Highly Conductive, Stable, and Self-Healing MXene-Based Hydrogel Sensor via a Controlled Assembly of Polydopamine and Cellulose Nanocrystal

Abstract

MXene is a promising conductive nanofiller for hydrogels due to its excellent electricity conductivity and water dispersibility. However, MXene is prone to oxidize in the presence of air and water, resulting in a significant loss of conductivity. Polydopamine (PDA) has been coated on MXene to enhance its antioxidation stability via the physical barrier and chemical reducing ability of PDA, which unavoidably causes severe aggregation and a significant decrease in conductivity due to the crosslinking and insulation of PDA. Herein, we propose a facile strategy to construct a highly conductive, stable, and self-healing MXene-based polyvinyl alcohol (PVA) hydrogel by a controlled assembly of PDA and cellulose nanocrystal (CNC). PDA is first formed by oxidation self-polymerization in PVA solution without the presence of CNC and MXene, which can effectively reduce the content of aggregation-inducing groups and avoid the formation of an insulating PDA layer on the surface of MXene. The addition of CNCs results in the easy dispersion of a high content of MXene via hydrogen bonding and electrostatic interactions. The PVA-PDA hydrogel with MXene and CNC as conductive and reinforcing nanofillers (PP-CM) is cross-linked by dynamic borax covalent bonds and shows a conductivity of 7.14 S m⁻¹. The introduction of PDA effectively protects MXene and results in only a 14% decrease in conductivity after 7 days, significantly improving antioxidant stability. This hydrogel also possesses rapid self-healing capabilities, achieving 90.5% self-healing efficiency within 10 min. This versatile approach opens new avenues for the preparation and application of MXene-based conductive hydrogels.

Keywords

cellulose nanocrystals / conductive hydrogel / MXene / polydopamine / sensor

References

[1] P. Lu, J. Xu, S. Liu, L. Fu, S. Wu, Z. Liu, T. Hou, H. Liu, D. Huang, Sci. Rep. 2025, 15, 7335.

[2] H. He, H. Li, A. Pu, W. Li, K. Ban, L. Xu, Nat. Commun. 2023, 14, 759.

[3] Y. Zhao, K. Zhao, R. Qian, Z. Yu, C. Ye, Chem. Eng. J. 2024, 486, 150197.

[4] Z. Meng, Z. Qiu, Y. Shi, S. Wang, G. Zhang, Y. Pi, H. Pang, Escience 2023, 3, 100092.

[5] E. Chalmers, H. Lee, C. Zhu, X. Liu, Chem. Mater. 2020, 32, 234.

[6] Z. Zhu, Y. Men, W. Zhang, W. Yang, F. Wang, Y. Zhang, Y. Zhang, X. Zeng, J. Xiao, C. Tang, X. Li, Y. Zhang, eScience 2024, 4, 100249.

[7] L. Han, L. Yan, M. Wang, K. Wang, L. Fang, J. Zhou, J. Fang, F. Ren, X. Lu, Chem. Mater. 2018, 30, 5561.

[8] J. Zou, J. Wu, Y. Wang, F. Deng, J. Jiang, Y. Zhang, S. Liu, N. Li, H. Zhang, J. Yu, Chem. Soc. Rev. 2022, 51, 3314.

[9] J. Wang, Q. Qin, F. Li, Y. Anjarsari, W. Sun, R. Azzahiidah, J. Zou, K. Xiang, H. Ma, J. Jiang, Arramel, Carbon Lett. 2023, 33, 1381.

[10] Y. Xu, Z. Zhang, B. Tang, G. Zhou, Prog. Chem. 2021, 33, 2033.

[11] S. Bai, M. Yang, J. Jiang, X. He, J. Zou, Z. Xiong, G. Liao, S. Liu, NPJ 2D Mater Appl. 2021, 5, 78.

[12] P. Praus, Carbon Lett. 2024, 34, 227.

[13] J. Jiang, F. Li, L. Ding, C. Zhang, Arramel, X. Li, Nano Res 2024, 17, 3429.

[14] J. Jiang, F. Li, J. Zou, S. Liu, J. Wang, Y. Zou, K. Xiang, H. Zhang, G. Zhu, Y. Zhang, X. Fu, J.-P. Hsu, Sci China Mater. 2022, 65, 2895.

[15] J. Fan, R. Yang, Y. Du, F. Wang, L. Wang, J. Yang, A. Zhou, Nano Energy 2024, 129, 109999.

[16] Z. Zhang, Y. Xu, T. Ma, G. Sèbe, Y. Niu, Y. Wang, B. Tang, G. Zhou, Renew. Sust. Energ. Rev. 2024, 203, 114787.

[17] J. Jiang, S. Bai, J. Zou, S. Liu, J.-P. Hsu, N. Li, G. Zhu, Z. Zhuang, Q. Kang, Y. Zhang, Nano Res 2022, 15, 6551.

[18] J. Li, C. Miao, J. Bian, S. Seyedin, K. Li, Chin. Chem. Lett. 2023, 34, 107996.

