The Effect of Crosslinker Ratio on the Performance of Piezoelectric Elastomers

Wen-Xian Zhang; Shun-Zhang Ni; Shi-Cheng Wei; Xiao-Li Sun; Shou-Ke Yan

doi:10.1007/s10118-026-3760-0

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The Effect of Crosslinker Ratio on the Performance of Piezoelectric Elastomers

RESEARCH ARTICLE | 更新时间：2026-10-30

- The Effect of Crosslinker Ratio on the Performance of Piezoelectric Elastomers
- The Effect of Crosslinker Ratio on the Performance of Piezoelectric Elastomers
- Chinese Journal of Polymer Science 2026年44卷页码：1-11
- 作者机构：
  
  a.State Key Laboratory of Chemical Resource Engineering, Beijing University of Chemical Technology, Beijing 100029, China
  b.Key Laboratory of Rubber-Plastics of Ministry of Education, Shandong Provincial Key Laboratory of Rubber-plastics, Qingdao University of Science & Technology, Qingdao 266042, China
- 作者简介：
  
  xiaolisun@mail.buct.edu.cn
- 基金信息：
  
  This work was partly financially supported by Beijing Nova Program (No. 20250484794) and the National Natural Science Foundation of China (Nos. 22022501 and 22073006). A portion of this work is based on the data obtained at BSRF-1W1A. The authors gratefully acknowledge the beamline scientists at BSRF-1W1A beamline for providing technical support and assistance in WAXD data collection. This work is dedicated to the memory of Prof. Shou-Ke Yan.;The authors declare no interest conflict.Electronic supplementary information (ESI) is available free of charge in the online version of this article at http://doi.org/10.1007/s10118-026-3760-0.The data supporting the findings of this study are available from the corresponding author upon reasonable request.
- DOI：10.1007/s10118-026-3760-0
  中图分类号：
- 收稿：2026-07-04，
  
  录用：2026-08-28，
  
  网络首发：2026-10-29，
  
  纸质出版：2026-07
- 稿件说明：
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Zhang, W. X.; Ni, S. Z.; Wei, S. C.; Sun, X. L.; Yan, S. K. The effect of crosslinker ratio on the performance of piezoelectric elastomers. Chinese J. Polym. Sci. https://doi.org/10.1007/s10118-026-3760-0

Wen-Xian Zhang, Shun-Zhang Ni, Shi-Cheng Wei, et al. The Effect of Crosslinker Ratio on the Performance of Piezoelectric Elastomers[J/OL]. Chinese Journal of Polymer Science, 2026, 441-11.
Zhang, W. X.; Ni, S. Z.; Wei, S. C.; Sun, X. L.; Yan, S. K. The effect of crosslinker ratio on the performance of piezoelectric elastomers. Chinese J. Polym. Sci. https://doi.org/10.1007/s10118-026-3760-0 DOI：

Wen-Xian Zhang, Shun-Zhang Ni, Shi-Cheng Wei, et al. The Effect of Crosslinker Ratio on the Performance of Piezoelectric Elastomers[J/OL]. Chinese Journal of Polymer Science, 2026, 441-11. DOI： 10.1007/s10118-026-3760-0.

摘要

Abstract

Piezoelectric elastic composites based on polydimethylsiloxane (PDMS) elastomer filled with polar phase poly(vinylidene fluoride) (PVDF) microspheres are fabricated. The regulatory role of the elastic polymer matrix structure on the performance of the composite

which is less concerned in previous studies

is explored. Here

we have elucidated that precise control of the PDMS crosslinked network governs the stress transfer mechanism

enabling rational design of high-performance piezoelectric composites. By tuning the crosslinker ratio

we achieve PDMS crosslinking densities ranging from 9.9×10

–6

mol·cm

–3

to 91.3×10

–6

mol·cm

–3

enhancing the output voltage of the piezoelectric composite with 10 wt% PVDF microsphere content from 5.3 V to 19.8 V. Finite element simulation attributes this enhancement to more efficient stress transfer within the elastomer matrix with higher crosslinking density

strength

ening the dipole polarization response of polar PVDF microspheres. By increasing PVDF microsphere content to 30 wt%

the composite exhibits a piezoelectric coefficient (

) of 74 pC·N

–1

and a sensitivity of 647 mV·N

–1

which are 37 and 20 times higher than unoptimized composites in this work

respectively. This work advances understanding of mechanoelectrical coupling in flexible piezocomposites and provides a platform for designing next-generation sensors for intelligent robotics and non-contact acoustic sensing.

关键词

Keywords

references

Nain, A.; Chakraborty, S.; Barman, S. R.; Gavit, P.; Indrakumar, S.; Agrawal, A.; Lin, Z. H.; Chatterjee, K. Progress in the development of piezoelectric biomaterials for tissue remodeling. Biomaterials 2024 , 307 , 122528..

