MXene-Based Elastomer Mimetic Stretchable Sensors: Design, Properties, and Applications

doi:10.1007/s40820-024-01349-w

Abstract

Abstract:

Flexible sensors based on MXene-polymer composites are highly prospective for next-generation wearable electronics used in human-machine interfaces. One of the motivating factors behind the progress of flexible sensors is the steady arrival of new conductive materials. MXenes, a new family of 2D nanomaterials, have been drawing attention since the last decade due to their high electronic conductivity, processability, mechanical robustness and chemical tunability. In this review, we encompass the fabrication of MXene-based polymeric nanocomposites, their structure-property relationship, and applications in the flexible sensor domain. Moreover, our discussion is not only limited to sensor design, their mechanism, and various modes of sensing platform, but also their future perspective and market throughout the world. With our article, we intend to fortify the bond between flexible matrices and MXenes thus promoting the swift advancement of flexible MXene-sensors for wearable technologies.

Key words: Flexible sensor, 2D nanomaterials, MXene, Wearable and conductive, Applications

Poushali Das, Parham Khoshbakht Marvi, Sayan Ganguly, Xiaowu (Shirley) Tang, Bo Wang, Seshasai Srinivasan, Amin Reza Rajabzadeh, Andreas Rosenkranz. MXene-Based Elastomer Mimetic Stretchable Sensors: Design, Properties, and Applications[J]. Nano-Micro Letters, 2024, 16(1): 135-.

Poushali Das, Parham Khoshbakht Marvi, Sayan Ganguly, Xiaowu (Shirley) Tang, Bo Wang, Seshasai Srinivasan, Amin Reza Rajabzadeh, Andreas Rosenkranz. [J]. Nano-Micro Letters, 2024, 16(1): 135-.

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Figures/Tables 20

Fig. 1 a Different techniques for synthesising MPCs. b Schematic illustration showing the preparation of d-Ti₃C₂T_x (HF-etching prior to delamination by DMSO and water and followed by high-temperature annealing) and PVC/Ti₃C₂T_x nanocomposite films. c Dielectric constant and (d) Young’s modulus as well as tensile strength of PVC/MXene nanocomposites. Reproduced with the permission from Ref. [90], Copyright Elsevier 2020. e Schematic representation of melt blending for the fabrication of Ti₃C₂T_x/PP nanocomposites. f Tensile strength and elongation at break of the Ti₃C₂T_x/PP nanocomposites as a function of the Ti₃C₂T_x content. SEM images of 2.0 wt% Ti₃C₂T_x/PP nanocomposite as well as g their fracture surface after freeze-brittle fracture. h and i Stretch-fracture surface; j Schematic models of mechanical failure (including H bonding break and slippage) of PP-g/Ti₃C₂T_x NS-2.0. Reproduced with the permission from Ref. [91], Copyright Elsevier 2019

Table 1 Overview of typical MXenes-based polymer composites with the respective application area and key features

MXenes type	Polymer matrix	Application area	Features	References
AgNWs/Ti₃C₂T_x	PU	Strain sensing	1000 cycling stability, response/recovery time of 344/344 ms	[77]
Ti₃C₂T_x	Chitosan and PU	Pressure sensing	High compressive strength	[78]
Mo₂C	PVA	Humidity sensing	1/1.8 s recovery time	[79]
TiO₂/Ti₃C₂T_x	Nafion	Peroxide sensing	Linear range of 0.1-380 μM, sensitivity of 447.3 μA (mM cm²)⁻¹, detection limit of 14 nM, 94.6% left after 60-day storage	[80]
GO_x/Au/Ti₃C₂T_x	Nafion	Glucose sensng	Sensitivity of 4.2 μA (mM cm²)⁻¹, detection limit of 5.9 μM (S/N = 3)	[81]
Ti₃C₂T_x	PVA	Capacitor	Electrical conductivities of 2.2 × 10⁴ S m⁻¹, volumetric capacitance of 530 F cm⁻³ at 2 mV s⁻¹	[82]
Ti₃C₂-S/d-Ti₃C₂	PP	Battery	Reversible capacitance	[83]
Ti₃C₂T_x	PDT	Supercapacitor	Capacitance of 52.4 mF cm⁻² (3.52 F cm⁻³) at 0.1 mA cm⁻², 10,000 charge-discharge cycles (100%)	[84]
Ti₃C₂T_x	PVDF	Antibacterial	Antibacterial rate of 73 and 67% against Bacillus subtilis Escherichia coli, respectively	[85]
Ti₃C₂T_x	PAN	Air purify	2.5 removal efficiency of 99.7%, low pressure drop of 42 Pa	[86]
Ti₃C₂T_x	PANI/PP	EMI	~ 40 dB	[87]

