The development of large‐scale energy storage systems (ESSs) aimed at application in renewable electricity sources and in smart grids is expected to address energy shortage and environmental issues. Sodium‐ion batteries (SIBs) exhibit remarkable potential for large‐scale ESSs because of the high richness and accessibility of sodium reserves. Using low‐cost and abundant elements in cathodes with long cycling stability is preferable for lowering expenses on cathodes. Many investigated cathodes for SIBs are dogged by structural and morphology changes, unstable interphases between the cathode and the electrolyte, and air sensitivity, causing unsatisfactory cycling performance. Therefore, understanding the mechanism of capacity degeneration in depth and developing precise solutions are critical for designing low‐cost cathodes that are highly stable under cycling. Herein, recent progress in long‐cycle‐life and low‐cost cathodes for SIBs is focused on, and a comprehensive discussion of the key points in SIBs toward large‐scale applications is provided. The roots of the unstable cycling performance of low‐cost cathodes are discussed. Also, effective strategies are summarized from the recent progress on long‐cycle‐life and low‐cost cathodes. This review is expected to encourage deeper investigation of long‐lifespan cathodes for SIBs, particularly for potential large‐scale industrialization.

Long‐Cycle‐Life Cathode Materials for  Sodium‐Ion Batteries toward Large‐Scale Energy Storage Systems

Prussian blue analogues (PBAs) have been regarded as promising cathode materials for sodium-ion batteries (SIBs) owing to their high theoretical energy density and low-cost. However, high water and vacancies content of PBAs lower their energy density and bring safety issues, impeding their large-scale application in SIBs. Herein, a facile "potassium-ions assisted" strategy is proposed to synthesize highly crystallized PBAs. By manipulating the dominant crystal plane and suppressing vacancies, the as-prepared PBAs exhibits increased redox potential resulting in high energy density up to ~450 Wh kg-1, which is at the same level of the well-known LiFePO4 cathodes for lithium-ion batteries. Remarkably, unconventional highly-reversible phase evolution and redox-active pairs were identified by multiple in-situ techniques for the first time. The preferred guest-ion storage sites and migration mechanism were systematically analysed through theoretical calculations. We believe these results could inspire the designing of safe SIBs with high energy density.

Prussian Blue Analogues with Optimized Crystal Plane Orientation and Low Crystal Defects toward 450 Wh kg-1 Sodium-Ion Batteries.

At present, the energy density of the mainstream lithium iron phosphate battery and ternary lithium battery is between 200 and 300 Wh kg−1 or even <200 Wh kg−1, which can hardly meet the continuous requirements of electronic products and large mobile electrical equipment for small size, light weight and large capacity of the battery. In order to achieve high energy density batteries, researchers have tried to develop electrode materials with higher energy density or modify existing electrode materials, improve the design of lithium batteries and develop new electrochemical energy systems, such as lithium air, lithium sulfur batteries, etc. Here, we analyze the influence of the existing chemical system and structure of lithium-ion battery on the energy density of lithium-ion battery, and summarizes the methods of improving the energy density of lithium-ion battery in the aspects of material preparation and battery structure design. Strategies such as improving the active material of the cathode, improving the specific capacity of the cathode/anode material, developing lithium metal anode/anode-free lithium batteries, using solid-state electrolytes and developing new energy storage systems have been used in the research of improving the energy density of lithium batteries. However, due to a number of difficulties, these high energy density batteries are still in the experimental stage, and further study is needed to improve their practical applicability. 

