Liquid metal (LM) dielectric elastomers with high flexibility and excellent dielectric properties are ideal for flexible capacitive pressure sensors. However, the development of LM dielectric elastomers is hindered by the challenge of unavoidable percolation at high LM fill ratios. Inhomogeneous distribution is an effective strategy to manipulate the percolation threshold. Herein, thermoplastic polyurethane (TPU) fiber mats featuring a unique rapeseed-shaped structure were designed for high LM content filling (up to 90 vol%) and prepared with the aid of an electrospinning technique, in which LM was locally concentrated in the TPU fibers of the composite mats to form isolated clusters, leading to an incredible improvement in the percolation threshold surpassing our calculated theoretical prediction (>90 vol% vs. 83 vol%). The LM/TPU-Fiber mats are proven to be recyclable, temperature-insensitive, and waterproof, making them suitable for multiple usage environments. A flexible capacitive sensor prepared with LM/TPU-Fiber mats, capable of exceptional relative capacitance change (Max. ΔC/C0 = 6.32), an impressive pressure range of 0–550 kPa with a sensitivity of 55 MPa−1, and high cyclic stability (>6000 cycles). With these outstanding attributes, the sensor holds great promise for applications in intelligent sorting, pressure distribution monitoring, and human–machine interaction.
| [1] |
LiuQ, LiuY, ShiJ, LiuZ, WangQ, GuoCF. High-porosity foam-based iontronic pressure sensor with superhigh sensitivity of 9280 kPa−1. Nanomicro Lett., 2022.
|
| [2] |
LiR, Panahi-SarmadM, ChenT, WangA, XuR, XiaoX. Highly sensitive and flexible capacitive pressure sensor based on a dual-structured nanofiber membrane as the dielectric for attachable wearable electronics. ACS Appl Electron Mater, 2022, 4: 469
|
| [3] |
MannsfeldSCB, TeeBCK, StoltenbergRM, ChenCVHH, BarmanS, MuirBVO, SokolovAN, ReeseC, BaoZ. Highly sensitive flexible pressure sensors with microstructured rubber dielectric layers. Nat Mater, 2010, 9: 859
|
| [4] |
YangJ, TangD, AoJ, GhoshT, NeumannTV, ZhangD, PiskarevY, YuT, TruongVK, XieK, LaiYC, LiY, DickeyMD. Ultrasoft liquid metal elastomer foams with positive and negative piezopermittivity for tactile sensing. Adv Funct Mater, 2020, 30: 2002611
|
| [5] |
HuY, MajidiC. Dielectric elastomers with liquid metal and polydopamine-coated graphene oxide inclusions. ACS Appl Mater Interfaces, 2023, 15: 24769
|
| [6] |
PanC, MarkvickaEJ, MalakootiMH, YanJ, HuL, MatyjaszewskiK, MajidiC. A liquid-metal–elastomer nanocomposite for stretchable dielectric materials. Adv Mater, 2019, 31: 1900663
|
| [7] |
MaJ, LiuZ, NguyenQ-K, ZhangP. Lightweight soft conductive composites embedded with liquid metal fiber networks. Adv Funct Mater, 2023, 34: 2308128
|
| [8] |
HuangLJ, GengL, PengHX. Microstructurally inhomogeneous composites: Is a homogeneous reinforcement distribution optimal?. Prog Mater Sci, 2015, 71: 93
|
| [9] |
QinF, PengM, EstevezD, BrosseauC. Electromagnetic composites: from effective medium theories to metamaterials. J Appl Phys, 2022, 132101101
|
| [10] |
MatosMAS, TagarielliVL, PinhoST. On the electrical conductivity of composites with a polymeric matrix and a non-uniform concentration of carbon nanotubes. Compos Sci Technol, 2020, 188108003
|
| [11] |
LyuQ, PengB, XieZ, DuS, ZhangL, ZhuJ. Moist-Induced electricity generation by electrospun cellulose acetate membranes with optimized porous structures. ACS Appl Mater Interfaces, 2020, 12: 57373
|
| [12] |
ZhangX, FuQ, WangY, ZhaoH, HaoS, MaC, XuF, YangJ. Tough liquid-free ionic conductive elastomers with robust adhesion and self-healing properties for ionotronic devices. Adv Funct Mater, 2023, 34: 2307400