Fig. 2 a Graphical representation of the fabrication of composite foams and films made from f-Ti₂CT_x/PVA. Reproduced with the permission from Ref. [93], Copyright American Chemical Society 2019. b Schematic representation of the synthesis procedure for freestanding nanocomposites. Reproduced with the permission from Ref. [94], Copyright Elsevier 2020. c Diagram depicting the generation of hybrid aerogels and PDMS-coated MS foams. Reproduced with the permission from Ref. [95], Copyright Elsevier 2020

Fig. 3 a Schematic representation of melt blending used to prepare Ti₃C₂T_x/TPU nanocomposites with the b corresponding SEM image of 1.0 wt% Ti₃C₂T_x/TPU. Resulting mechanical properties of the Ti₃C₂T_x/TPU nanocomposites as a function of the MXene content including c tensile stress-strain curves, d tensile strength, e elongation at break, and f hardness. Reproduced with the permission from Ref. [96] Copyright Elsevier 2019

Table 2 General information regarding Ti₃C₂T_x MXene/thermoplastic nanocomposites

Thermoplastic Polymer	Method of preparation	References
PU	Emulsion method	[92]
PVA	Casting/evaporation method	[89]
UHMWPE	Melt blending	[98]
PEDOT:PSS	Vacuum-assisted filtration process	[99]
NR	Vacuum-assisted filtration process	[97]
PVA	Solution blending method	[88]
PVC	Solution blending method	[90]

Fig. 4 a Schematics of MXene/epoxy nanocomposites processing techniques. b Schematic illustration of the fabrication process of c rGH, d rGMH, and e rGMH/epoxy nanocomposites. Axial and radial SEM images of c', c" rGH, d', d" rGMH, and e', e" rGMH/epoxy nanocomposites, respectively. Reproduced with the permission from Ref. [111], Copyright Elsevier 2020. f Schematic representation of the fabrication process employed to produce MCF/epoxy nanocomposites. Reproduced with the permission from Ref. [112], Copyright Elsevier 2019. g Graphical representation of the synthesis method for TCTA/epoxy nanocomposites. Reproduced with the permission from Ref. [113] Copyright American Association for the Advancement of Science 2020

Fig. 5 a Schematic depiction of the PVA/Ti₃C₂T_x MPC thin-film synthesis process, the related optical image of the resultant MPC, and the cross-sectional SEM images of the film with different content of PVA varying from 50 to 0%. Reproduced with the permission from Ref. [117], Copyright Elsevier 2021. b Schematic illustration of the Janus nanofibrous MXene/chitosan/polyurethane MPC with interfacial hydrogen bonding and the pertinent SEM images. Reproduced with the permission from Ref. [118], Copyright Elsevier 2023. c Schematic diagram of Ti₃C₂T_x nanosheet fabrication and SEM images of Ti₃AlC₂ and multi-layered MXene nanosheets, as well as TEM image of monolayered MXene nanosheet plus the schematic diagram of PAM/PAA/MXene/TA hydrogel fabrication and the sectional and top-view SEM images of the resultant MPC. Reproduced with the permission from Ref. [119], Copyright Elsevier 2022

Table 3 Structural properties of MPCs (D_pore: Pore Size, SSA: specific surface area, ESA: electrochemical surface area)

