Liu Mengyu, Zhang Liming, Rostami Jowan, Zhang Teng, Matthews Kyle, Chen Sheng, Fan Wenjie, Zhu Yue, Chen Jingwei, Huang Minghua, Wu Jingyi, Wang Huanlei, Hamedi Mahiar Max, Xu Feng, Tian Weiqian, Wågberg Lars, Gogotsi Yury
School of Materials Science and Engineering, Ocean University of China, Qingdao 266100, China.
College of Textile and Clothing, Qingdao University, Qingdao 266071, China.
ACS Nano. 2025 Apr 8;19(13):13399-13413. doi: 10.1021/acsnano.5c01497. Epub 2025 Mar 25.
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, 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 and 0.52 mS cm, and high zincophilicity with a high binding energy (1.33 eV) and low migration energy barrier (0.24 eV) for Zn. 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 in Zn||MnO 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.
开发具有优异机械完整性的锌负极离子电子界面层是抑制锌枝晶生长以利于水系锌离子电池（AZIBs）循环稳定性的有效策略之一。在此，我们组装了由一维纤维素纳米纤维（CNF）双网络交联的坚固二维MXene基水凝胶薄膜，作为稳定锌负极的界面层。MXene-CNF水凝胶薄膜具有多种功能，包括18.39 MJ m的高面内韧性、0.85和3.65 GPa的高面内/面外弹性模量、1.53 S cm和0.52 mS cm的混合电子/离子（离子电子）电导率，以及对锌具有高亲锌性，其对锌的结合能高（1.33 eV）且迁移能垒低（0.24 eV）。这些集成的多功能性赋予了耦合多场效应，包括对锌负极的强应力限制和均匀的离子/电子场分布，有效地抑制了枝晶生长，实验和模拟均证明了这一点。与裸锌相比，MXene-CNF|Zn的一个例子显示其成核过电位降低了19 mV，在Zn||Zn电池中的循环寿命延长至超过2700 h，在Zn||MnO电池中的容量高达323 mAh g。这项工作为探索机械坚固的一维/二维离子电子水凝胶界面层以稳定AZIBs的锌负极提供了一种方法。