Chen, S.; Tong, X.; Huo, Y.; Liu, S.; Yin, Y.; Tan, M.-L.; Cai, K.; Ji, W. Piezoelectric biomaterials inspired by nature for applications in biomedicine and nanotechnology. Adv. Mater. 2024 , 36 , 2406192..

Zhu, W.; Wu, B.; Lei, Z.; Wu, P. Piezoionic elastomers by phase and interface engineering for high-performance energy-harvesting ionotronics. Adv. Mater. 2024 , 36 , 2313127..

Hu, Q.; Zhang, Y.; Rao, X.; Wang, L.; Gao, L.; Li, F.; Shen, H.; Pan, L.; Hu, B.-L. Biocompatible piezoelectric elastomer for self-powered electronics. Nano Lett. 2025 , 25 , 9646−9653..

Zhou, W.; Chen, Z.; Yuan, X.; Yu, H.; Zhang, Y.; Zhao, W.; Li, X.; Zhang, X.; Cui, Z.; Fu, P.; Pang, X.; Liu, M. Self-powered wireless piezoelectric sensor based on polyamide elastomer/BaTiO 3 for machine learning-assisted human motion monitoring. ACS Appl. Mater. Interfaces 2025 , 17 , 57500−57515..

Liu, Y.; Zheng, H.; Zhao, L.; Liu, S.; Yao, K.; Li, D.; Yiu, C.; Gao, S.; Avila, R.; Chirarattananon, P.; Chang, L.; Wang, Z.; Huang, X.; Xie, Z.; Yang, Z.; Yu, X. Electronic skin from high-throughput fabrication of intrinsically stretchable lead zirconate titanate elastomer. Research 2020 , 2020 , 1085417..

Wang, Y.; Xu, B.; Li, H.; Chu, X.; Bai, X.; Li, H.; Yan, S.; Sun, X. Intrinsic ferroelectric elastomers with ultrahigh Curie temperature and fast polarization switching. Nat. Commun. 2025 , 16 , 9219..

Liu, M.; Zhang, W.; Zhao, J.; Hua, L.; Ren, Z.; Yan, S.; Sun, X. Grafting-induced conformational engineering breaks polarization barriers in PVDF for high-temperature piezoelectrics. Chem. Mater. 2026 , 38 , 1445−1456..

Chu, X.; Kang, J. Q.; Hong, Y.; Zhu, G. D.; Yan, S. K.; Wang, X. Y.; Sun, X. L. The effect of substrate on the properties of non-volatile ferroelectric P(VDF-TrFE)/P3HT memory devices. Chinese J. Polym. Sci. 2022 , 40 , 692−699..

Chen, Z.; Wang, X.; Xu, J.; Li, H.; Su, H.; Hua, Q.; Shen, G. Bioinspired amphibious soft robotics with conformable ultrasonic array for adaptive defect mapping and terrain reconstruction. Adv. Funct. Mater. 2026 , 36 , e22932..

Mu, W.; Zhao, W.; Li, B.; Liu, Y.; Yin, R. A novel piezoelectric-driven and sensing soft robot. Adv. Mater. Technol. 2025 , 10 , e01142..

Bai, X.; Hou, C.; Chu, X.; Sun, X.; Yan, S. Grain-size engineering unlocks curie transition dynamics in P(VDF-TrFE). Macromolecules 2025 , 58 , 7334−7342..

Ghosh, S. K.; Pal, S.; Roy, K.; Yue, W.; Gao, Y.; Xia, F.; He, P.; Sarkar, S.; Teng, M.; Park, J.; Tsao, P.; Li, X.; Tofail, S. A. M.; Messersmith, P. B.; Lin, L. Highly responsive self-healing and degradable piezoelectric soft machines. Adv. Mater. 2025 , 37 , 2507859..

Wang, X.; Liu, Q.; Hu, X.; You, M.; Zhang, Q.; Hu, K.; Zhang, Q.; Xiang, Y. Highly stretchable lactate-based piezoelectric elastomer with high current density and fast self-healing behaviors. Nano Energy 2022 , 97 , 107176..

Wang, Z.; Tang, C.; Wang, Y.; Zhou, L.; Dong, X.; Jiang, S.; Pan, Y.; Liu, X.-J.; Zhao, H. Enhancing the energy conversion efficiency of dielectric elastomer generators via elastic energy storage and recovery. Appl. Energy 2025 , 379 , 124854..

Zhu, C.; Xue, H.; Zhou, Q.; Jiang, L.; Wu, J. Flexible lead-free cruciform piezo-arrays for implantable wireless energy harvesting on complex surfaces. J. Mater. Chem. A 2024 , 12 , 16116−16128..

Guan, X.; Xu, B.; Gong, J. Hierarchically architected polydopamine modified BaTiO 3 @P(VDF-TrFE) nanocomposite fiber mats for flexible piezoelectric nanogenerators and self-powered sensors. Nano Energy 2020 , 70 , 104516..

