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Lithium-ion batteries have had a profound impact on our daily life, but inherent limitations make it difficult for Li-ion chemistries to meet the growing demands for portable electronics, electric vehicles and grid-scale energy storage. Therefore, chemistries beyond Li-ion are currently being investigated and need to be made viable for commercial applications. The use of metallic Li is one of the most favoured choices for next-generation Li batteries, especially Li-S and Li-air systems. After falling into oblivion for several decades because of safety concerns, metallic Li is now ready for a revival, thanks to the development of investigative tools and nanotechnology-based solutions. In this Review, we first summarize the current understanding on Li anodes, then highlight the recent key progress in materials design and advanced characterization techniques, and finally discuss the opportunities and possible directions for future development of Li anodes in applications.

Reviving the lithium metal anode for high-energy batteries

There is still an ongoing effort to search for sustainable, clean and highly efficient energy generation to satisfy the energy needs of modern society. Among various advanced technologies, electrocatalysis for the oxygen evolution reaction (OER) plays a key role and numerous new electrocatalysts have been developed to improve the efficiency of gas evolution. Along the way, enormous effort has been devoted to finding high-performance electrocatalysts, which has also stimulated the invention of new techniques to investigate the properties of materials or the fundamental mechanism of the OER. This accumulated knowledge not only establishes the foundation of the mechanism of the OER, but also points out the important criteria for a good electrocatalyst based on a variety of studies. Even though it may be difficult to include all cases, the aim of this review is to inspect the current progress and offer a comprehensive insight toward the OER. This review begins with examining the theoretical principles of electrode kinetics and some measurement criteria for achieving a fair evaluation among the catalysts. The second part of this review acquaints some materials for performing OER activity, in which the metal oxide materials build the basis of OER mechanism while non-oxide materials exhibit greatly promising performance toward overall water-splitting. Attention of this review is also paid to in situ approaches to electrocatalytic behavior during OER, and this information is crucial and can provide efficient strategies to design perfect electrocatalysts for OER. Finally, the OER mechanism from the perspective of both recent experimental and theoretical investigations is discussed, as well as probable strategies for improving OER performance with regards to future developments.

Electrocatalysis for the oxygen evolution reaction: recent development and future perspectives

The lithium metal battery is strongly considered to be one of the most promising candidates for high-energy-density energy storage devices in our modern and technology-based society. However, uncontrollable lithium dendrite growth induces poor cycling efficiency and severe safety concerns, dragging lithium metal batteries out of practical applications. This review presents a comprehensive overview of the lithium metal anode and its dendritic lithium growth. First, the working principles and technical challenges of a lithium metal anode are underscored. Specific attention is paid to the mechanistic understandings and quantitative models for solid electrolyte interphase (SEI) formation, lithium dendrite nucleation, and growth. On the basis of previous theoretical understanding and analysis, recently proposed strategies to suppress dendrite growth of lithium metal anode and some other metal anodes are reviewed. A section dedicated to the potential of full-cell lithium metal batteries for practical applicatio...

Toward Safe Lithium Metal Anode in Rechargeable Batteries: A Review.

Civilization continues to be transformed by our ability to harness energy beyond human and animal power. A series of industrial and agricultural revolutions have allowed an increasing fraction of the world population to heat and light their homes, fertilize and irrigate their crops, connect to one another and travel around the world. All of this progress is fuelled by our ability to find, extract and use energy with ever increasing dexterity. Research in materials science is contributing to progress towards a sustainable future based on clean energy generation, transmission and distribution, the storage of electrical and chemical energy, energy efficiency, and better energy management systems.

The path towards sustainable energy

Stretchable Lithium Metal Anode with Improved Mechanical and Electrochemical Cycling Stability

Li metal chemistry is a promising alternative with a much higher energy density than that of state-of-the-art Li-ion counterparts. However, significant challenges including safety issues and poor cyclability have severely impeded Li metal technology from becoming viable. In recent years, nanotechnologies have become increasingly important in materials design and fabrication for Li metal anodes, contributing to major progress in the field. In this review, we first introduce the main achievements in Li metal battery systems fulfilled by nanotechnologies, particularly regarding Li metal anode design and protection, ultrastrong separator engineering, safety monitoring, and smart functions. Next, we introduce recent studies on nanoscale Li nucleation/deposition. Finally, we discuss possible future research directions. We hope this review delivers an overall picture of the role of nanoscale approaches in the recent progress of Li metal battery technology and inspires more research in the future. 
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Nanoscale perspective: Materials designs and understandings in lithium metal anodes

Solid-state lithium (Li) metal batteries are prominent among next-generation energy storage technologies due to their significantly high energy density and reduced safety risks. Previously, solid electrolytes have been intensively studied and several materials with high ionic conductivity have been identified. However, there are still at least three obstacles before making the Li metal foil-based solid-state systems viable, namely, high interfacial resistance at the Li/electrolyte interface, low areal capacity, and poor power output. The problems are addressed by incorporating a flowable interfacial layer and three-dimensional Li into the system. The flowable interfacial layer can accommodate the interfacial fluctuation and guarantee excellent adhesion at all time, whereas the three-dimensional Li significantly reduces the interfacial fluctuation from the whole electrode level (tens of micrometers) to local scale (submicrometer) and also decreases the effective current density for high-capacity and high-power operations. As a consequence, both symmetric and full-cell configurations can achieve greatly improved electrochemical performances in comparison to the conventional Li foil, which are among the best reported values in the literature. Noticeably, solid-state full cells paired with high–mass loading LiFePO 4 exhibited, at 80°C, a satisfactory specific capacity even at a rate of 5 C (110 mA·hour g −1 ) and a capacity retention of 93.6% after 300 cycles at a current density of 3 mA cm −2 using a composite solid electrolyte middle layer. In addition, when a ceramic electrolyte middle layer was adopted, stable cycling with greatly improved capacity could even be realized at room temperature.

https://advances.sciencemag.org/content/advances/3/10/eaao0713.full.pdf

Yayuan Liu

Papers

Stretchable Lithium Metal Anode with Improved Mechanical and Electrochemical Cycling Stability

Nanoscale perspective: Materials designs and understandings in lithium metal anodes

Transforming from planar to three-dimensional lithium with flowable interphase for solid lithium metal batteries

An Interconnected Channel‐Like Framework as Host for Lithium Metal Composite Anodes

A general prelithiation approach for group IV elements and corresponding oxides