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

The solid electrolyte interface (SEI) formed on the anode is one of the key factors that determine the life span of sodium metal batteries (SMBs). However, the continuous evolution of SEI during charging/discharging processes complicates the fundamental understanding of its chemistry and structure. In this work, we studied the underlying mechanisms of the protection effect offered by the SEI derived from sodium difluoro(oxalato)borate (NaDFOB). In situ nuclear magnetic resonance (NMR) shows that the prior reduction of DFOB anion contributes to the SEI formation, and it suppresses the decomposition of carbonate solvents. Depth-profiling x-ray photoelectron spectroscopy and high-resolution solid-state NMR reveal that the DFOB anion is gradually turned into borate and fluoride-rich SEI with cycling. The protection effect of SEI reaches the optimum at 50 cycles, which triples the life span of SMB. The detailed investigations provide valuable guidelines for the SEI engineering.

https://www.science.org/doi/pdf/10.1126/sciadv.abm4606?download=true

The chemical evolution of solid electrolyte interface in sodium metal batteries

Sodium-ion batteries (SIBs) are considered as a low-cost complementary or alternative system to prestigious lithium-ion batteries (LIBs) because of their similar working principle to LIBs, cost-effectiveness, and sustainable availability of sodium resources, especially in large-scale energy storage systems (EESs). Among various cathode candidates for SIBs, Na-based layered transition metal oxides have received extensive attention for their relatively large specific capacity, high operating potential, facile synthesis, and environmental benignity. However, there are a series of fatal issues in terms of poor air stability, unstable cathode/electrolyte interphase, and irreversible phase transition that lead to unsatisfactory battery performance from the perspective of preparation to application, outside to inside of layered oxide cathodes, which severely limit their practical application. This work is meant to review these critical problems associated with layered oxide cathodes to understand their fundamental roots and degradation mechanisms, and to provide a comprehensive summary of mainstream modification strategies including chemical substitution, surface modification, structure modulation, and so forth, concentrating on how to improve air stability, reduce interfacial side reaction, and suppress phase transition for realizing high structural reversibility, fast Na+ kinetics, and superior comprehensive electrochemical performance. The advantages and disadvantages of different strategies are discussed, and insights into future challenges and opportunities for layered oxide cathodes are also presented. 

https://onlinelibrary.wiley.com/doi/pdfdirect/10.1002/inf2.12422

Layered oxide cathodes for sodium‐ion batteries: From air stability, interface chemistry to phase transition

Structure evolution of layered transition metal oxide cathode materials for Na-ion batteries: Issues, mechanism and strategies

Sodium-ion batteries (SIBs) are experiencing a large-scale renaissance to supplement or replace expensive lithium-ion batteries (LIBs) and low energy density lead-acid batteries in electrical energy storage systems and other applications. In this case, layered oxide materials have become one of the most popular cathode candidates for SIBs because of their low cost and comparatively facile synthesis method. However, the intrinsic shortcomings of layered oxide cathodes, which severely limit their commercialization process, urgently need to be addressed. In this review, inherent challenges associated with layered oxide cathodes for SIBs, such as their irreversible multiphase transition, poor air stability, and low energy density, are systematically summarized and discussed, together with strategies to overcome these dilemmas through bulk phase modulation, surface/interface modification, functional structure manipulation, and cationic and anionic redox optimization. Emphasis is placed on investigating variations in the chemical composition and structural configuration of layered oxide cathodes and how they affect the electrochemical behavior of the cathodes to illustrate how these issues can be addressed. The summary of failure mechanisms and corresponding modification strategies of layered oxide cathodes presented herein provides a valuable reference for scientific and practical issues related to the development of SIBs.

Routes to high-performance layered oxide cathodes for sodium-ion batteries.

The air-sensitivity of transition metal oxide cathode materials (NaxTMO2, TM: transition metal) is a challenge for their practical application in sodium-ion batteries for large-scale energy storage. However, the deterioration mechanism of NaxTMO2 under ambient air is unclear, which hinders the precise design of air-stable NaxTMO2. Here, we revealed the origin of NaxTMO2 degradation by capturing the initial degradation status and microstructural evolution under ambient atmospheres with optimal humidity. It was found that the insertion of CO2 into Na layers along (003) planes of NaxTMO2 led to initial growth of Na2CO3 nanoseeds between TM layers, which initiated fast structure degradation with surface cracks and extrusion of Na2CO3 out of NaxTMO2. The degradation extents and pathways for NaxTMO2 could be highly associated with crystal orientation, particle morphology, and ambient humidity. Interestingly, the deteriorated NaxTMO2 could be completely healed through optimal recalcination, showing even improved air-stability and electrochemical performance. This work provides a helpful perspective on the interfacical structure design of high-performance NaxTMO2 cathodes for sodium-ion batteries.

Origin of Air-Stability for Transition Metal Oxide Cathodes in Sodium-Ion Batteries.

Polyanion-type sodium superionic conductor (NASICON) Na3V2(PO4)2F (NVOPF) is a promising cathode material for sodium ion batteries (SIBs). However, NVOPF shows relatively low specific capacity and ...

Revealing the Structural Reversibility of High-Performance Surface-Enhanced NVOPF Cathode Materials for Sodium Ion Batteries

Graphdiyne (GDY) is a fascinating graphene-like 2D carbon allotrope comprising sp and sp2 hybridized carbon atoms. However, GDY materials synthesized by solution-phase methods normally come as thick and porous films or amorphous powders with severely disordered stacking modes that obstruct macroscopic applications. Here, a facile and scalable synthesis of ultrathin holey graphdiyne (HGDY) nanosheets is reported via palladium/copper co-catalyzed homocoupling of 1,3,5-triethynylbenzene. The resulting freestanding 2D HGDY self-assembles into 3D foam-like networks which can in situ anchor clusters of palladium atoms on their surfaces. The Pd/HGDY hybrids exhibit high electrocatalytic activity and stability for the oxygen reduction reaction which outperforms that of Pt/C benchmark. Based on the ultrathin graphene-like sheets and their unique 3D interconnected macrostructures, Pd/HGDY holds great promise for practical electrochemical catalysis and energy-related applications.

Synthesis and Self-Assembly of Ultrathin Holey Graphdiyne Nanosheets for Oxygen Reduction Reaction.

Crystalline materials are often considered to have rigid periodic lattices, while soft materials are associated with flexibility and nonperiodicity. The continuous evolution of metal-organic frameworks (MOFs) has erased the boundaries between these two distinct conceptions. Flexibility, disorder, and defects have been found to be abundant in MOF materials with imperfect crystallinity, and their intricate interplay is poorly understood because of the limited strategies for characterizing disordered structures. Here, we apply advanced nuclear magnetic resonance spectroscopy to elucidate the mesoscale structures in a defective MOF with a semicrystalline lattice. We show that engineered defects can tune the degree of lattice flexibility by combining both ordered and disordered compartments. The one-dimensional alignment of correlated defects is the key for the reversible topological transition. The unique matrix is featured with both rigid framework of nanoporosity and flexible linkage of high swellability.

https://www.science.org/doi/pdf/10.1126/sciadv.ade6975?download=true

One-dimensional alignment of defects in a flexible metal-organic framework

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