Li-ion battery materials: present and future

All-solid-state lithium batteries (ASSLBs) have the potential to revolutionize battery systems for electric vehicles due to their benefits in safety, energy density, packaging, and operable temperature range. As the key component in ASSLBs, inorganic lithium-ion-based solid-state electrolytes (SSEs) have attracted great interest, and advances in SSEs are vital to deliver the promise of ASSLBs. Herein, a survey of emerging SSEs is presented, and ion-transport mechanisms are briefly discussed. Techniques for increasing the ionic conductivity of SSEs, including substitution and mechanical strain treatment, are highlighted. Recent advances in various classes of SSEs enabled by different preparation methods are described. Then, the issues of chemical stabilities, electrochemical compatibility, and the interfaces between electrodes and SSEs are focused on. A variety of research addressing these issues is outlined accordingly. Given their importance for next-generation battery systems and transportation style, a perspective on the current challenges and opportunities is provided, and suggestions for future research directions for SSEs and ASSLBs are suggested.

Promises, Challenges, and Recent Progress of Inorganic Solid-State Electrolytes for All-Solid-State Lithium Batteries

An all-solid-state battery with a lithium metal anode is a strong candidate for surpassing conventional lithium-ion battery capabilities. However, undesirable Li dendrite growth and low Coulombic efficiency impede their practical application. Here we report that a high-performance all-solid-state lithium metal battery with a sulfide electrolyte is enabled by a Ag–C composite anode with no excess Li. We show that the thin Ag–C layer can effectively regulate Li deposition, which leads to a genuinely long electrochemical cyclability. In our full-cell demonstrations, we employed a high-Ni layered oxide cathode with a high specific capacity (>210 mAh g−1) and high areal capacity (>6.8 mAh cm−2) and an argyrodite-type sulfide electrolyte. A warm isostatic pressing technique was also introduced to improve the contact between the electrode and the electrolyte. A prototype pouch cell (0.6 Ah) thus prepared exhibited a high energy density (>900 Wh l−1), stable Coulombic efficiency over 99.8% and long cycle life (1,000 times). Solid-state Li metal batteries represent one of the most promising rechargeable battery technologies. Here the authors report an exceptional high-performance prototype solid-state pouch cell made of a sulfide electrolyte, a high-Ni layered oxide cathode and, in particular, a silver–carbon composite anode with no excess Li.

High-energy long-cycling all-solid-state lithium metal batteries enabled by silver–carbon composite anodes

Solid-state batteries have been attracting wide attention for next generation energy storage devices due to the probability to realize higher energy density and superior safety performance compared with the state-of-the-art lithium ion batteries. However, there are still intimidating challenges for developing low cost and industrially scalable solid-state batteries with high energy density and stable cycling life for large-scale energy storage and electric vehicle applications. This review presents an overview on the scientific challenges, fundamental mechanisms, and design strategies for solid-state batteries, specifically focusing on the stability issues of solid-state electrolytes and the associated interfaces with both cathode and anode electrodes. First, we give a brief overview on the history of solid-state battery technologies, followed by introduction and discussion on different types of solid-state electrolytes. Then, the associated stability issues, from phenomena to fundamental understandings, are intensively discussed, including chemical, electrochemical, mechanical, and thermal stability issues; effective optimization strategies are also summarized. State-of-the-art characterization techniques and in situ and operando measurement methods deployed and developed to study the aforementioned issues are summarized as well. Following the obtained insights, perspectives are given in the end on how to design practically accessible solid-state batteries in the future.

Approaching Practically Accessible Solid-State Batteries: Stability Issues Related to Solid Electrolytes and Interfaces

The need for lighter, thinner, and smaller products makes lithium ion batteries popular power sources for applications such as mobile phones, laptop computers, digital cameras, electric vehicles, and hybrid electric vehicles. For high power applications, the development of high capacity and high voltage electrode materials is in progress. Battery performance and safety issues are also related to the properties of the electrolytes used. To improve the properties of the electrolytes, small amounts of other components, known as electrolyte additives, are incorporated. This paper reviews the recent progress in electrolyte additives used to improve performance and other properties, such as safety. This review classifies the additives based on their functions and their effects on specific electrode materials focusing on electrodes under current development. From anodes: carbonaceous electrodes, silicon, tin and Li4Ti5O12; from layered cathodes: LiCoO2, Li-rich and LiNiyMnyCo1−2yO2 (NMC); from spinel: LiMn2O4, and from olivine: LiFePO4 are selected. We believe that this approach will help readers easily identify and understand the additives suitable for their target materials.

Electrolyte additives for lithium ion battery electrodes: progress and perspectives

A rocking chair type all-solid-state lithium ion battery adopting Li2O–ZrO2 coated LiNi0.8Co0.15Al0.05O2 and a sulfide based electrolyte

Garnet related lithium ion conductor processed by spark plasma sintering for all solid state batteries

Does the Li4Ti5O12 electrode need a carbon additive in lithium-ion batteries? We answered this question in our previous work by showing that the partially reduced Ti4+ on the surface of Li4Ti5O12 could provide enough electronic conductivity to initiate the electrochemical process. In this work, we discuss the generally accepted fact that a solid electrolyte interphase (SEI) is hardly formed on the surface of the Li4Ti5O12 electrode owing to its high redox potential by using the carbon-free Li4Ti5O12 electrode to exclude the influences of carbon. In contrast to the previous argument, Li4Ti5O12 was found to have certain reactivity towards electrolytes at room and high temperature (60 °C). Moreover, in the presence of carbon in the electrode (i.e. the conventional electrode formulation), the reactivity of the electrode towards an electrolyte was significantly increased at high temperatures. These results were discussed based on surface analyses and electrode morphology observation before and after cycling, and correlated with the electrochemical performance.

Is Li4Ti5O12 a solid-electrolyte-interphase-free electrode material in Li-ion batteries? Reactivity between the Li4Ti5O12 electrode and electrolyte

Characteristics of ABO3 and A2BO4 (ASm, Sr; BCo, Fe, Ni) samarium oxide system as cathode materials for intermediate temperature-operating solid oxide fuel cell

Seung-Wook Baek

Papers

A rocking chair type all-solid-state lithium ion battery adopting Li2O–ZrO2 coated LiNi0.8Co0.15Al0.05O2 and a sulfide based electrolyte

Garnet related lithium ion conductor processed by spark plasma sintering for all solid state batteries

Is Li4Ti5O12 a solid-electrolyte-interphase-free electrode material in Li-ion batteries? Reactivity between the Li4Ti5O12 electrode and electrolyte

Characteristics of ABO3 and A2BO4 (ASm, Sr; BCo, Fe, Ni) samarium oxide system as cathode materials for intermediate temperature-operating solid oxide fuel cell

Cathode reaction mechanism of porous-structured Sm0.5Sr0.5CoO3−δ and Sm0.5Sr0.5CoO3−δ/Sm0.2Ce0.8O1.9 for solid oxide fuel cells