A strain sensor was prepared by reinforcing acrylonitrile butadiene rubber (NBR)-5 parts per hundred of rubber (phr) carbon black (CBH) separately with small concentration (∼0.1phr) of reduced graphene oxide (GL), multi-walled, and carbon nanotube (NTL) via a combination of conventional solution and solid processing techniques. The interactions and the electronic properties among carbon based fillers NT, CB, G and their synergy effects (NBR-CBH-GL and NBR-CBH-NTL) were investigated by using density functional theory (DFT) modeling approach. The DFT predictions were in correspondence with the experimental results. The optimum design (NBR-CBH-GL) was found to show high curing, mechanical and improved electrical properties. On account of strain sensing performance, NBR-CBH-GL exhibited high gauge factor (GF) ∼105 at 0–40% strain, which was over 900% than NBR-CBH (GF ∼104 at 0–30% strain) and the highest reported so far. This was explained by the breaking of CB networks caused by tight NBR-G structures on straining, leading to high electrical resistance. The NBR-CBH-GL also demonstrated high stability and repeatability in the cyclic loading. In terms of applications, NBR-CBH-GL exhibited high capability for vibration detections and wearable sensing, especially for detection of human bodily motions like speeches, facial deformations, bending, and relaxation of the fingers.
YinGHuNKarubeY, et al.A carbon nanotube/polymer strain sensor with linear and anti-symmetric piezoresistivity. J Compos Mater2011; 45(12): 1315–1323.
2.
XuWAllenMG. Fabrication of patterned carbon nanotube (CNT)/elastomer bilayer material and its utilization as force sensors, In AllenMG (eds). Solid-State Sensors, Actuators and Microsystems Conference. Denver, CO, 21-25, June 2009.
3.
LohKJLynchJPShimBS, et al.Tailoring piezoresistive sensitivity of multilayer carbon nanotube composite strain sensors. J Intell Mater Syst Structures2008; 19(7): 747–764.
4.
LuhengWTianhuaiDPengW. Influence of carbon black concentration on piezoresistivity for carbon-black-filled silicone rubber composite. Carbon2009; 47(14): 3151–3157.
5.
WangLMaFShiQ, et al.Study on compressive resistance creep and recovery of flexible pressure sensitive material based on carbon black filled silicone rubber composite. Sensors Actuators A: Phys2011; 165(2): 207–215.
6.
ZhouBLiCLiuZ, et al.A highly sensitive and flexible strain sensor based on dopamine-modified electrospun styrene-ethylene-butylene-styrene block copolymer yarns and multi walled carbon nanotubes. Polymers (Basel)2022; 14(15): 11.
7.
GarciaJRO’SuilleabhainDKaurH, et al.A simple model relating gauge factor to filler loading in nanocomposite strain sensors. ACS Appl Nano Mater2021; 4(3): 2876–2886.
8.
LiuHGaoHHuG. Highly sensitive natural rubber/pristine graphene strain sensor prepared by a simple method. Composites B: Eng2019; 171: 138–145.
9.
DaiHThostensonETSchumacherT. Processing and characterization of a novel distributed strain sensor using carbon nanotube-based nonwoven composites. Sensors2015; 15(7): 17728–17747.
10.
HuNKarubeYAraiM, et al.Investigation on sensitivity of a polymer/carbon nanotube composite strain sensor. Carbon2010; 48(3): 680–687.
11.
Shuai ChenZLChenDChenZ, et al.Highly flexible strain sensor based on ZnO nanowires and P(VDF-TrFE) fibers for wearable electronic device. Sci China Mater2016; 59.
12.
YamadaTHayamizuYYamamotoY, et al.A stretchable carbon nanotube strain sensor for human-motion detection. Nat Nano2011; 6(5): 296–301.
13.
TadakaluruSThongsuwanWSingjaiP. Stretchable and flexible high-strain sensors made using carbon nanotubes and graphite films on natural rubber. Sensors2014; 14(1): 868–876.
14.
