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Abbreviation (ISO4): Prog Chem      Editor in chief: Jincai ZHAO

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Progress in Chemistry >

2023 , Vol. 35 >Issue 8: 1177 - 1190

DOI: https://doi.org/10.7536/PC221220

Review

All Solid-State Sodium Batteries and Its Interface Modification

  • Dongrong Yang 1, 2, 3 ,
  • Da Zhang , 1, 2, 3, * ,
  • Kun Ren 1, 2, 3 ,
  • Fupeng Li 1, 2, 3 ,
  • Peng Dong 1, 2, 3 ,
  • Jiaqing Zhang 1, 2, 3 ,
  • Bin Yang 1, 2, 3 ,
  • Feng Liang , 1, 2, 3, *
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  • 1 Key Laboratory for Nonferrous Vacuum Metallurgy of Yunnan Province, Kunming University of Science and Technology,Kunming 650093, China
  • 2 National Engineering Research Center of Vacuum Metallurgy, Kunming University of Science and Technology, Kunming 650093, China
  • 3 Faculty of Metallurgical and Energy Engineering, Kunming University of Science and Technology, Kunming 650093, China
*Corresponding author e-mail: (Feng Liang);
(Da Zhang)

Received date: 2022-12-28

  Revised date: 2023-05-24

  Online published: 2023-07-18

Supported by

National Natural Science Foundation of China(12175089)

National Natural Science Foundation of China(12205127)

Key Research and Development Program of Yunnan Province(202103AF140006)

Applied Basic Research Programs of Yunnan Provincial Science and Technology Department(202001AW070004)

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Abstract

All solid-state sodium batteries have great potential for portable electronics, electric vehicles, and large-scale energy storage applications due to the low cost of sodium, high security, and high energy density. However, the development and large-scale application of all-solid-state sodium ion batteries urgently need to solve the problems such as low ion conductivity of solid electrolyte, high charge-transfer impedance on interface, insufficient interfacial contact, and compatibility issues between electrodes and electrolytes solid electrolyte. Herein, combining the latest reports with our research findings, the research progress and development trend of β-Al2O3 electrolytes, NASICON electrolytes, sulfide electrolytes, polymer electrolytes, and composite electrolytes were summarized. The latest achievements in interface characteristics, the modification strategies of the interface between the electrodes and solid electrolytes and modification methods for surfaces of solid electrolytes were reviewed. Finally, the development direction of interface modification strategy for solid-state sodium ion batteries was prospected. This review have contributed to understand the interface science issues of all solid-state sodium ion batteries and provides a theoretical guidance for the development and application of solid-state sodium ion batteries.

Contents

1 Introduction

2 Solid-state electrolytes

3 Challenges for all solid-state sodium batteries

4 Interfaces engineering

4.1 Cathode/electrolyte interfaces

4.2 Anode/electrolytes interfaces

4.3 Structure design for interfaces engineering

5 Conclusion and future perspectives

Key words： all solid-state sodium batteries; solid-state electrolytes; interface; modification

Cite this article

Dongrong Yang , Da Zhang , Kun Ren , Fupeng Li , Peng Dong , Jiaqing Zhang , Bin Yang , Feng Liang . All Solid-State Sodium Batteries and Its Interface Modification[J]. Progress in Chemistry, 2023 , 35(8) : 1177 -1190 . DOI: 10.7536/PC221220

