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. 2025 Apr 10;10(15):14666-14675.
doi: 10.1021/acsomega.4c07933. eCollection 2025 Apr 22.

Cellulose Nanocrystal and Self-Assembling Lignin Enhanced the PEDOT/PSS/PVA Composite on Mechanical and Self-Powered Wearable Properties

Shih-Chen Shi  1 , Yan-Ching Hsieh  1 , Dieter Rahmadiawan  1   2
Affiliations

Cellulose Nanocrystal and Self-Assembling Lignin Enhanced the PEDOT/PSS/PVA Composite on Mechanical and Self-Powered Wearable Properties

Shih-Chen Shi et al. ACS Omega. .

Abstract

Lignin nanomicelle (LNM) synthesis via deep eutectic solvent (DES) has been optimized from a conventional duration of 2-3 days to a streamlined 12 h procedure utilizing autoclave reactor heating. This approach facilitates the efficient extraction of lignin from straw and its subsequent formation into LNMs via a simultaneous self-assembly mechanism. Integration of these amphiphilic LNMs into a cellulose nanocrystal (CNC) framework, combined with PEDOT: PSS in a poly(vinyl alcohol) (PVA) matrix, yields a self-powered strain sensor characterized by enhanced tensile properties and heightened strain sensitivity. Incorporating carboxyl functional groups from LNMs on the PVA matrix significantly augments the sensor's mechanical strength and elasticity. This is evidenced by achieving Young's modulus of 65.9 MPa and an elongation capacity of 320%, ensuring its efficacy in human motion detection. The synergistic inclusion of CNCs and LNMs amplifies the sensor's gauge factor, thereby augmenting its strain responsiveness. The elevated aspect ratio of CNCs establishes an efficacious electrical network that, in concert with the interaction between CNCs and PEDOT: PSS, diminishes the electrical percolation threshold, culminating in an improved gauge factor of 19, indicative of enhanced strain detection capabilities. Furthermore, the sensor can generate a thermoelectric voltage in response to thermal gradients, with the dynamic structures of LNM improving the conductivity and PEDOT: PSS dispersion within the PVA matrix, thereby optimizing the Seebeck coefficient. After enduring 5000 cycles of 100% strain deformation tests, the sensor demonstrates consistent performance, underscoring its reliability and durability. The fabricated PVA/Gly-LNM/CNCs/PEDOT: PSS composite material has been successfully applied to detect nuanced human gestures, including finger and wrist movements, affirming its potential utility in wearable technology applications.

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Conflict of interest statement

The authors declare no competing financial interest.

Figures

Figure 1
Figure 1
Purity and yield of LNMs produced by the DES method.
Figure 2
Figure 2
Surface morphology of LNMs at 110 °C 8 h (a), 110 °C 12 h (b), 110 °C 16 h (c), 120 °C 8 h (d), 120 °C 12 h (e), 120 °C 16 h (f), 130 °C 8 h (g), 130 °C 12 h (h), and 130 °C 16 h (i).
Figure 3
Figure 3
SEM images of PVA/Gly-PEDOT:PSS (a) and PVA/Gly-PEDOT:PSS/CNCs/LNM (b) composite surface.
Figure 4
Figure 4
XRD (a) and FTIR spectra (b) of samples with and without CNC-LNM. Tensile test results with various LNM contents (c) and Gly contents (d).
Figure 5
Figure 5
Resistance change rate (a) and gauge factor under various strains (b).
Figure 6
Figure 6
Seebeck coefficients of various LNM contents.
Figure 7
Figure 7
Thermoelectric voltage under various temperature differences.
Figure 8
Figure 8
Thermoelectric current change rate under various strains.
Figure 9
Figure 9
Thermoelectric voltage (a) and current of various DMSO contents (b) under various strains.
Figure 10
Figure 10
Resistance rate under 0–25% (a), 0–50% (b), and 0–100% (c) strain cyclic stretching test.
Figure 11
Figure 11
Testing the self-powered thermoelectric properties with 9 mg of LNM at 100% strain after 2500 (a), 5000 (b), 7500 (c), and 10,000 (d) reciprocations.
Figure 12
Figure 12
Resistance change rate for various strains on the wrist (a), finger (b), and elbow (c).
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