BolandCSKhanUBackesC, et al.Sensitive, high-strain, high-rate bodily motion sensors based on graphene-rubber composites. ACS Nano2014; 8(9): 8819–8830.
15.
TungTTKarunagaranRTranDNH, et al.Engineering of graphene/epoxy nanocomposites with improved distribution of graphene nanosheets for advanced piezo-resistive mechanical sensing. J Mater Chem C2016; 4(16): 3422–3430.
16.
QiuAAakyiirMWangR, et al.Stretchable and calibratable graphene sensors for accurate strain measurement. Mater Adv2020; 1(2): 235–243.
17.
KurianAMohanVBBhattacharyyaD. Embedded large strain sensors with graphene-carbon black-silicone rubber composites. Sensors Actuators A Phys2018; 282: 11.
18.
SongPWangGZhangY. Preparation and performance of graphene/carbon black silicone rubber composites used for highly sensitive and flexible strain sensors. Sensors Actuators A: Phys2021; 323: 112659.
19.
CaiWHuangYWangD, et al.Piezoresistive behavior of graphene nanoplatelets/carbon black/silicone rubber nanocomposite. J Appl Polym Sci2014; 131(3): 11.
20.
SongPSongJZhangY. Stretchable conductor based on carbon nanotube/carbon black silicone rubber nanocomposites with highly mechanical, electrical properties and strain sensitivity. Composites Part B: Eng2020; 191: 107979.
21.
CataldoFUrsiniOAngeliniG. MWCNTs elastomer nanocomposite, part 1: the addition of MWCNTs to a natural rubber‐based carbon black‐filled rubber compound. Fullerenes, Nanotubes and Carbon Nanostructures2009; 17(1): 38–54.
22.
WalterPPodsiadłyBZychM, et al.CNT/graphite/SBS conductive fibers for strain sensing in wearable telerehabilitation devices. Sensors2022; 22(3): 800.
23.
ZhuW-BXueS-SZhangH, et al.Direct ink writing of a graphene/CNT/silicone composite strain sensor with a near-zero temperature coefficient of resistance. J Mater Chem C2022; 10(21): 8226–8233.
24.
MensahBKumarDLimD-K, et al.Preparation and properties of acrylonitrile–butadiene rubber–graphene nanocomposites. J Appl Polym Sci2015; 132(36): 11.
25.
MensahBKimSArepalliS, et al.A study of graphene oxide-reinforced rubber nanocomposite. J Appl Polym Sci2014; 131(16): 11.
26.
FloryPJRehnerJ. Statistical mechanics of cross‐linked polymer networks II. Swelling J Chem Phys1943; 11(11): 521–526.
27.
BristowGMWatsonWF. Cohesive energy densities of polymers. Part 1.-cohesive energy densities of rubbers by swelling measurements. Trans Faraday Soc1958; 54(0): 1731–1741.
28.
NajithaSPredeepP. Electrical and optical properties of nitrile rubber modified by ion implantation. AIP Conf Proc2014; 1620: 11.
29.
AbidSPIslamSSMishraP, et al.Reduced graphene oxide (rGO) based wideband optical sensor and the role of temperature, defect states and quantum efficiency. Scientific Reports2018; 8(1): 3537.
30.
BrodieBC. On the atomic weight of graphite. Philos Trans R Soc Lond1859; 149: 249–259.
MensahBKimHGLeeJ-H, et al.Carbon nanotube-reinforced elastomeric nanocomposites: a review. Int J Smart Nano Mater2015; 6(4): 211–238.
33.
KimS-MKimK-J. Effects of accelerators on the vulcanization properties of silica vs. carbon black filled natural rubber compounds. Polym Korea2013; 37(3): 269–275.
34.
MensahBGuptaKCKangG, et al.A comparative study on vulcanization behavior of acrylonitrile-butadiene rubber reinforced with graphene oxide and reduced graphene oxide as fillers. Polym Test2019; 76: 127–137.
35.