MPC composition	Morphology of the microstructure	References
Ti₃C₂T_x/polydopamine	Cylindrical mesochannels	[115]
Ti₃C₂T_x/polydopamine	(D_pore = 7.6 nm, SSA = 89.5 m² g⁻¹)	[115]
Ti₃C₂T_x/SWCNT/PANI	Hierarchical structure	[116]
Ti₃C₂T_x/SWCNT/PANI	(ESA = 10.80 cm² per unit area of the platinum electrode)	[116]
Ti₃C₂T_x/PVA	Hierarchical structure	[117]
Ti₃C₂T_x/PVA	(D_pore = 0-2 µm)	[117]
Ti₃C₂T_x/polypyrrole	Cylindrical to spherical mesostructures and spherical macrostructure	[120]
Ti₃C₂T_x/polypyrrole	(D_pore = 7.8-52 nm, SSA = 129-188 m² g⁻¹)	[120]
Ti₃C₂T_x/cellulose acetate/sodium alginate	Unique ordered porous network	[121]
Ti₃C₂T_x/cellulose acetate/sodium alginate	(D_pore = 30-50 μm)	[121]
Ti₃C₂T_x/gelatin/polyacrylamide	Compact honeycomb-like porous structure	[122]
Ti₃C₂T_x/polyacrylamide/polyacrylic acid/tannic acid	Smooth microstructure	[119]
Ti₃C₂T_x/chitosan/polyurethane	Janus core-shell porous network	[118]
Ti₃C₂T_x/chitosan/polyurethane	(D_pore = few micrometers)	[118]

Fig. 6 Graphical representation of the property improvements in MXenes-polymer nanocomposites in comparison to bare polymers

Fig. 7 Primary steps in making MXenes/PDMS-based elastomeric nanocomposites and their physical interactions. Reproduced with the permission from Ref. [145], Copyright American Chemical Society 2020

Fig. 8 Diagrammatic representation of the manufacturing process for MXene/PMN hydrogels. Reproduced with the permission from Ref. [154], Copyright Elsevier 2022

Fig. 9 Human motions detection. a How the bilayer composite hydrogel strain sensor’s electrical signal changes when the arm bends. b When the wrist moves in two different ways, the relative current of the strain gauge changes. c How the piezoresistive reaction of the strain sensor changes when the head moves. d The electrical output from the strain sensor when the finger is bent 45° and 60°. e When the mouth opens, there is a change in the relative resistance of the strain gauge. f Response curves for smiling right now. Reproduced with the permission from Ref. [3] Copyright Elsevier 2021

Fig. 10 a Sensitivities (a₁, a₃, a₅) and response times (a₂, a₄, a₆) of MXene/CNF. Reproduced with the permission from Ref [167]. (Copyright American Chemical Society, 2019), MXene/SF [172] (Copyright Elsevier, 2020) and MXene/CS [177] (Copyright Elsevier, 2023) based pressure sensors, as well as b their applications in human health detections, such as face expression [167] (Copyright American Chemical Society, 2019), finger bending [177] (Copyright Elsevier, 2023), pulse measurement [168] (Copyright Elsevier, 2021), acoustic vibration [177] (Copyright Elsevier, 2023), and foot movement [176] (Copyright Elsevier, 2023)

