DOI: 10.1002/aenm.202000974 and the relatively high cell cost raises concerns on the sustainable development of LIBs, especially in the large-scale energy storage area, which put specific requirements on the price cost, safety, and durability of the battery.[1] In addition to the concern over potential shortage of lithium, the incidents associated with fires and explosions of state-of-the-art LIBs are stimulating advanced strategies and new safe alternatives in recent years. Sodium-ion batteries (SIBs), with identical internal components and working principles with LIBs, have been proposed as one of the most promising nextgeneration energy storage technology because of the evident advantages of lowcost and worldwide abundance of charge carriers.[2] Besides, the cost of SIBs could be further reduced by use of Co/Ni-free cathode materials[3] and aluminum current collector on the anode side since sodium does not alloy with aluminum.[4] In addition to the economic benefits, the configuration of SIBs offers a potentially safe way for batteries storage and transportation. Since Al current collector does not dissolve into electrolyte at a voltage of 0 V, shipping and storing SIBs which contain no energy (a fully discharged state) is potentially feasible.[5] Moreover, Dahn’s group investigated the thermal stability of positive materials for SIBs and found that the desodiated Na0.5CrO2 cathode was less reactive than Li0FePO4 in nonaqueous electrolyte at elevated temperatures.[6] Robinson et al. found that the self-heating rate in a Na-ion pouch cell is significantly slower than that in a commercial LiCoO2 (LCO) pouch cell and the thermal runaway process is less exothermic for Na-ion cells, indicating that SIBs could be a potentially safer option compared with LIBs.[7] However, the larger and heavier Na ions have poor kinetic characteristic in the host structure during insertion reaction process, so it may lead to rapid degradation of the host materials with exothermic reaction.[8–10] In addition, the higher solubility of solid electrolyte interphase (SEI) of SIBs resulting from lower Lewis acidity of sodium complex, indicates that the incomplete coverage of electrode may further lead to undesired side reactions, accelerating heat generation. The cathode materials reported so far, roughly including oxides, polyanions, organics, Prussian blue and its analogues, which have poor electronic/ionic conductivity, will bring issues to thermal diffusion as well.[11] So far, nonaqueous liquid electrolyte is still the primary option for SIBs because of wide electrochemical stable window, high ionic conductivity, and rapid mass transfer at the electrolyteelectrode interface, yet giving rise to safety hazards.[12] Recent Sodium-ion batteries, with their evident superiority in resource abundance and cost, are emerging as promising next-generation energy storage systems for large-scale applications, such as smart grids and low-speed electric vehicles. Accidents related to fires and explosions for batteries are a reminder that safety is prerequisite for energy storage systems, especially when aiming for grid-scale use. In a typical electrochemical secondary battery, the electrical power is stored and released via processes that generate thermal energy, leading to temperature increments in the battery system, which is the main cause for battery thermal abuse. The investigation of the energy generated during the chemical/electrochemical reactions is of paramount importance for battery safety, unfortunately, it has not received the attention it deserves. In this review, the fundamentals of the heat generation, accumulation, and transportation in a battery system are summarized and recent key research on materials design to improve sodium-ion battery safety is highlighted. Several effective materials design concepts are also discussed. This review is designed to arouse the attention of researcher and scholars and inspire further improvements in battery safety.