Sahoo, R.; Mishra, S.; Ramadoss, A.; Mohanty, S.; Mahapatra, S.; Nayak, S. K. An approach towards the fabrication of energy harvesting device using Ca-doped ZnO/PVDF-TrFE composite film. Polymer 2020 , 205 , 122869..

Zhang, H.; Jeong, C. K.; Shen, Z.; Wang, J.; Sun, H.; Jian, Z.; Chen, W.; Zhang, Y. Ultrahigh augmentation of flexible composite-based piezoelectric energy harvesting efficiency via polymer-impregnated nanoparticles network within 3D cellulose scaffold. Compos. Part B Eng. 2022 , 236 , 109813..

Kang, F.; He, H.; Guan, F.; Zhai, H.; Zhang, C.; Liu, Y.; Shen, Y.; Han, L. Enhanced self-poled output performance of flexible and mechanically robust in situ synthesized ZnO/PVDF hybrid piezoelectric composite films for human motion monitoring. Compos. Sci. Technol. 2025 , 269 , 111232..

Ramyashri, S.; Amiruddin, R.; E melyanov, A. V.; Santhosh Kumar, M. C. Development of Al foil-based flexible ZnO nanowires/PTAA hybrid piezoelectric nanogenerators. Appl. Surf. Sci. 2025 , 709 , 163818..

Yu, Q.; Ge, R.; Wen, J.; Du, T.; Zhai, J.; Liu, S.; Wang, L.; Qin, Y. Highly sensitive strain sensors based on piezotronic tunneling junction. Nat. Commun. 2022 , 13 , 778..

Glaum, J.; Hoffman, M. Electric fatigue of lead-free piezoelectric materials. J. Am. Ceram. Soc. 2014 , 97 , 665−680..

Liu, W.; Ren, X. Large piezoelectric effect in Pb-free ceramics. Phys. Rev. Lett. 2009 , 103 , 257602..

Li, J.; Chai, X.; Peng, D.; Zou, H.; Wang, X.; Yao, X. Largely enhanced electromechanical properties of BaTiO 3 -(Na 0.5 Er 0.5 )TiO 3 lead-free piezoelectric ceramics. Appl. Phys. Lett. 2014 , 105 , 082901..

Koç, M. Effect of multilayer fabrication of PVDF/PZT fibers on output performance in piezoelectric nanogenerator (PEN). J. Polym. Res. 2024 , 31 , 160..

Zhang, X.; Le, M.-Q.; Zahhaf, O.; Capsal, J.-F.; Cottinet, P.-J.; Petit, L. Enhancing dielectric and piezoelectric properties of micro-ZnO/PDMS composite-based dielectrophoresis. Mater. Des. 2020 , 192 , 108783..

Zhou, Z.; Du, X.; Zhang, Z.; Luo, J.; Niu, S.; Shen, D.; Wang, Y.; Yang, H.; Zhang, Q.; Dong, S. Interface modulated 0-D piezoceramic nanoparticles/PDMS based piezoelectric composites for highly efficient energy harvesting application. Nano Energy 2021 , 82 , 105709..

Gu, B.; Pu, G.; Ding, B.; Zhang, K.; He, R.; Fan, J.; Xing, T.; Wu, J.; Yang, W. Improved interfacial bonding strength of silicone rubber/carbon fiber modified by dopamine. Polym. Compos. 2022 , 43 , 6975−6986..

Li, Y.; Yuan, J.; Xue, J.; Cai, F.; Chen, F.; Fu, Q. Towards suppressing loss tangent: effect of polydopamine coating layers on dielectric properties of core–shell barium titanate filled polyvinylidene fluoride composites. Compos. Sci. Technol. 2015 , 118 , 198−206..

Li, Y.; Fan, M.; Wu, K.; Yu, F.; Chai, S.; Chen, F.; Fu, Q. Polydopamine coating layer on graphene for suppressing loss tangent and enhancing dielectric constant of poly(vinylidene fluoride)/graphene composites. Compos. Part A Appl. Sci. Manuf. 2015 , 73 , 85−92..

[Kang, H. B.; Han, C.-S.; Pyun, J. C.; Ryu, W. H.; Kang, C.-Y.; Cho, Y. S. (Na, K)NbO 3 nanoparticle-embedded piezoelectric nanofiber composites for flexible nanogenerators. Compos. Sci. Technol . 2015 , 111 , 1−8..

[Lakes, R. S. in Viscoelastic Solids . Boca Raton, FL, USA, CRC Press, 1999 ..

Kuelpmann, A.; Osman, M. A.; Kocher, L.; Suter, U. W. Influence of platelet aspect ratio and orientation on the storage and loss moduli of HDPE-mica composites. Polymer 2005 , 46 , 523−530..

