2021, Zhu, Minshen, Hu, Junping, Lu, Qiongqiong, Dong, Haiyun, Karnaushenko, Dmitriy D., Becker, Christian, Karnaushenko, Daniil, Li, Yang, Tang, Hongmei, Qu, Zhe, Ge, Jin, Schmidt, Oliver G.

Owing to their high safety and reversibility, aqueous microbatteries using zinc anodes and an acid electrolyte have emerged as promising candidates for wearable electronics. However, a critical limitation that prevents implementing zinc chemistry at the microscale lies in its spontaneous corrosion in an acidic electrolyte that causes a capacity loss of 40% after a ten-hour rest. Widespread anti-corrosion techniques, such as polymer coating, often retard the kinetics of zinc plating/stripping and lack spatial control at the microscale. Here, a polyimide coating that resolves this dilemma is reported. The coating prevents corrosion and hence reduces the capacity loss of a standby microbattery to 10%. The coordination of carbonyl oxygen in the polyimide with zinc ions builds up over cycling, creating a zinc blanket that minimizes the concentration gradient through the electrode/electrolyte interface and thus allows for fast kinetics and low plating/stripping overpotential. The polyimide's patternable feature energizes microbatteries in both aqueous and hydrogel electrolytes, delivering a supercapacitor-level rate performance and 400 stable cycles in the hydrogel electrolyte. Moreover, the microbattery is able to be attached to human skin and offers strong resistance to deformations, splashing, and external shock. The skin-mountable microbattery demonstrates an excellent combination of anti-corrosion, reversibility, and durability in wearables. © 2021 The Authors. Advanced Materials published by Wiley-VCH GmbH

2021, Li, Fei, Li, Yang, Qu, Jiang, Wang, Jinhui, Bandari, Vineeth Kumar, Zhu, Feng, Schmidt, Oliver G.

The rapid development of wearable and portable electronics has dramatically increased the application for miniaturized energy storage components. Stamping micro-supercapacitors (MSCs) with planar interdigital configurations are considered as a promising candidate to meet the requirements. In this review, recent progress of the different stamping materials and various stamping technologies are first discussed. The merits of each material, manufacturing process of each stamping method and the properties of stamping MSCs are scrutinized, respectively. Further insights on technical difficulties and scientific challenges are finally demonstrated, including the limited thickness of printed electrodes, poor overlay accuracy and printing resolution.

2020, Zhu, Minshen, Wang, Xiaojie, Tang, Hongmei, Wang, Jiawei, Hao, Qi, Liu, Lixiang, Li, Yang, Zhang, Kai, Schmidt, Oliver G.

Hydrogels are widely used in flexible aqueous batteries due to their liquid-like ion transportation abilities and solid-like mechanical properties. Their potential applications in flexible and wearable electronics introduce a fundamental challenge: how to lower the freezing point of hydrogels to preserve these merits without sacrificing hydrogels' basic advantages in low cost and high safety. Moreover, zinc as an ideal anode in aqueous batteries suffers from low reversibility because of the formation of insulative byproducts, which is mainly caused by hydrogen evolution via extensive hydration of zinc ions. This, in principle, requires the suppression of hydration, which induces an undesirable increase in the freezing point of hydrogels. Here, it is demonstrated that cooperatively hydrated cations, zinc and lithium ions in hydrogels, are very effective in addressing the above challenges. This simple but unique hydrogel not only enables a 98% capacity retention upon cooling down to −20 °C from room temperature but also allows a near 100% capacity retention with >99.5% Coulombic efficiency over 500 cycles at −20 °C. In addition, the strengthened mechanical properties of the hydrogel under subzero temperatures result in excellent durability under various harsh deformations after the freezing process. © 2019 The Authors. Published by WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim

2021, Li, Yang, Qu, Jiang, Li, Fei, Qu, Zhe, Tang, Hongmei, Liu, Lixiang, Zhu, Minshen, Schmidt, Oliver G.

Rechargeable microbatteries are important power supplies for microelectronic devices. Two essential targets for rechargeable microbatteries are high output energy and minimal footprint areas. In addition to the development of new high-performance electrode materials, the device configurations of microbatteries also play an important role in enhancing the output energy and miniaturizing the footprint area. To make a clear vision on the design principle of rechargeable microbatteries, we firstly summarize the typical configurations of microbatteries. The advantages of different configurations are thoroughly discussed from the aspects of fabrication technologies and material engineering. Towards the high energy output at a minimal footprint area, a revolutionary design for microbatteries is of great importance. In this perspective, we review the progress of fabricating microbatteries based on the rolled-up nanotechnology, a derivative origami technology. Finally, we discussed the challenges and perspectives in the device design and materials optimization.

2021, Weng, Qunhong, Wang, Sitao, Liu, Lixiang, Lu, Xueyi, Zhu, Minshen, Li, Yang, Gabler, Felix, Schmidt, Oliver G.

Independent and well-packaged miniaturized energy storage devices (MESDs) are indispensable as power sources or backup units for integrated circuits and many dispersive electronics applications. Challenges associated with MESD development relate to their low packaged areal energy density and poor battery performance. Here, we propose a compact tube-in-tube battery configuration to overcome the areal energy density and packaging problems in microbatteries. Compact microtubular microelectrodes rolled up from patterned nanomembranes are sealed in an inert glass capillary with a thin tube wall. The resultant tube-in-tube microsized lithium-ion batteries (micro-LIBs), based on various active materials, exhibit very high and scalable packaged areal energy densities up to 605 microampere hours per square centimeter (μAh cm−2) or 313 μWh cm−2 with footprints as small as 0.39–0.79 mm2. This approach is a practical alternative for microbattery microelectrode, packaging, and configuration innovations.