Insights on rational design and energy storage mechanism of Mn-based cathode materials towards high performance aqueous zinc-ion batteries

Aqueous zinc‐ion batteries (AZIBs) may have applications in macroscale energy storage on account of their advantages of high‐safety, cost‐effectiveness, and ecofriendliness. As a promising application, flexible quasi‐solid‐state AZIBs (FQAZIBs) can withstand mechanical deformation, and can act as favorable power supply devices for wearable electronics. As FQAZIBs are one of the most exciting and rapidly ongoing topics among aqueous batteries, it is critical yet timely to summarize the latest development in this field, providing the much‐needed guidance for the fabrication of FQAZIBs. In this review, the recent progress and rational design strategies for FQAZIBs from mechanisms, design principles, and applications are systematically presented. First, the energy storage and flexible mechanisms of FQAZIBs are illuminated in detail. Subsequently, the design philosophies of FQAZIBs are also systematically elucidated. Moreover, the latest progress and practical applications of FQAZIBs in wearable electronics are reviewed in detail according to various functions such as compressibility, stretchability, electrochromic ability, anti‐freezing ability, self‐healing ability, self‐charging properties, photodetecting function, shape memory, biodegradability, and actuated function. Finally, some applications and promising prospects in the research area of FQAZIBs are demonstrated to supply guidelines on the exploitation of their practical applications.

Flexible Quasi‐Solid‐State Aqueous Zinc‐Ion Batteries: Design Principles, Functionalization Strategies, and Applications

Flexible aqueous batteries have been thriving with the growing demand for wearable and portable electrical devices. In particular, flexible aqueous multivalent ion batteries (FAMIBs), the charge carriers of which include Zn2+, Al3+, Mg2+, and Ca2+, have great potential for development owing to their high safety, high elemental abundance in the Earth's crust, and a multi-electron redox mechanism with a high theoretical specific capacity. Therefore, for a comprehensive understanding of this developing field, it is necessary to summarize the recent research progress of FAMIBs in a timely manner. Herein, the advancements of the state-of-the-art FAMIBs are reviewed, and the prospects toward this field are also proposed. This study focuses on the rational material and configuration design for FAMIBs in recent studies to achieve high battery performances under deformation conditions, which is elaborated on by classification of the anode, cathode, hydrogel electrolyte, and configurations of FAMIBs. Besides, the electrochemical performance of FAMIBs under flexible conditions is also reviewed from the perspective of their working voltage, specific capacity, and cycling stability. Finally, the approaches to improve the performance of FAMIBs are comprehensively evaluated, followed by the outlook on the challenges and opportunities in future development of FAMIBs. 

Recent progress of flexible aqueous multivalent ion batteries

To promote the real application of zinc‐ion batteries (ZIBs), reconciling the high mass loading and gravimetric performance of MnO2 electrodes is of paramount importance. Herein, the rational regulation of 3D‐printed carbon microlattices (3DP CMs) enabling an ultrathick MnO2 electrode with well‐maintained gravimetric capacities is demonstrated. The 3DP CMs made of graphene and carbon nanotubes (CNTs) are fabricated by direct ink 3D printing and subsequent high‐temperature annealing. 3D printing enables a periodic structure of 3DP CMs, while the thermal annealing contributes to high conductivity and defective surfaces. Due to these structural merits, uniform electrical field distribution and facilitated MnO2 deposition over the 3DP CMs are permitted. The optimal electrode with MnO2 loaded on the 3DP CMs can achieve a record‐high specific capacity of 282.8 mAh g−1 even at a high mass loading of 28.4 mg cm−2 and high ion transfer dynamics, which reconciles the loading mass and gravimetric performance. As a result, the aqueous ZIBs based on the 3DP CMs loaded MnO2 afford an outstanding performance superior to most of the previous reports. This study reveals the essential role of interaction between active materials and current collectors, providing an alternative strategy for designing high‐performance energy storage devices.

Reconciling Mass Loading and Gravimetric Performance of MnO2 Cathodes by 3D‐Printed Carbon Structures for Zinc‐Ion Batteries

The flexible electronics attract great attentions with the enhanced flexibility of electronic devices, which could be used as flexible sensor, flexible battery, electronic skin, soft robot and so on. The...

Fabricating Flexible Conductive Structures by Printing Techniques and Printable Conductive Materials

2D metal patterns transformed from 3D printed stamps for flexible Zn//MnO2 in-plane micro-batteries

Paper and textile are two ideal carriers in wearable and printed electronics because of their flexibility and low price. However, the porous and fibrous structures restrain their use in printed ele...

Polydimethylsiloxane-Assisted Catalytic Printing for Highly Conductive, Adhesive, and Precise Metal Patterns Enabled on Paper and Textiles.

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2D metal patterns transformed from 3D printed stamps for flexible Zn//MnO2 in-plane micro-batteries

Polydimethylsiloxane-Assisted Catalytic Printing for Highly Conductive, Adhesive, and Precise Metal Patterns Enabled on Paper and Textiles.