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.

2020, Tang, Hongmei, Karnaushenko, Dmitriy D., Neu, Volker, Gabler, Felix, Wang, Sitao, Liu, Lixiang, Li, Yang, Wang, Jiawei, Zhu, Minshen, Schmidt, Oliver G.

Miniaturization of batteries lags behind the success of modern electronic devices. Neither the device volume nor the energy density of microbatteries meets the requirement of microscale electronic devices. The main limitation for pushing the energy density of microbatteries arises from the low mass loading of active materials. However, merely pushing the mass loading through increased electrode thickness is accompanied by the long charge transfer pathway and inferior mechanical properties for long‐term operation. Here, a new spiral microelectrode upon stress‐actuation accomplishes high mass loading but short charge transfer pathways. At a small footprint area of around 1 mm2, a 21‐fold increase of the mass loading is achieved while featuring fast charge transfer at the nanoscale. The spiral microelectrode delivers a maximum area capacity of 1053 µAh cm−2 with a retention of 67% over 50 cycles. Moreover, the energy density of the cylinder microbattery using the spiral microelectrode as the anode reaches 12.6 mWh cm−3 at an ultrasmall volume of 3 mm3. In terms of the device volume and energy density, the cylinder microbattery outperforms most of the current microbattery technologies, and hence provides a new strategy to develop high‐performance microbatteries that can be integrated with miniaturized electronic devices.