[19] Y. Hou, Z. Zhang, S. Harrisson, G. Sèbe, Carbohydr. Polym. 2024, 341, 122346.

[20] Z. Zhang, M. Zhong, H. Xiang, Y. Ding, Y. Wang, Y. Shi, G. Yang, B. Tang, K. C. Tam, G. Zhou, Int. J. Biol. Macromol. 2023, 253, 127263.

[21] W. Sun, Z. Zhang, Z. Zhang, N. He, Q. Wei, L. Feng, Z. Wang, J. Wu, C. Liu, S. Fu, Y. Hou, G. Sèbe, G. Zhou, Sci. China Mater. 2024, 67, 3225.

[22] Y. Xu, B. Tang, X. Fang, T. Ma, D. Yu, G. Zhou, Z. Zhang, Ind. Eng. Chem. Res. 2022, 61, 18109.

[23] H. Xiang, B. Wang, M. Zhong, W. Liu, D. Yu, Y. Wang, K. C. Tam, G. Zhou, Z. Zhang, ACS Sustain. Chem. Eng. 2022, 10, 5939.

[24] Y. Li, J. Wang, H. Chen, H. Sun, H. Xu, D. Yang, Polymer 2024, 307, 127239.

[25] C. He, T. Yang, Z. Wang, Y. Liang, Y. Tong, W. Li, J. Membr. Sci. 2023, 679, 121661.

[26] L. Qin, J. Jiang, L. Hou, F. Zhang, J. Rosen, Energy Environ. Mater. 2024, 7, e12653.

[27] B. Wan, N. Liu, Z. Zhang, X. Fang, Y. Ding, H. Xiang, Y. He, M. Liu, X. Lin, J. Tang, Y. Li, B. Tang, G. Zhou, Carbohydr. Polym. 2023, 314, 120929.

[28] Z. Zhang, X. Lin, J. Lin, N. Liu, B. Wan, X. Fang, L. Shui, Y. Li, K. C. Tam, J. Huang, G. Zhou, Chem. Eng. J. 2023, 473, 145435.

[29] N. Ramasamy, A. Sivalingam, S. S. Saravanabhavan, K. N. Palani, B. Natesan, Carbon Lett. 2024, 34, 743.

[30] C. Zhu, S. Yang, M. Wang, Y. Zeng, L. Chu, W. Xie, P. Lan, L. Lan, G. Zhou, Z. Zhang, J. Colloid Interface Sci. 2025, 695, 137834.

[31] Z. Zhang, X. Fang, Z. Wang, W. Sun, Y. Zhang, G. Zhou, J Mater Chem A 2025, 13, 10709.

[32] J. Zhou, X. Gong, J. Kang, S. Chen, Z. Hu, M. Nie, L. Sun, J. Power Sources 2025, 638, 236637.

[33] C. F. Mok, Y. C. Ching, F. Muhamad, N. A. Abu Osman, N. D. Hai, C. R. Che Hassan, J. Polym. Environ. 2020, 28, 775.

[34] X. Yu, W. Qin, X. Li, Y. Wang, C. Gu, J. Chen, S. J. J. o. M. C. A. Yin, J Mater Chem A 2022, 28, 15000.

[35] Z. Chen, Z. Du, L. Li, K. Jiang, D. Chen, G. Shen, Energy Environ. Mater. 2024, 7, e12756.

[36] N. Liu, B. Wan, Z. Zhang, X. Fang, X. Lin, Y. Wang, J. Tang, X. Bai, Y. Li, Y. Yao, G. Zhou, Int. J. Biol. Macromol. 2023, 235, 123830.

[37] W. Sun, Z. Zhang, M. Wang, J. Zeng, L. Feng, X. Wang, Y. Hu, C. Ma, G. Zhou, Small 2025, 21, 2501598.

[38] I. E. Imiete, L. Giannini, L. Tadiello, M. Orlandi, L. Zoia, Cellulose 2023, 30, 8929.

[39] Y. Bai, B. Zhang, L. Chen, Z. Lin, X. Zhang, D. Ge, W. Shi, Y. Sun, Nanoscale Res. Lett. 2018, 13, 287.

[40] J. Ai, K. Li, J. Li, F. Yu, J. Ma, Int. J. Biol. Macromol. 2021, 172, 66.

[41] Y. Yang, L. Shao, J. Wang, W. Wang, C. Su, C. Li, H. Di, J. Ma, Z. Ji, Compos. Commun. 2025, 54, 102267.

[42] Q.-Y. Ni, X.-F. He, J.-L. Zhou, Y.-Q. Yang, Z.-F. Zeng, P.-F. Mao, Y.-H. Luo, J.-M. Xu, B. Jiang, Q. Wu, B. Wang, Y.-Q. Qin, L.-X. Gong, L.-C. Tang, S.-N. Li, J. Mater. Sci. Technol. 2024, 191, 181.

[43] C. Xiong, M. Zhao, T. Wang, J. Han, Y. Zhang, Z. Zhang, X. Ji, Q. Xiong, Y. Ni, J. Mater. Sci. Technol. 2025, 205, 53.