Table 4 Performance of the biopolymer/MXene-based stretchable sensors

Sensing materials	Sensor type	Sensitivity	Sensing range; detection limit	Stability; response time	References
MXene/BC	Pressure sensor	12.5 kPa⁻¹ (0-10 kPa)	0-10 kPa; 1.0 Pa	100 cycles (99% strain), 100,000 cycles (50% strain); 167 ms	[167]
MXene/CNF		419.7 kPa⁻¹ (0-8.04 kPa), 649.3 kPa⁻¹ (8.04-20.55 kPa)	0-20.55 kPa; 4.0 Pa	10,000 cycles; 123 ms	[168]
MXene/CNF		95.2 kPa⁻¹ (2-50 Pa), 27.5 kPa⁻¹ (0.05-3 kPa), 0.94 kPa⁻¹ (3-10 kPa)	2-10 kPa; 0.4 Pa	25,000 cycles; 95 ms	[169]
MXene/CNF		10.7 kPa⁻¹ (0-240 kPa), 34.6 kPa⁻¹ (240-640 kPa), 16.6 kPa⁻¹ (640-950 kPa)	0-950 kPa; -	3000 cycles; 298 ms	[170]
MXene/CNT/CNF		817 (0-0.2 kPa), 234.9 (0.2-1.5 kPa)	0-1.5 kPa; -	2000 cycles (30% strain);74 ms	[171]
MXene/SF		25.5 kPa⁻¹ (0.1-0.5 kPa), 3.4 kPa⁻¹ (1.0-20 kPa)	0-20 kPa; 9.8 Pa	3500 cycles (73 Pa); 40 ms	[172]
MXene/SF/GO		14.23 kPa⁻¹ (MXene/SF (9:1), 1.4 kPa), 12.53 kPa⁻¹ (MXene/SF (5:1), 1.4 kPa),	0-1.5 kPa; 72 Pa	-	[173]
MXene/SF/TA		GF: 0.59	20-100% strain; -	600 cycles (self-healing); -	[175]
MXene/SF/HA	Strain sensor	GF: 4.5-11.3 (5-80% strain)	-	10,000 cycles (50% strain); -	[176]
Mxene/CS/PA	Strain sensor	GF: 3.15 (− 20 °C), 3.93 (25 °C), 2.55 (80 °C)	1-600% strain, 0.08-3.2 kPa stress; 0.5 g	-; 500 ms	[158]

Fig. 11 a Structure (a₁), properties (a₂, a₃), and speech detection application (a₄) of the Ti₃C₂T_x/ENR stretchable sensor. Reproduced with permission from Ref [178]. (Copyright American Chemical Society, 2020). b Optical image (b1), and sensing performance (b2-b5) of the self-powered Ti₃C₂T_x/SEBS sensing system. Reproduced with permission from Ref [184]. (Copyright Elsevier, 2022). c Comparison of gauge factor between MXene/TPU/PDA and MXene/TPU/CNF stretchable sensors. Reproduced with permission from Refs [181,182,183]. (Copyright Elsevier, 2022), (Copyright American Chemical Society, 2022), (Copyright American Chemical Society, 2021)

Fig. 12 Proof-of-concept for HMI systems made with MXene-coated cotton. a, b Digital picture and circuit layout of the MXene-coated cotton pressure-sensing fabric interface. c Software for using MXene-coated cotton pressure-sensing cloth, called MXene Tools. d, e MXene Tools pressure sensing (single area and multi-region) and pressure-sensitive data modelling diagrams in 3D. Reproduced with the permission from Ref. [4], Copyright American Chemical Society 2020

Fig. 13 a Simulated adsorption energy of eight different gas molecules on Ti₂CO₂ monolayers as a function of applied biaxial strains, and side- as well as top-view of schematic of the pertinent adsorption. Reproduced with permission from Ref. [212], Copyright American Chemical Society 2015. b DFT adsorption energy values of ethanol molecule on Ti₃C₂(OH)₂, Ti₃C₂O₂, and Ti₃C₂F₂ and c Comparison of adsorption energy values for ethanol, methanol, ammonia, and acetone gas molecules on Ti₃C₂(OH)₂; d Optical images of flexible PANI/Ti₃C₂T_x sensors with the sensitivity values against varied bending angles (exposed to 150 ppm ethanol gas molecules); e The juxtaposition of the pristine Ti₃C₂T_x and PANI/Ti₃C₂T_x MPC in terms of selectivity for various gas targets (200 ppm) and dynamic response/recovery trends ranging within 50-200 ppm of ethanol, both performed at RT, and f bending stability of flexible sensors to 150 ppm ethanol gas molecules. Reproduced with the permission from Ref. [219], Copyright Wiley 2019. g Schematic illustration of the fabrication process, SEM image of the 3D PVA/PI/Ti₃C₂T_x, as well as the resistance changes of the 3D MPC sensor and MXene sensor during 5 successive cycles of exposure to 5 ppm methanol and ethanol; h Sensing performance of the 3D MPC sensor at 20 ppm acetone undergoing different bending cycles. Reproduced with the permission from Ref. [220], Copyright Royal Society of Chemistry 2018. i Schematic illustration of P/MXene chemical structure and the pinning strategy to acquire long-term sensing stability, comparison of the sensing responses of P/MXene and MXene at 20 ppm of formaldehyde, response intensities of P/MXene and MXene to various gas species, and sensing responses of P/O-MXene and P/pin-O-MXene to various gas species (P/MXene, P/O-MXene, and P/pin-O-MXene stand for PDA/MXene, partially oxidized P/MXene, and final pinned P/O-MXene, respectively). Reproduced with the permission from Ref. [222], Copyright Wiley 2020