Strategies toward the development of high-energy-density lithium batteries

The solid electrolyte interface (SEI) formed via electrolyte decomposition on the anode of lithium ion batteries is largely responsible for the stable cycling of conventional lithium ion batteries. Similarly, there is a lesser-known analogous layer on the cathode side of a lithium ion battery, termed the cathode electrolyte interface (CEI), whose composition and role are debated. To confirm the existence and composition of the CEI, desorption electrospray ionization mass spectrometry (DESI-MS) is applied to study common lithium ion battery cathodes. We observe CEI formation on the LiMn2O4 cathode material after cycling between 3.5 and 4.5 V vs Li/Li(+) in electrolyte solution containing 1 M LiPF6 or LiClO4 in 1:1 (v/v) ethylene carbonate (EC) and dimethyl carbonate (DMC). Intact poly(ethylene glycol) dimethyl ether is identified as the electrolyte degradation product on the cathode surface by the high mass-resolution Orbitrap mass spectrometer. When EC is paired with ethyl methyl carbonate (EMC), poly(ethylene glycol) dimethyl ether, poly(ethylene glycol) ethyl methyl ether, and poly(ethylene glycol) are found on the surface simultaneously. The presence of ethoxy and methoxy end groups indicates both methoxide and ethoxide are produced and involved in the process of oligomerization. Au surfaces cycled under different electrochemical windows as model systems for Li-ion battery anodes are also examined. Interestingly, the identical oligomeric species to those found in the CEI are found on Au surfaces after running five cycles between 2.0 and 0.1 V vs Li/Li(+) in half-cells. These results show that DESI-MS provides intact molecular information on battery electrodes, enabling deeper understanding of the SEI or CEI composition.

Characterization of the Cathode Electrolyte Interface in Lithium Ion Batteries By Desorption Electrospray Ionization Mass Spectrometry (DESI-MS)

Insights on rational design and regulation strategies of Prussian blue analogues and their derivatives towards high-performance electrocatalysts

Non-aqueous synthesis of high-quality Prussian blue analogues for Na-ion batteries.

Dual-site lattice co-doping strategy regulated crystal-structure and microstructure for enhanced cycling stability of Co-free Ni-rich layered cathode

Spent lithium-ion batteries can be recycled to effectively re-utilize them. This can be conducive to secondary resource utilization as well as environmental protection. Here, it is suggested to roast the spent cathode materials with sodium sulfite to extract lithium more effectively. Under the ideal circumstances of a roasting temperature of 750 °C, the molar ratio of Na2SO3 to spent cathode material of 3.0, and a roasting period of 2 h, the leaching efficiency of Li reaches 94.06%. During the sodium sulfite roasting process, the spent LiNi0.6Co0.2Mn0.2O2 materials were transformed into LiNa(SO4), LiMnO2, NiO, LiMn2O4, Co9S8, and Ni, Co, and Mn. The LiNi0.6Co0.2Mn0.2O2 materials that were produced using the recovered Li2CO3 exhibit good electrochemical performance. The closed-loop process based on Sodium sulfite roasting is expected to be applied in the recycling industry of spent lithium-ion batteries. 

Sodium sulfite roasting for preferential lithium extraction from cathode material of spent lithium-ion batteries

High separation efficiency of ternary cathode materials from spent lithium-ion batteries by ternary molten Li-salt method

It is well accepted that a lithiophilic interface can effectively regulate Li deposition behaviors, but the influence of the lithiophilic interface is gradually diminished upon continuous Li deposition that completely isolates Li from the lithiophilic metals. Herein, we perform in-depth studies on the creation of dynamic alloy interfaces upon Li deposition, arising from the exceptionally high diffusion coefficient of Hg in the amalgam solid solution. As a comparison, other metals such as Au, Ag, and Zn have typical diffusion coefficients of 10–20 orders of magnitude lower than that of Hg in the similar solid solution phases. This difference induces compact Li deposition pattern with an amalgam substrate even with a high areal capacity of 55 mAh cm−2. This finding provides new insight into the rational design of Li anode substrate for the stable cycling of Li metal batteries. 

https://onlinelibrary.wiley.com/doi/pdfdirect/10.1002/eem2.12618

Construction of Dynamic Alloy Interfaces for Uniform Li Deposition in
 Li‐Metal
 Batteries

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Papers

Non-aqueous synthesis of high-quality Prussian blue analogues for Na-ion batteries.

Dual-site lattice co-doping strategy regulated crystal-structure and microstructure for enhanced cycling stability of Co-free Ni-rich layered cathode

Sodium sulfite roasting for preferential lithium extraction from cathode material of spent lithium-ion batteries

High separation efficiency of ternary cathode materials from spent lithium-ion batteries by ternary molten Li-salt method

Construction of Dynamic Alloy Interfaces for Uniform Li Deposition in Li‐Metal Batteries