|
| [13] |
LuT, CuiJ, QuQ, WangY, ZhangJ, XiongR, MaW, HuangC. Multistructured electrospun nanofibers for air filtration: a review. ACS Appl Mater Interfaces, 2021, 13: 23293
|
| [14] |
LiuY, HeJ-H, YuJ-y, ZengH-m. Controlling numbers and sizes of beads in electrospun nanofibers. Polym Int, 2008, 57: 632
|
| [15] |
KhanMR, EakerCB, BowdenEF, DickeyMD. Giant and switchable surface activity of liquid metal via surface oxidation. P NATL A SCI, 2014, 111: 14047
|
| [16] |
DickeyMD. Stretchable and soft electronics using liquid metals. Adv Mater, 2017, 29: 1606425
|
| [17] |
UmIC, FangD, HsiaoBS, OkamotoA, ChuB. Electro-spinning and electro-blowing of hyaluronic acid. Biomacromol, 2004, 5: 1428
|
| [18] |
LiJ, ZhangD, YangT, YangS, YangX, ZhuH. Nanofibrous membrane of graphene oxide-in-polyacrylonitrile composite with low filtration resistance for the effective capture of PM2.5. J Membr Sci, 2018, 551: 85
|
| [19] |
HeH, WuM, ZhuJ, YangY, GeR, YuD-G. Engineered spindles of little molecules around electrospun nanofibers for biphasic drug release. Adv Fiber Mater, 2022, 4: 305
|
| [20] |
ZhouW, GongX, LiY, SiY, ZhangS, YuJ, DingB. Environmentally friendly waterborne polyurethane nanofibrous membranes by emulsion electrospinning for waterproof and breathable textiles. Chem Eng J, 2022, 427130925
|
| [21] |
JacksonN, StamF. Sloshing liquid-metal mass for widening the bandwidth of a vibration energy harvester. Sens Actuator A Phys, 2018, 284: 17
|
| [22] |
ZhangQ, LuH, YunG, GongL, ChenZ, JinS, DuH, JiangZ, LiW. A laminated gravity-driven liquid metal-doped hydrogel of unparalleled toughness and conductivity. Adv Funct Mater, 2023, 34: 2308113
|
| [23] |
YiS-Q, SunH, JinY-F, ZouK-K, LiJ, JiaL-C, YanD-X, LiZ-M. CNT-assisted design of stable liquid metal droplets for flexible multifunctional composites. Compos B Eng, 2022, 239109961
|
| [24] |
BuryE, KohAS. Multimodal deformation of liquid metal multimaterial composites as stretchable, dielectric materials for capacitive pressure sensing. ACS Appl Mater Interfaces, 2022, 14: 13678
|
| [25] |
TutikaR, KmiecS, HaqueABMT, MartinSW, BartlettMD. Liquid metal–elastomer soft composites with independently controllable and highly tunable droplet size and volume loading. ACS Appl Mater Interfaces, 2019, 11: 17873
|
| [26] |
BartlettMD, FasslerA, KazemN, MarkvickaEJ, MandalP, MajidiC. Stretchable, high-k dielectric elastomers through liquid-metal inclusions. Adv Mater, 2016, 28: 3726
|
| [27] |
LiuY, JiX, LiangJ. Rupture stress of liquid metal nanoparticles and their applications in stretchable conductors and dielectrics. npj Flex Electron, 2021, 5: 11
|
| [28] |
SuY, SuiG, LanJ, YangX. A highly stretchable dielectric elastomer based on core–shell structured soft polymer-coated liquid-metal nanofillers. ChemComm, 2020, 56: 11625
|
| [29] |
SongD, LiX, LiX-P, JiaX, MinP, YuZ-Z. Hollow-structured MXene-PDMS composites as flexible, wearable and highly bendable sensors with wide working range. J Colloid Interface Sci, 2019, 555: 751
|
| [30] |
YangX, WangY, QingX. A flexible capacitive sensor based on the electrospun PVDF nanofiber membrane with carbon nanotubes. Sens Actuator A Phys, 2019, 299111579
|
| [31] |
DuH, LiY, CaoC. Effect of temperature on dielectric properties of Si3N4/SiO2 composite and silica ceramic. J Alloys Compd, 2010, 503: L9
|
Funding
National Natural Science Foundation of China(No. 52473267)
National Key Research and Development Program of China(No. 2021YFB3501504)
Key Research and Development Program of Zhejiang Province(2024C01157)
Zhejiang University Ningbo Five in One Campus Project(K-20213539)
RIGHTS & PERMISSIONS
Donghua University, Shanghai, China