Doddi, P. R. V.; Chanamala, R.; Dora, S. P. Effect of fiber orientation on dynamic mechanical properties of PALF hybridized with basalt reinforced epoxy composites. Mater. Res. Express 2020 , 7 , 015329..

Zhang, W.; Yang, J.; Sun, Q.; Peng, L.; Lin, T.; Yan, S.; Sun, X. Microspheres trigged-stress concentration regulating piezoelectric properties of PVDF/elastomer composites. Sci. China Chem. 2025 , 68 , 2605−2614..

Raman Venkatesan, T.; Owusu, F.; Nüesch, F. A.; Schulze, M.; Opris, D. M. Pyroelectricity in poled all-organic polar polynorbornene/polydimethylsiloxane-based stretchable electrets. J. Mater. Chem. C 2024 , 12 , 8408−8417..

Martins, P.; Lopes, A. C.; Lanceros-Mendez, S. Electroactive phases of poly (vinylidene fluoride): determination, processing and applications. Prog. Polym. Sci. 2014 , 39 , 683−706..

Hou, C.; Zhang, W.; Dai, X.; Qiu, J.; Russell, T. P.; Sun, X.; Yan, S. Spatially confined fabrication of polar poly (vinylidene fluoride) nanotubes. Small 2022 , 18 , 2205790..

Xu, Q.; Jia, M.; Zhou, P.; Zhang, Y.; Guo, W.; Zhao, S.; Zeng, H.; Zhang, J.; Yan, M.; Jiang, S.; Zhou, K.; Zhang, D.; Bowen, C. High-performance ultrasensitive flexible piezoelectric thin film sensors via a cost-effective transfer strategy. Adv. Funct. Mater. 2025 , 35 , 2414211..

Jang, H.; Kim, G. H.; Jeon, D. W.; Park, H. J.; Bae, B.; Alluri, N. R.; Kim, C. M.; Baek, C.; Lee, M.-K.; Cho, S. B.; Lee, G.-J.; Park, K.-I. Long-lasting, steady and enhanced energy harvesting by inserting a conductive layer into the piezoelectric polymer. Adv. Funct. Mater. 2025 , 35 , 2415501..

Han, J.; Park, S. H.; Jung, Y. S.; Cho, Y. S. High-performance piezoelectric energy harvesting in amorphous perovskite thin films deposited directly on a plastic substrate. Nat. Commun. 2024 , 15 , 4129..

Lozano, H.; Catalán, G.; Esteve, J.; Domingo, N.; Murillo, G. Non-linear nanoscale piezoresponse of single ZnO nanowires affected by piezotronic effect. Nanotechnology 2021 , 32 , 025202..

Sheridan, G. S.; Evans, C. M. Understanding the roles of mesh size, T g , and segmental dynamics on probe diffusion in dense polymer networks. Macromolecules 2021 , 54 , 11198−11208..

Zhao, Y.; Liao, Q.; Zhang, G.; Zhang, Z.; Liang, Q.; Liao, X.; Zhang, Y. High outputpiezoelectric nanocomposite generators composed of oriented BaTiO 3 NPs@PVDF. Nano Energy 2015 , 11 , 719−727..

Ghosh, S. K.; Mandal, D. Synergistically enhanced piezoelectric output in highly aligned 1D polymer nanofibers integrated all-fiber nanogenerator for wearable nano-tactile sensor. Nano Energy 2018 , 53 , 245−257..

Park, D. Y.; Joe, D. J.; Kim, D. H.; Park, H.; Han, J. H.; Jeong, C. K.; Park, H.; Park, J. G.; Joung, B.; Lee, K. J. Self-powered real-time arterial pulse monitoring using ultrathin epidermal piezoelectric sensors. Adv. Mater. 2017 , 29 , 1702308..

Lee, J.-H.; Yoon, H.-J.; Kim, T. Y.; Gupta, M. K.; Lee, J. H.; Seung, W.; Ryu, H.; Kim, S.-W. Micropatterned P(VDF-TrFE) film-based piezoelectric nanogenerators for highly sensitive self-powered pressure sensors. Adv. Funct. Mater. 2015 , 25 , 3203−3209..

Dörr, D.; Henning, F.; Kärger, L. Nonlinear hyperviscoelastic modelling of intra-ply deformation behaviour in finite element forming simulation of continuously fibre-reinforced thermoplastics. Compos. Part A Appl. Sci. Manuf. 2018 , 109 , 585−596..

Yang, J.; Chen, J.; Su, Y.; Jing, Q.; Li, Z.; Yi, F.; Wen, X.; Wang, Z.; Wang, Z.-L. Eardrum-inspired active sensors for self-powered cardiovascular system characterization and throat-attached anti-interference voice recognition. Adv. Mater. 2015 , 27 , 1316−1326..

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