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SCIENCE CHINA Materials, Volume 62, Issue 7: 995-1004(2019) https://doi.org/10.1007/s40843-018-9402-1

1-D polymer ternary composites: Understanding materials interaction, percolation behaviors and mechanism toward ultra-high stretchable and super-sensitive strain sensors

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  • ReceivedDec 17, 2018
  • AcceptedFeb 11, 2019
  • PublishedMar 4, 2019

Abstract

A series of 1-D polymer ternary composites based on poly(styrene-butadiene-styrene) (SBS)/carbon nanotubes (CNTs)/few-layer graphene (FLG) conductive fibers (SCGFs) were prepared via wet-spinning. Employed as ultra-high stretchable and super-sensitive strain sensors, the ternary composite fiber materials’ interaction, percolation behaviors and mechanism were systematically explored. The resultant SCGFs-based strain sensors simultaneously exhibited high sensitivity, superior stretchability (with a gauge factor of 5,467 under 600% deformation) and excellent durability under different test conditions due to excellent flexibility of SBS, the synergistic effect of hybrid conductive nanofibers and the strong π-π interaction. Besides, the conductive networks in SBS matrix were greatly affected by the mass ratio of CNTs and FLG, and thus the piezoresistive performances of the strain sensors could be controlled by changing the content of hybrid conductive fillers. Especially, the SCGFs with 0.30 wt.% CNTs (equal to their percolation threshold 0.30 wt.%) and 2.7 wt.% FLG demonstrated the highest sensitivity owing to the bridge effect of FLG between adjacent CNTs. Whereas, the SCGFs with 1.0 wt.% CNTs (higher than their percolation threshold) and 2.0 wt.% FLG showed the maximum strain detection range (600%) due to the welding connection caused by FLG between the contiguous CNTs. To evaluate the fabricated sensors, the tensile and the cyclic mechanical recovery properties of SCGFs were tested and analyzed. Additionally, a theoretical piezoresistive mechanism of the ternary composite fiber was investigated by the evolution of conductive networks according to tunneling theory.


Funded by

the Fundamental Research Funds for the Central Universities(2232018D3-03,2232018A3-01)

the Program for Changjiang Scholars and Innovative Research Team in University(IRT16R13)

the National Natural Science Foundation of China(51603033)

the Science and Technology Commission of Shanghai Municipality(16JC1400700)

the Innovation Program of Shanghai Municipal Education Commission(2017-01-07-00-03-E00055)


Acknowledgment

This work was supported by the Fundamental Research Funds for the Central Universities (2232018D3-03 and 2232018A3-01), the Program for Changjiang Scholars and Innovative Research Team in University (IRT16R13), the National Natural Science Foundation of China (51603033), the Science and Technology Commission of Shanghai Municipality (16JC1400700) and the Innovation Program of Shanghai Municipal Education Commission (2017-01-07-00-03-E00055).


Interest statement

The authors declare no conflict of interest.


Contributions statement

Zhu M and Xiang H supervised the project. Yu S designed and performed the experiments, analyzed the data and wrote the manuscript with support from Wang X and Tebyetekerwa M. All authors contributed to the general discussion.


Author information

Senlong Yu is now a PhD candidate in Prof. Meifang Zhu’s group at the College of Materials Science and Engineering, Donghua University. His current research focuses on the smart fiber materials.


Hengxue Xiang is an assistant research fellow of Donghua University. He obtained his PhD at the College of Materials Science and Engineering, Donghua University. His research focuses on the fiber formation of bio-based fibers and intelligent fibers.


Meifang Zhu is a professor at the College of Materials Science and Engineering, Donghua University. Her research mainly focuses on polymer fiber and nanocomposite functional materials, application and key technology research of organic/inorganic nano hybrid materials.


Supplement

Supplementary information

Supporting data are available in the online version of the paper.


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  • Figure 1

    Cross-sectional SEM images of SCGFs: (a) SBS/0.3C/2.7G, (b) SBS/0.5C/2.5G, (c) SBS/1C/2G, (d–f) are the higher magnification of (a–c), respectively.

  • Figure 2

    (a) Stress-strain curves of SCGFs with different mass ratios of CNTs to FLG. (b) Mechanical properties of the SCGFs.

  • Figure 3

    (a) Stress-strain curves of SBS/1C/2G composite fibers in cyclic elastic tests with growing maximal strain from 50%~600%. (b) Elastic recovery of SCGFs during cyclic stretching-releasing tests as a function of growing maximum strain. (c) Mechanical hysteresis of 50% strain for 5 cycles of SBS/1C/2G fiber. (d) Mechanical hysteresis for 50%, 100%, 200%, 400% and 600% strain of SBS/1C/2G fibers.

  • Figure 4

    (a, b) ΔR/R0 of SCGFs as a function of applied strain. (c) GF of SCGFs as a function of applied strain. (d) Comparison of the performance of the SCGFs sensor with that of recently reported flexible strain sensors. Note: ΔR/R0 and GFs of (b–d) are in logarithmic coordinates.

  • Figure 5

    Schematic illustration of the conductive network consisting of CNTs and FLG before and after stretching for SCGFs with CNTs contents below and above 0.30 wt.%.

  • Figure 6

    (a) The dynamic strain sensing behaviors of SCGFs under cyclic stretching and releasing at a strain of 0–50% (Note: The ΔR/R0 is in logarithmic coordinates). (b) The representation of where recovery ratio (D/P) and amplitude are derived. (c) The D/P of conductive network and amplitude of ΔR/R0 peak during dynamic stretching.

  • Figure 7

    (a) The dynamic strain sensing behavior of SBS/1C/2G fiber with a cyclic loading-unloading of 100%, 200%, 300%, 400% and 500%. (b) The representation of where recovery ratio (D/P) and amplitude are derived. (c) The D/P of conductive network and amplitude ΔR/R0 peak during dynamic stretching. Note: The ΔR/R0 is in logarithmic coordinates.

  • Figure 8

    Effect of strain rate on the dynamic sensing performance of SBS/1C/2G composite fibers.

  • Figure 9

    Experimental ΔR/R0 as a function of the applied strain and the fitted curve for the SBS/1C/2G composite fibers.

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