Future Lithium-based Batteries

From smartphones to electric vehicles, Li-ion batteries have revolutionized our daily lives. Here, we discuss the most important aspects that have enabled lithium-ion batteries to thrive, and introduce some of our articles that contribute to the evolution of these devices.

The 2019 Nobel Prize in Chemistry has been awarded to John B. Goodenough, M. Stanley Whittingham and Akira Yoshino for their contributions in the development of lithium-ion batteries, a technology that has revolutionized our way of life. Here we look back at the milestone discoveries that have shaped the modern lithium-ion batteries for inspirational insights to guide future breakthroughs.

It would be unwise to assume ‘conventional’ lithium-ion batteries are approaching the end of their era and so we discuss current strategies to improve the current and next generation systems, where a holistic approach will be needed to unlock higher energy density while also maintaining lifetime and safety. We end by briefly reviewing areas where fundamental science advances will be needed to enable revolutionary new battery systems.

The 2019 Nobel Prize in Chemistry has been awarded to a trio of pioneers of the modern lithium-ion battery. Here, Professor Arumugam Manthiram looks back at the evolution of cathode chemistry, discussing the three major categories of oxide cathode materials with an emphasis on the fundamental solid-state chemistry that has enabled these advances.

The development of high performing metal-ion batteries require guidelines to build improved electrodes and electrolytes. Here, the authors review the current state-of-the-art in the rational design of battery materials by exploiting the interplay between composition, crystal structure and electrochemical properties.

A reversible oxygen redox process contributes extra capacity and understanding this behavior is of high importance. Here, aided by resonant inelastic X-ray scattering, the authors reveal the distinctive anionic oxygen activity of battery electrodes with different transition metals.

Electrochemical processes induce thermo-mechanical effects that mediate battery performance. Here the authors directly visualize cracking dynamics in a thermally perturbed, delithiated LiNi_0.6Mn_0.2Co_0.2O₂ cathode to demonstrate coupling between thermal, mechanical and electrochemical factors.

For high-energy lithium-sulfur batteries, a dense electrode with low porosity is desired to minimize electrolyte intake, parasitic weight, and cost. Here the authors show the impact of porosity on the performance of lithium-sulfur batteries and reveal the mechanism through analytical modeling.

The electrode/electrolyte interface plays a critical role in a Li-ion battery. Here the authors report that Al doping can tailor the interfacial reactions to lead to enhanced structural stability and cyclability of cathode. Al dopants form not only lattice solid solution but also Al₂O₃ islands on the surface.

Practical application of high-energy-density lithium-rich materials remains a challenge due to issues including voltage fade and poor energy efficiency. Here the authors report a novel densified phase together with a trick to recover capacity in these materials that could help in curing their practical limitations.

Developing understanding of degradation phenomena in nickel rich cathodes is under intense investigation. Here the authors use learning-assisted statistical analysis and experiment-informed mathematical modelling to resolve the microstructure of a Ni-rich NMC composite cathode.

The formation of lithium dendrites remains a great challenge to lithium metal batteries. Here the authors show an anode design to laterally direct the dendrite growth inside the compartments, providing a feasible post-mortem solution to batteries with lithium dendrites already present.

The dendrite growth of alkali metal anodes leads to charge/discharge cycling instability. Here, the authors show that electrochemical polishing can yield near-perfect anodes of three alkali metals by constructing smooth and thin solid-electrolyte interphase layers.

Rechargeable lithium metal batteries could offer a major leap in energy capacity but suffer from the electrolyte reactivity and dendrite growth. Here the authors apply neutron depth profiling to provide quantitative insight into the evolution of the Li-metal morphology during plating and stripping.

The lithium metal is a promising anode material for batteries; however, the growth of dendrite and its instability against moisture are two technical challenges. Here the authors address both issues by introducing a bifunctional layer consisting of hydrophobic graphite fluoride and lithium fluoride.

Understanding the solid–electrolyte interphase (SEI) is key to developing safe dendrite-free lithium batteries. Here, by exploiting the electrons in lithium metal to selectively hyperpolarise the NMR signals, the authors reveal the chemistry and spatial distribution of species at the metal–SEI interface.

Interface chemistry is essential for highly reversible lithium-metal batteries. Here the authors investigate amide-based electrolyte that lead to desirable interface species, resulting in dense Li-metal plating and top-down Li-metal stripping, responsible for the highly reversible cycling.

Solid-state electrolytes may improve the performance of batteries; however, many are unstable towards metallic lithium, and little is known about the chemical evolution of the interfaces that form during cycling. Here, the authors use an operando method to map the formation and evolution of a solid-electrolyte interphase during cycling.

All-solid-state batteries could deliver high energy densities without using organic liquid electrolytes. Here the authors report a complex hydride Li-ion conductor 0.7Li(CB₉H₁₀)–0.3Li(CB₁₁H₁₂) that exhibits impressive ionic conductivity and other electrochemical characteristics in an all-solid-state cell.

Glasses are promising electrolytes for solid-state lithium batteries; however, due to their amorphous structure, the ionic conduction mechanism remains poorly understood. Here, atomic-scale modeling reveals that lithium migration occurs via concerted hopping of Li-ions coupled to quasi-permanent rotations of tetrahedral anions.

While the impetus to develop lithium metal solid-state batteries is clear, identifying a practical manufacturing process is challenging. Herewith, authors study the underlying mechanisms controlling in-situ anode formation that could enable viable lithium-free manufacturing.

Formation of insulating lithium carbonate on surface of lithium garnets hinders their application as solid electrolyte in lithium ion batteries. Here the authors explore a scalable sintering approach to utilize the undesired Li₂CO₃ and improve the active material-electrolyte interface within cathodes.

Solid state battery is regarded as one of the most promising next generation energy storage systems due to high safety and high energy density. Here, authors demonstrate the importance of interfacial local environment in polycrystalline cathodes for electrochemical reactions in solid-state batteries.