Dr Xuhui Yao

Rational design of the morphology and complementary compounding of electrode materials have contributed substantially to improving battery performance, yet the capabilities of conventional electrode materials have remained limited in some key parameters including energy and power density, cycling stability, etc. because of their intrinsic properties, especially the restricted thermodynamics of reactions and the inherent slow diffusion dynamics induced by the crystal structures. In contrast, preintercalation of ions or molecules into the crystal structure with/without further lattice reconstruction could provide fundamental optimizations to overcome these intrinsic limitations. In this Perspective, we discuss the essential optimization mechanisms of preintercalation in improving electronic conductivity and ionic diffusion, inhibiting “lattice breathing” and screening the carrier charge. We also summarize the current challenges in preintercalation and offer insights on future opportunities for the rational design of preintercalation electrodes in next-generation rechargeable batteries.

The constant increase in global energy demand and stricter environmental standards are calling for advanced energy storage technologies that can store electricity from intermittent renewable sources such as wind, solar, and tidal power, to allow the broader implementation of the renewables. The grid-oriented sodium-ion batteries, potassium ion batteries and multivalent ion batteries are cheaper and more sustainable alternatives to Li-ion, although they are still in the early stages of development. Additional optimisation of these battery systems is required, to improve the energy and power density, and to solve the safety issues caused by dendrites growth in anodes. Electrolyte, one of the most critical components in these batteries, could significantly influence the electrochemical performances and operations of batteries. In this review, the definitions and influences of three critical components (salts, solvents, and additives) in electrolytes are discussed. The significant advantages, challenges, recent progress and future optimisation directions of various electrolytes for monovalent and multivalent ions batteries (i.e. organic, ionic liquid and aqueous liquid electrolytes, polymer and inorganic solid electrolytes) are summarised to guide the practical application for grid-oriented batteries.

Despite the long-established rocking-chair theory of lithium-ion batteries (LIBs), developing novel characterization methodology with higher spatiotemporal resolution facilitates a better understanding of the solid electrolyte interphase studies to shape the reaction mechanisms. In this work, we develop a Xenon ion plasma focused ion beam (Xe+ PFIB)-based characterization technique to probe the cross-sectional interface of both ternary cathode and graphite anode electrodes, with the focus on revealing the chemical composition and distribution underneath the electrode surface by in-depth analysis of secondary ions. Particularly, the lithium fluoride is detected in the pristine cathode prior to contact with the electrolyte, reflecting that the electrode degradation is in the form of the loss of lithium inventory during electrode preparation. This degradation is related to the hydrolysis of the cathode material and the decomposition of the PVDF binder. Through the quantitative analysis of the transition-metal degradation products, manganese is found to be the dominant element in the newly formed inactive fluoride deposition on the cathode, while no transition metal signal can be found inside the anode electrode. These insights at high resolution implemented via a PFIB-based characterization technique not only enrich the understanding of the degradation mechanism in the LIBs but also identify and enable a high-sensitivity methodology to obtain the chemical survey at the subsurface, which will help remove the capacity-fade observed in most LIBs.

Voltage plateau is an eigenvalue associated with the electrochemical reaction and hence a feasible tool for real-time detection of the state of charge in batteries. The variation of voltage plateau generally relates to the degradation of batteries, indicating the changes in the structure and/or the composition of electrode materials. In this work, we focus on a voltage plateau variation in a bismuth-potassium cell, investigating the electrode evolutions by two in situ methodologies. The phase transition reveals an intermediate phase in the reaction process, featuring a very limited but constant mass fraction. An irreversible structural collapse that follows leads to the exponential magnifying of the intermediate phase, taking responsibility for the distinct diffraction peaks and new voltage plateaus in the following cycles. This reaction mechanism builds the bridge between voltage plateau variation and electrode evolution, highlighting a combined effect of intermediate phase and structural collapse.

Electronic skins (e-skins), which can seamlessly adapt and adhere to the body to mimic the functionality of human skin, are a rapidly emerging research area. Such e-skins have the potential to revolutionize artificial prosthetics, robotics, human-machine interfacing, and health monitoring applications. Powering the e-skin is a critical challenge at present due to strict performance criteria, including flexibility, stretchability, mobility, and autonomous operation. One of the most promising approaches to overcome some of these challenges is to scavenge energy from the human body's movements and its surrounding environment. This paper outlines some of the key potential developments that enable energy harvesting through mechanical, thermal affects, and low light sources, as well as energy management and storage technologies, which could lead toward the construction of autonomous e-skin modules and self-powered sensing systems.

Miniaturized flexible photo-rechargeable systems show bright prospects for wide applications in internet of things, self-powered health monitoring and emergency electronics. However, conventional systems still suffer from complex manufacturing processes, slow photo-charging and discharging rate, and mismatch between photovoltaic and energy storage components in size, mechanics and voltage, etc. Here, we demonstrate a facile inkjet printing and electrodeposition approach for fabricating a highly integrated flexible photo-rechargeable system by combining stable and ultra-high-rate quasi-solid-state Zn-MnO2 micro-batteries (ZMBs) with flexible perovskite solar cells (FPSCs). In particular, Ni protective layer is first introduced into ZMBs to stabilize battery configuration and facilitate enhanced electrochemical performance. The optimized ZMB exhibits ultrahigh volumetric energy density of 148 mWh cm−3 (16.3 μWh cm−2) and power density of 55 W cm−3 (6.1 mW cm−2) at the current density of 400 C (5 mA cm−2), enabling them comparable with the state-of-the-art micro-batteries or supercapacitors fabricated by conventional methods. The embedded FPSCs show excellent photovoltaic performance, sufficient to charge ZMBs and create a self-charging system capable to offer energy autonomy in miniaturized wearable electronics. The integrated systems can achieve an ultrafast photo-charging within 30 s, with sufficient energy to power other functional electronics (e.g., LED bulb and pressure sensor) for tens of minutes. This prototype offers a promising scheme for next-generation miniaturized flexible photo-rechargeable systems.