AliMChughJPHaghighatS. Effects of silica on the cure properties of some compounds of styrene-butadiene rubber. Iranian Polym J2000; 9(2): 1026–1265.
36.
NahCLimJYSenguptaR, et al.Slipping of carbon nanotubes in a rubber matrix. Polym Int2011; 60(1): 42–44.
37.
NahCLimJYChoBH, et al.Reinforcing rubber with carbon nanotubes. J Appl Polym Sci2010; 118.
38.
FröhlichJNiedermeierWLuginslandHD. The effect of filler–filler and filler–elastomer interaction on rubber reinforcement. Composites A: Appl Sci Manufacturing2005; 36(4): 449–460.
39.
KucherskiiAM. Hysteresis losses in carbon-black-filled rubbers under small and large elongations. Polym Test2005; 24(6): 733–738.
40.
D’AmbrosioPDe TommasiDFerriD, et al.A phenomenological model for healing and hysteresis in rubber-like materials. Int J Eng Sci2008; 46(4): 293–305.
41.
LiZ-YSongY-HZhengQ. Payne effect and weak overshoot in rubber nanocomposites. Chin J Polym Sci2022; 40(1): 85–92.
42.
MensahBAgyei-TuffourBNyanksonE, et al.Preparation and characterization of rubber blends for industrial tire tread fabrication. Int J Polym Sci2018; 2018: 2473286.
43.
ShahriaryLAthawaleA. Graphene oxide synthesized by using modified hummers approach. Int J Renew Energ Environ Eng2014; 02(01): 11.
44.
MensahBGuptaKCKimH, et al.Graphene-reinforced elastomeric nanocomposites: A review. Polym Test2018; 68: 160–184.
45.
SalaehSBoiteuxGCassagnauP, et al.Conductive elastomer composites with low percolation threshold based on carbon black and epoxidized natural rubber. Polym Composites2018; 39(6): 1835–1844.
46.
DasAKasaliwalGRJurkR, et al.Rubber composites based on graphene nanoplatelets, expanded graphite, carbon nanotubes and their combination: a comparative study. Composites Sci Tech2012; 72(16): 1961–1967.
47.
YamaguchiKJJCBThomasAG. Electrical and mechanical behavior of filled elastomers. I. The effect of strain. J Polym Sci B: Polym Phys2003; 41(17): 2079–2089.
48.
HayichelaehCReuvekampLAEMDierkesWK, et al.Reinforcement of natural rubber by silica/silane in dependence of different amine types. Rubber Chem Tech2017; 90(4): 651–666.
49.
LuhrsCCDaskamCDGonzalezE, et al.Fabrication of a low density carbon fiber foam and its characterization as a strain gauge. Materials2014; 7(5): 3699–3714.
50.
NaHRLeeHJJeonJH, et al.Vertical graphene on flexible substrate, overcoming limits of crack-based resistive strain sensors. Npj Flexible Electro2022; 6(1): 2.
51.
HuangLWangHWuP, et al.Wearable flexible strain sensor based on three-dimensional wavy laser-induced graphene and silicone rubber. Sensors2020; 20(15): 4266.
52.
LiuYZhangDWangK, et al.A novel strain sensor based on graphene composite films with layered structure. Composites Part A: Appl Sci Manufacturing2016; 80: 95–103.
53.
AmjadiMYoonYJParkI. Ultra-stretchable and skin-mountable strain sensors using carbon nanotubes? Ecoflex nanocomposites. Nanotechnology2015; 26(37): 375501.
54.
RenT-LTianHXieD, et al.Flexible graphite-on-paper piezoresistive sensors. Sensors2012; 12(5): 6685–6694.
55.
LiuXMwangiMLiX, et al.Paper-based piezoresistive MEMS sensors. Lab A Chip2011; 11(13): 2189–2196.
56.
MullinsL. Softening of rubber by deformation. Rubber Chemistry Technology1969; 42(1): 339–362.
57.
PalazzoloA. Vibration theory and applications with finite elements and active vibration control. Wiley, 2016.