[44] Q. Wei, Z. Zhang, W. Sun, J. Wu, X. Wang, Y. Yu, X. Cai, X. Zhang, L. Wang, J. Chen, X. Li, G. Zhou, Chem. Eng. J. 2025, 511, 162036.

[45] W. Li, S. Wu, M. Kang, X. Zhang, X. Zhong, H. Qiao, J. Chen, P. Wang, L. Tao, J. Mater. Sci. Technol. 2024, 201, 130.

[46] T. Ke, L. Zhao, X. Fan, H. Gu, J. Mater. Sci. Technol. 2023, 135, 199.

[47] X. He, E. Obeng, X. Sun, N. Kwon, J. Shen, J. Yoon, Mater. Today Bio. 2022, 15, 100329.

[48] H. Montazerian, A. Baidya, R. Haghniaz, E. Davoodi, S. Ahadian, N. Annabi, A. Khademhosseini, P. S. Weiss, ACS Appl. Mater. Interfaces 2021, 13, 40290.

[49] L. Sun, G. Song, Y. Sun, Q. Fu, C. Pan, ACS Appl. Mater. Interfaces 2020, 12, 44777.

[50] P. Zhang, W. Zhang, Z. Wang, X. Wang, Q. Ren, S. Zhang, Y. Wang, L. He, P. Liu, Q. Zhang, Z. Shi, eScience 2023, 3, 100184.

[51] J. Yang, Y. Fan, X. Xiong, Q. Jiang, P. Li, J. Jian, L. Chen, Appl. Phys. A Mater. Sci. Process. 2024, 130, 157.

[52] B. Guo, S. He, M. Yao, Z. Tan, X. Li, M. Liu, C. Yu, L. Liang, Z. Zhao, Z. Guo, M. Shi, Y. Wei, H. Zhang, F. Yao, J. Li, Chem. Eng. J. 2023, 461, 142099.

[53] S. Ullah, J. Shen, H.-T. Xu, Chin. Chem. Lett. 2025, 36, 110553.

[54] W. Zhao, D. Zhang, Y. Yang, C. Du, B. Zhang, J Mater Chem A 2021, 9, 22082.

[55] N. Li, J. Peng, W.-J. Ong, T. Ma, Arramel, P. Zhang, J. Jiang, X. Yuan, C. Zhang, Matter 2021, 4, 377.

[56] Y. Oh, J. Choi, J. Shim, S. Y. Kim, J. Ind. Eng. Chem. 2025.

[57] L. Liu, L. Wang, X. Liu, W. Yuan, M. Yuan, Q. Xia, Q. Hu, A. Zhou, Nanomaterials 2021, 11, 889.

[58] W. Yuan, J. Yang, M. Yuan, J. Fan, K. Li, L. Wang, A. Zhou, J. Nanoelectron. Optoelectron. 2021, 3, 1123.

[59] W. Shi, Z. Wang, H. Song, Y. Chang, W. Hou, Y. Li, G. Han, ACS Appl. Mater. Interfaces 2022, 14, 35114.

[60] T. Wang, J. Wang, Z. Li, M. Yue, X. Qing, P. Zhang, X. Liao, Z. Fan, S. Yang, J. Appl. Polym. Sci. 2022, 139, 51627.

[61] W. Zhang, J. Y. Wen, M. G. Ma, M. F. Li, F. Peng, J. Bian, J. Mater. Res. Technol. 2021, 14, 555.

[62] Q. Jiao, L. Cao, Z. Zhao, H. Zhang, J. Li, Y. Wei, Biomacromolecules 2021, 22, 1220.

[63] D. Chen, X. Zhao, X. Wei, J. Zhang, D. Wang, H. Lu, P. Jia, ACS Appl. Mater. Interfaces 2020, 12, 53247.

[64] J. Song, S. Chen, L. Sun, Y. Guo, L. Zhang, S. Wang, H. Xuan, Q. Guan, Z. You, Adv. Mater. 2020, 32, 1906994.

[65] J. Fan, M. Yuan, L. Wang, Q. Xia, H. Zheng, A. Zhou, Nano Energy 2023, 105, 107973.

[66] D. Thakur, S. Seo, J. Hyun, J. Ind. Eng. Chem. 2023, 123, 220.

[67] Q. Wei, W. Sun, Z. Zhang, G. Zhou, Z. Zhang, Int. J. Biol. Macromol. 2025, 284, 138162.

[68] J. Lin, Z. Zhang, X. Lin, X. Cai, S. Fu, X. Fang, Y. Ding, X. Wang, G. Sèbe, G. Zhou, Adv. Funct. Mater. 2024, 34, 2314231.

[69] L. Li, X. Wang, Y. Hu, W. Sun, Y. Ding, N. He, G. Zhou, Z. Zhang, ACS Sustain. Chem. Eng. 2024, 12, 17566.

[70] Z. Zhang, Z. Zhang, T. Chang, J. Wang, X. Wang, G. Zhou, Chem. Eng. J. 2022, 428, 131164.

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2025 The Author(s). Energy & Environmental Materials published by John Wiley & Sons Australia, Ltd on behalf of Zhengzhou University.