Materials Design for High-Safety Sodium-Ion Battery

at an average storage voltage of 3.2 V with long cycle life. When coupled with hard carbon anode, a prototype rechargeable sodium-ion battery offers an energy density of 210 Wh kg −1 , a round-trip energy effi ciency of 90%, high rate capability, and excellent cycling stability. These desired performances make this system to be closer to the level of practical applications. The Na 0.9 [Cu 0.22 Fe 0.30 Mn 0.48 ]O 2 (Na 0.9 [Cu II 0.22 Fe III 0.30 Mn III 0.16 Mn IV 0.32 ]O 2 ) material was synthesized by a simple solid-state reaction at 850 °C in air atmosphere using precursors of Na 2 CO 3 , CuO, Fe 2 O 3 , and Mn 2 O 3 . The crystal structure of the as-synthesized material was determined by X-ray diffraction (XRD) as shown in Figure 1 a together with its refi nement results by the Rietveld method (see Table S1, Supporting Information). It can be seen that all the Bragg diffraction peaks are in excellent agreement with the JC DS No. 01-0821495 (O3-type α-NaFeO 2 ) and can be indexed to a hexagonal layered structure with a space group of 3 R m − , indicative of a typical O3-type layered structure (note that the letter “O” refers to the Na coordination environment of octahedral site whereas the number “3” refers to the number of MO 2 slab according to Delmas’ notation. [ 13 ] A schematic illustration of the O3-type structure is also shown in Figure 1 b. The structure refi nement gives the lattice parameters a = 2.9587(7) A, c = 16.3742(6) A. The lattice parameter of c -axis is slightly larger than that of other O3-type materials [ 5f–h , 6b , 8a ] because the Na content is less than 1. The inductively coupled plasma (ICP) result confi rms the composition of Na 0.89 [Cu 0.22 Fe 0.30 Mn 0.48 ]O 2 (see Table S2, Supporting Information). The morphology of the resulting sample is shown in Figure 1 c. The distribution of the particle size is in the range of 10–30 μm with about 3 μm sized primary particle agglomerations together (Figure 1 d). Most importantly, unlike other O3-type materials, [ 4–9,12 ] this material is very stable against water. In order to confi rm this, we intentionally design an accelerated aging experiment as described in the Experimental Section which was verifi ed by LiMO 2 as shown in Figure S1 (Supporting Information). We placed the as-synthesized material in deionized water for 3 d and then dried the material at 100 °C for overnight. The obtained material was checked by XRD again. It can be seen that the XRD pattern is nearly identical to that of the as-synthesized material, which is very different from other O3-type materials as shown in Figure S2 (Supporting Information). These results suggest that the O3-Na 0.9 [Cu 0.22 Fe 0.30 Mn 0.48 ]O 2 is very stable against water. Furthermore, after the material was stored in air for one month Large-scale electrical energy storage systems are one of the core technologies in renewable energies and smart grid, among which sodium-ion batteries show great promise due to the abundant sodium resources. Layered metal oxides (of general formula: A x MO 2 , where A = Li, Na; M = Co, Ni, Mn, Cr, Fe, etc.) with alternating alkali metal layer and transition metal layer have long been of particular interest since the early 1980s as an important class of cathode materials for rechargeable batteries due to their easy synthesis and high energy density. [ 1 ] One of the most successful examples is LiCoO 2 , [ 1a ] which is commonly used as a cathode in lithium-ion batteries with the highest volumetric energy density for portable electronic devices. Its metal substituted materials (LiCo 1− x − y − z Ni x Mn y Al z O 2 ) are being used in power batteries for electric vehicles. In the case of sodiumion batteries operated at room temperature which are proposed for large-scale electrical energy storage owing to the naturally abundant sodium resources in recent years. [ 2,3 ] Na x CoO 2 that can electrochemically and reversibly intercalate Na is the fi rst example, [ 1b ] then a large number of layered metal oxides have been extensively exploited. [ 4–12 ] However, the practical applications have been hindered by two major challenges. First, unlike LiMO 2 , almost all the Na x MO 2 are not stable against moisture (either they can be oxidized by water or water/carbon dioxide molecules can be intercalated into alkali metal layer). [ 4–9,11,12 ]

/pdf/prototype-sodium-ion-batteries-using-air-stable-and-co-ni-5fwg7s03of.pdf

Prototype Sodium-Ion Batteries Using Air-Stable and Co/Ni-Free O3-Layered Metal Oxide Cathode

Heterostructuring electrodes with multiple electroactive and inactive supporting components to simultaneously satisfy electrochemical and structural requirements has recently been identified as a viable pathway to achieve high‐capacity and durable sodium‐ion batteries (SIBs). Here, a new design of heterostructured SIB anode is reported consisting of double metal‐sulfide (SnCo)S2 nanocubes interlaced with 2D sulfur‐doped graphene (SG) nanosheets. The heterostructured (SnCo)S2/SG nanocubes exhibit an excellent rate capability (469 mAh g−1 at 10.0 A g−1) and durability (5000 cycles, 487 mAh g−1 at 5.0 A g−1, 92.6% capacity retention). In situ X‐ray diffraction reveals that the (SnCo)S2/SG anode undergoes a six‐stage Na+ storage mechanism of combined intercalation, conversion, and alloying reactions. The first‐principle density functional theory calculations suggest high concentration of p–n heterojunctions at SnS2/CoS2 interfaces responsible for the high rate performance, while in situ transmission electron microscopy unveils that the interlacing and elastic SG nanosheets play a key role in extending the cycle life.

