Tough MXene-Cellulose Nanofibril Ionotronic Dual-Network Hydrogel Films for Stable Zinc Anodes

Developing ionotronic interface layers for zinc anodes with superior mechanical integrity is one of the efficient strategies to suppress the growth of zinc dendrites in favor of the cycling stability of aqueous zinc-ion batteries (AZIBs). Herein, we assembled robust 2D MXene-based hydrogel films cross-linked by 1D cellulose nanofibril (CNF) dual networks, acting as interface layers to stabilize Zn anodes. The MXene-CNF hydrogel films integrated multifunctionalities, including a high in-plane toughness of 18.39 MJ m<sup>-3</sup>, high in-plane/out-of-plane elastic modulus of 0.85 and 3.65 GPa, mixed electronic/ionic (ionotronic) conductivity of 1.53 S cm<sup>-1</sup> and 0.52 mS cm<sup>-1</sup>, and high zincophilicity with a high binding energy (1.33 eV) and low migration energy barrier (0.24 eV) for Zn<sup>2+</sup>. These integrated multifunctionalities, endowed with coupled multifield effects, including strong stress confinement and uniform ionic/electronic field distributions on Zn anodes, effectively suppressed dendrite growth, as proven by experiments and simulations. An example of the MXene-CNF|Zn showed a reduced nucleation overpotential of 19 mV, an extended cycling life of over 2700 h in Zn||Zn cells, and a high capacity of 323 mAh g<sup>-1</sup> in Zn||MnO<sub>2</sub> cells, compared with bare Zn. This work offers an approach for exploring mechanically robust 1D/2D ionotronic hydrogel interface layers to stabilize the Zn anodes of AZIBs.

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Publication Details

Journal
ACS Nano
Published
2025-03-25
DOI
https://doi.org/10.1021/acsnano.5c01497
Citations
35
Primary Topic
Advanced battery technologies research
Type
article
Field-Weighted Citation Impact
25.57

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article

Tough MXene-Cellulose Nanofibril Ionotronic Dual-Network Hydrogel Films for Stable Zinc Anodes

Sheng Chen, Huanlei Wang, Kyle Matthews, Weiqian Tian et al.
35 citations
ACS Nano
Advanced battery technologies research
25.57
article

Tough MXene-Cellulose Nanofibril Ionotronic Dual-Network Hydrogel Films for Stable Zinc Anodes

Sheng Chen, Huanlei Wang, Kyle Matthews, Weiqian Tian, Yury G. Gogotsi, Minghua Huang, Mahiar Max Hamedi, Feng Xu, Teng Zhang, Jowan Rostami, Liming Zhang, Jingwei Chen, Wenjie Fan, Mengyu Liu, Lars Wågberg, Yue Zhu, Jingyi Wu
article en
35 citations

Abstract

Developing ionotronic interface layers for zinc anodes with superior mechanical integrity is one of the efficient strategies to suppress the growth of zinc dendrites in favor of the cycling stability of aqueous zinc-ion batteries (AZIBs). Herein, we assembled robust 2D MXene-based hydrogel films cross-linked by 1D cellulose nanofibril (CNF) dual networks, acting as interface layers to stabilize Zn anodes. The MXene-CNF hydrogel films integrated multifunctionalities, including a high in-plane toughness of 18.39 MJ m<sup>-3</sup>, high in-plane/out-of-plane elastic modulus of 0.85 and 3.65 GPa, mixed electronic/ionic (ionotronic) conductivity of 1.53 S cm<sup>-1</sup> and 0.52 mS cm<sup>-1</sup>, and high zincophilicity with a high binding energy (1.33 eV) and low migration energy barrier (0.24 eV) for Zn<sup>2+</sup>. These integrated multifunctionalities, endowed with coupled multifield effects, including strong stress confinement and uniform ionic/electronic field distributions on Zn anodes, effectively suppressed dendrite growth, as proven by experiments and simulations. An example of the MXene-CNF|Zn showed a reduced nucleation overpotential of 19 mV, an extended cycling life of over 2700 h in Zn||Zn cells, and a high capacity of 323 mAh g<sup>-1</sup> in Zn||MnO<sub>2</sub> cells, compared with bare Zn. This work offers an approach for exploring mechanically robust 1D/2D ionotronic hydrogel interface layers to stabilize the Zn anodes of AZIBs.

ACS NanoVol. 19(13)
Qingdao University (CN), Beijing Forestry University (CN), Nanomaterials Research (United States) (US), Division of Materials Science and Engineering (AU), Ocean University of China (CN), Drexel University (US), KTH Royal Institute of Technology (SE)
National Natural Science Foundation of China, Vetenskapsrådet, Natural Science Foundation of Shandong Province, Taishan Scholar Project of Shandong Province, Higher Education Discipline Innovation Project, Fundamental Research Funds for the Central Universities
Openalex Percentile: Top 0%
Advanced battery technologies research
25.57
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