Cellulose-based Ionic Conductive Hydrogels with Tunable Flexibility and Ionic Conductivity for Multifunctional Applications in Flexible Electronics

Ziqian Ye1,2

Yanshuo Yu2,3

Haiyue Miao2,4

Yiyang Liu5,6

Xiaojuan Huang7

Chongyang Zheng7

Xi Zhang8

Xiaobin Fu2

Jun Xu9

Hailong Huang2, Email

Min Ge2

Yisheng Xu1, Email

Yuan Qian2, Email

1State Key Laboratory of Green Chemical Engineering and Industrial Catalysis, State Key Laboratory of Chemical Engineering, School of Chemical Engineering, East China University of Science and Technology, 130 Meilong Road, Shanghai, 200237, China
2State Key Laboratory of Thorium Energy, Shanghai Institute of Applied Physics, Chinese Academy of Science, 2019 Jialuo Road, Shanghai, 201800, China
3College of Science, Shenyang University of Chemical Technology, 11 11th Street, Shenyang, 110142, China
4University of Chinese Academy of Sciences, Beijing, 100049, China
5Photon Science Research Center for Carbon Dioxide, Shanghai Advanced Research Institute, Chinese Academy of Sciences, Shanghai, 201210, China
6State Key Laboratory of Low Carbon Catalysis and Carbon Dioxide Utilization, Shanghai Advanced Research Institute, Chinese Academy of Sciences, Shanghai, 201210, China
7Department of Oral and Maxillofacial-Head & Neck Oncology, Shanghai Ninth People’s Hospital, Shanghai Jiao Tong University School of Medicine, Shanghai, 200011, China
8Public Technology Service Center, Shanghai Institute of Organic Chemistry, Chinese Academy of Sciences, Shanghai, 200062, China
9Large Industrial Reactor Engineering Research Center of Ministry of Education, School of Chemical Engineering, East China University of Science and Technology, 130 Meilong Road, Shanghai, 200237, China

Abstract

Wearable sensors and flexible energy storage devices impose distinct requirements on ionic conductive hydrogels, particularly regarding the balance between flexibility and conductivity. However, existing hydrogels lack a simple and scalable approach to tailor these properties for targeted applications, meeting the requirements of different applications. Here, we propose a strategy to regulate the microstructure of cellulose-based ionic conductive hydrogels (ICH) by leveraging competitive hydration effects between Zn2+ and Li+ ions, enabling single-step performance tuning. When Zn2+ dominates (ICH-1), hydrated ions expand cellulose chain spacing, enhancing ion mobility and yielding good conductivity (18.48 mS·cm-1). The resulting asymmetric flexible capacitor (ICH-1) achieves a 0-2.0 V voltage window, with exceptional energy density (50.6 Wh·kg-1) and power density (1000.1 W·kg-1). Conversely, Li+-dominant ICH-3 exhibits compact cellulose chains, endowing good flexibility (311.84 kPa at 35% strain), ionic conductivity (13.16 mS·cm-1) and sensitive electromechanical performance (GF=2.78). This enables its application as a biomimetic e-skin sensor for real-time human motion monitoring and human-computer interaction. Our method addresses the limitations of conventional ICH fabrication, offering scalable production and demonstrating significant industrial potential.