Fig. 14 a Schematic of drop-castedTi₃C₂T_x/PDDS hybrid films on the electrodes and b the selectivity of the fabricated sensor. Reproduced with the permission from Ref. [228], Copyright Wiley 2022. c Illustration of ammonia sensing mechanism of flexible Ti₃C₂T_x/urchin-like PANI hollow nanosphere composite sensors; d Comparison between pristine u-PANI and MP-15 (MPC with 15 wt% aniline) selectivity to different targets; e Dynamic response-recovery curves under successive bending cycles with different bending angles (inset depicts the bending orientation), and f Response-concentration fitting plots ranging within 2-10 ppm. Reproduced with the permission from Ref. [229], Copyright Elsevier 2022. g Sensing mechanism of Ti₃C₂T_x/PANI:PSS MPC, and h the comparison between MPC and pure PANI:PSS in terms of selectivity. Reproduced with the permission from Ref. [230], Copyright Elsevier 2023. i Gas response of the Ti₃C₂T_x/PANI:PSS composite-based sensor towards 100 ppm NH₃ at varied bending angles and the linear dependence between the gas response and ammonia concentration. Reproduced with the permission from Ref. [231], Copyright American Chemical Society 2020. j Fabrication process of the Nb₂CT_x/PANI sensors; and k humidity influence on the sensing response for 100 ppm ammonia. Reproduced with the permission from Ref. [232], Copyright Elsevier 2021. l DFT-simulated adsorption modes and adsorption distance between PDAC and two different target molecules, namely NH₃ and CO, and m real-time resistance of the developed Ti₃C₂T_x@PDAC paper-based sensor versus time with respect to the ammonia concentration in flat, folded, and rolled states. Reproduced with the permission from Ref. [235], Copyright Royal Society of Chemistry 2023

Fig. 15 a Schematic illustration of Ti₃C₂T_x/PDS-Cl nanocomposite synthesis and sensor fabrication: addition of MXene ink to the water dissolved PDS-Cl polymer, tip sonication (for 2 min at 20 W) for accelerating the physical blending, and fabrication of H₂S sensor by drop-casting the MPCs solution on prepatterned Au electrodes; b Selectivity of Ti₃C₂T_x/PDS-Cl (with 10 wt.- % of MXene: MP-10) toward 6 different analytes with a negative response for H₂S (inset shows the selectivity of pristine Ti₃C₂T_x), dynamic sensing response of MP-10 for various concentrations of H₂S, and the related calibration curve. Reproduced with the permission from Ref. [237], Copyright American Chemical Society 2023. c Response of the ternary N-doped- Ti₃C₂T_x/PEI/rGO as a function of RH, the pertinent linear fitting of response toward 8-600 ppm CO₂, and selectivity under 62% RH. Reproduced with the permission from Ref. [240], Copyright American Chemical Society 2020. d Dynamic responses of the MXene@AuNP DN hydrogel sensor to 1 ppm TMA under multiple deformation states (initial, twisting, knotting, and folding states), selectivity of the gas sensor, and the acquired linear fitted response versus TMA concentration at RT. Reproduced with the permission from Ref. [242], Copyright American Chemical Society 2022

Fig. 16 Significant technical obstacles in the application of MXenes and their composites

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