Heterostructured Nanocube-Shaped Binary Sulfide (SnCo)S2 Interlaced with S-Doped Graphene as a High-Performance Anode for Advanced Na+ Batteries

Metal-based anodes have recently aroused much attention in sodium ion batteries (SIBs) owing to their high theoretical capacities and low sodiation potentials. However, their progresses are prevented by the inferior cycling performance caused by severe volumetric change and pulverization during the (de)sodiation process. To address this issue, herein an alloying strategy was proposed and nanoporous bismuth (Bi)–antimony (Sb) alloys were fabricated by dealloying of ternary Mg-based precursors. As an anode for SIBs, the nanoporous Bi2Sb6 alloy exhibits an ultralong cycling performance (10 000 cycles) at 1 A/g corresponding to a capacity decay of merely 0.0072% per cycle, due to the porous structure, alloying effect and proper Bi/Sb atomic ratio. More importantly, a (de)sodiation mechanism ((Bi,Sb) ↔ Na(Bi,Sb) ↔ Na3(Bi,Sb)) is identified for the discharge/charge processes of Bi–Sb alloys by using operando X-ray diffraction and density functional theory calculations.

A Dealloying Synthetic Strategy for Nanoporous Bismuth-Antimony Anodes for Sodium Ion Batteries.

Coating methodology is commonly employed in the enhancement of Ni-rich cathodes for Li-ion batteries as an efficient approach, while its strategy and effect are still great challenges to achieve success in surface modifications for comprehensive electrochemical properties. In this work, the surface of Ni-rich cathode LiNi0.82Co0.15Al0.03O2 (NCA) is modified by intimately coating NASICON-type solid electrolyte LiZr2(PO4)3 (LZP) via a facile approach involving electrostatic attraction. With well-designed architecture and a uniform NASICON-type LZP nanolayer wrapping over the NCA microsphere, the entire electrode demonstrates exceptional Li+ diffusion and conductivity and suppresses the side reaction between electrolyte and electroactive NCA, stabilizing the phase interface with less Li+/Ni2+ cation mixing. As a result, the NCA@LZP can deliver a high reversible capacity of 182 mAh g-1 at 1C in 2.7-4.3 V, maintaining the capacity retention of 84.6% after 100 cycles. More importantly, the structure stability of NCA is enhanced substantially by surface modification of LZP at high cutoff voltage. It achieves a reversible capacity of 204 mAh g-1 and keeps 100.4 mAh g-1 after 500 cycles at 1C in the potential range of 2.7-4.5 V. This effective strategy of using NASICON fast ionic conductor like LZP as a coating layer may provide a new insight to modify the surface of Ni-rich electrode, improving the rate capability and cyclic performance under high voltage.

Enhancing High-Voltage Performance of Ni-Rich Cathode by Surface Modification of Self-Assembled NASICON Fast Ionic Conductor LiZr2(PO4)3

Mn doped NaV3(PO4)3/C anode with high-rate and long cycle-life for sodium ion batteries

Exploration of VPO4 as a new anode material for sodium-ion batteries.

Unravelling the electrochemical properties and thermal behavior of NaNi2/3Sb1/3O2 cathode for sodium-ion batteries by in situ X-ray diffraction investigation

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Mn doped NaV3(PO4)3/C anode with high-rate and long cycle-life for sodium ion batteries

Exploration of VPO4 as a new anode material for sodium-ion batteries.

Unravelling the electrochemical properties and thermal behavior of NaNi2/3Sb1/3O2 cathode for sodium-ion batteries by in situ X-ray diffraction investigation