-H.; Kim, J.-M. Simple and Rapid Micropatterning of Conductive Carbon Composites and Its Application to Elastic Strain Sensors. Carbon 2014, 77, (18) Hwang, B. U.; Lee, J. H.; Trung, T. Q.; Roh, E.; Kim, D. I.; Kim, S. W.; Lee, N. E. Transparent Stretchable Self-Powered Patchable Sensor Platform with Ultrasensitive Recognition of Human Activities. ACS Nano 2015, 9, S-6

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