1 Introduction

Lithium-ion batteries (LIBs) have long dominated the markets of portable electronic devices and electric vehicles since their commercialization in 1991. However, the shortage of lithium resources and high cost have inhibited the application of LIBs in the field of large-scale energy storage[1⇓~3]. Na-ion batteries have the advantages of abundant resources, low cost and energy storage mechanism similar to lithium-ion batteries, which make them very potential for industrial applications such as portable electronic devices, hybrid and all-electric vehicles[4,5]. However, traditional liquid sodium-ion batteries (SIBs) have safety problems such as electrolyte leakage and flammability, and the uncontrollable growth of sodium dendrites leads to poor battery stability, and the formation of "dead sodium" will also lead to reversible capacity loss of SIBs[6]. Solid-state sodium-ion batteries (SSBs) use solid electrolytes (SEs) to replace traditional organic electrolytes to solve the safety problems of combustion and explosion caused by electrolyte volatilization and leakage. At the same time, the superior mechanical properties and thermal/chemical stability of SEs improve the battery life and stability, and realize the matching use of high-energy positive electrode and metal sodium negative electrode in SSBs. In addition, SEs can simplify the design of batteries without additional electrolyte containers or separator assemblies, thus improving the energy density of batteries. SSBs take into account both high energy density and high safety, which is of great significance for developing the next generation of high energy density batteries and solving the energy crisis[7⇓⇓⇓~11].
However, as the core materials of SSBs, SEs still face the problems of low ionic conductivity at room temperature, narrow electrochemical window, poor compatibility with the electrode interface and poor contact[12⇓⇓~15]. Therefore, enhancing the Na+ conductivity, interface compatibility, interface stability, and reducing the interface impedance of SEs are the key to the performance improvement and commercial application of SSBs. The interface impedance between cathode and SEs is mainly due to the loose contact, the electrode volume effect and the space charge layer during the charge-discharge process. The interface stability is mainly manifested by the chemical reaction and the mutual diffusion of interface elements. The interface problems between anode and SEs are mainly dendrite growth, poor interface contact and poor interface compatibility. In order to solve the above problems, surface coating modification, electrode composition regulation, introduction of interface interlayer, and design of new cell structure are generally used to reduce the interface impedance and improve the interface stability of SSBs[12,17⇓⇓⇓⇓⇓⇓~24].
To sum up, the construction of electrode/SEs interface with good wettability, strong compatibility, high ionic conductivity and electronic insulation is very important to obtain SSBs with excellent rate performance, charge-discharge efficiency and cycle stability[16]. In this paper, the research progress of SSBs in recent years is reviewed, and the research progress of sodium-based inorganic solid electrolytes, polymer solid electrolytes and composite solid electrolytes is summarized. The effects of thermodynamic stability, mechanical stability, space charge layer, matching between electrode and electrolyte, and sodium dendrite on the performance of SSBs were discussed. The latest research results of SSBs interface were reviewed from the aspects of surface modification of SEs, interface interlayer, and design of new cell structure.

2 Research Status and Trend of Solid Electrolyte

The working principle of SSBs is similar to that of traditional sodium-ion batteries. When charging, the Na+ comes out of the positive electrode and reaches the negative electrode through SEs. The negative electrode is in a sodium-rich state, while the positive electrode is in a sodium-poor state. The electrons reach the negative electrode from the positive electrode through an external circuit, thus ensuring the charge balance of the negative electrode. When discharging, the Na+ comes out from the negative electrode and is embedded into the positive electrode through the SEs, the positive electrode is in a sodium-rich state, the negative electrode is in a sodium-poor state, and the electrons reach the positive electrode from the negative electrode through an external circuit for charge compensation[25]. The solid electrolyte acts as both a separator and a Na+ conducting medium in SSBs. Therefore, as the core material of SSBs, the Na+ conductivity, chemical/electrochemical stability, electrode compatibility and thermal stability of SEs are the key factors affecting the energy density, cycle life and safety of SSBs[7,26].
Fig. 1 is a comparison of that property of a common inorganic solid electrolyte and an organic polymer solid electrolyte. The results show that inorganic solid electrolyte has higher conductivity and better mechanical properties than organic solid electrolyte at room temperature, and its safety and stability are better than those of organic solid electrolyte[28⇓⇓⇓⇓⇓⇓⇓⇓⇓⇓~39]. Combined with Fig. 1, Table 1 summarizes the current status of SEs such as oxides, sulfides, polymers, and gels: the Na+ conductivity and thermal stability of oxide solid electrolytes are high, but the interfacial wettability is poor; Sulfide solid electrolyte has good toughness and high Na+ conductivity, but it is unstable in air and has poor compatibility with sodium metal. Polymer solid electrolyte has good flexibility and interfacial wettability, but poor thermal stability and low Na+ conductivity at room temperature. Borohydride solid electrolyte has high thermal stability, chemical stability and Na+ conductivity at room temperature, but its interface impedance is high. Gel polymer solid electrolyte has good flexibility, interface stability and Na+ conductivity, but poor thermal stability and high cost.
图1 无机固体电解质(a,b,c,d,e)和有机聚合物固体电解质(f)性质对比图[27]

Fig.1 Performance comparison of (a, b, c, d, e) inorganic solid electrolytes, and (f) solid polymer electrolytes[27]

表1 常见无机固体电解质的特性和优缺点[40,41]

Table 1 The characteristics, advantages, and disadvantages of common inorganic solid electrolytes[40,41]

Type Selected materials Conductivity
(S·cm-1)		 Potential window
(V (vs Na+ / Na))		 Advantages Disadvantages
Oxides Na-β″-Al2O3, NASICON,
Na2M2TeO6,		 10-4 ~ 10-3 Up to 7 High thermal stability
High ionic conductivity		 High interface resistance
Poor interface wetting
Sulfides Na3PS4, Na11Sn2PS12, etc. 10-4 ~ 10-3 < 4 for Na3PS4
Others up to 5		 High ionic conductivity
High flexibility		 Low chemical stability,
Poor compatibility with Na
Polymer based PEO, PEG, PVDF-HFP, etc. 10-6 ~ 10-4 About 4.5 High flexibility
Good interface wetting		 Low ionic conductivity,
Low thermal stability
High cost
Boron
hydrides		 Na2-x(B12H12)x(B10H10)1-x
Na2-x(CB11H12)x(B12H12)1-x, etc.		 10-4 ~ 10-2 Up to 5 High thermal stability High chemical stability
High ionic conductivity		 Large interfacial resistance
Gel Polymer EPTA-NaPF6-PC/FEC/PS-NaPF6,
BP/PEO-HKUST-1-NaClO4-EC/
DEC/FEC, etc.		 10-4 ~ 10-3 Up to 5 High ionic conductivity
High flexibility
Good interfacial stability		 Low thermal stability
High cost

2.1 Inorganic solid electrolyte

β-Al2O3-type solid electrolyte refers to M2O·nAl2O3 (M = Na, K, Rb, Ag, Ti, etc.) compounds, including β-Al2O3 (hexagonal phase structure,P63/mmc,a0=b0=5.58Å,c0=22.45Å, general formula :Na2O·(8~11)Al2O3) and β″-Al2O3 (rhombohedral crystal phase structure,R 3 - m,a0=b0=5.61Å,c0=33.85Å, general formula :Na2O·(5~7)Al2O3) two crystal structures[42,43]. As shown in Figure 2A, both β-Al2O3 and β″-Al2O3 are stacked by spinel structures composed of [AlO4] tetrahedra and [AlO6] octahedra, and the adjacent spinel structures are connected by oxygen atoms and form conductive planes with the surrounding Na+. Because of that high concentration of mobile Na+ in the ion-conducting plane of the β″-Al2O3 and the weak electrostatic force between the ions of bridge oxygen in the β″-Al2O3structure and the surrounding Na+,So that it has a higher ionic conductivity at room temperature, so the conductivity of β″-Al2O3Na+ is higher than that of β-Al2O3.For example, the ionic conductivity of β″-Al2O3 at room temperature and 300 ℃ is 2.0×10-3 and 0.2~0.4 S·cm-1, respectively, but the β″-Al2O3 based SSBs need to operate at high temperature.Moreover, the β″-Al2O3 is unstable to air and has low mechanical strength, and the β″-Al2O3 will decompose into Al2O3 and β-Al2O3 under high temperature process, resulting in impure products[26,44,45][26,46,47]. The results show that the addition of trace additives such as MgO, TiO2, Y2O3 or ZrO2 in the synthesis process of Na-β″-Al2O3 can effectively inhibit the high temperature decomposition of Na-β″-Al2O and obtain SEs with higher conductivity.In addition, the addition of excessive sodium source during the preparation of Beta-Al2O3 can promote the generation of Na-β″-Al2O, and the appropriate mass ratio of Na-β″-Al2O to Na-β-Al2O3 is beneficial to the improvement of ionic conductivity and mechanical properties[26].
图2 (a)β-Al2O3和β″-Al2O3晶体结构[26];(b)Na3Zr2Si2PO12钠离子传输路径示意图[27];(c)Na3PS4晶体结构[26];(d)聚合物固体电解质Na+传导机理图[54]

Fig.2 (a) Crystal structures of β-Al2O3 and β″-Al2O3[26]; (b) schematic illustration of Na+ conducting pathways in Na3Zr2Si2PO12[27]; (c) crystal structures of the Na3PS4[26]; (d) schematic illustration of Na+ transport mechanism in polymer solid electrolytes[54]

Compared with β-Al2O3 solid electrolyte, Na1+xZr2SixP3-xO12(0≤x≤3) solid electrolyte is stable to air and easy to obtain products with high purity. It mainly exists in hexagonal (R-3c) and monoclinic (C2/C, 1.8 ≤ X ≤ 2.2) crystal structures[48⇓⇓~51]. As shown in Figure 2B, the Na1 site in the hexagonal structure is located between two ZrO6 octahedra, which are connected by PO4 tetrahedra to form a Na-ZrO6-ZrO6-Na-ZrO6-ZrO6 structural band along the C axis, while the Na2 site is located between two structural bands and forms a three-dimensional Na+ diffusion channel with the Na1 site[27,52]. The partial substitution of P by Si in the monoclinic crystal structure leads to the reduction of the crystal structure symmetry, so that the Na2 site is split (Na2 and Na3 sites are generated) to form Na1-Na2 and Na1-Na3 Na+ transport channels, and in addition, the additional Na+ occupied sites can be used as exchange sites for ion transport, thereby improving the ionic conductivity[27,53]. The Na+ conductivity of Na3Zr2Si2PO12 (monoclinic structure) is the highest among the currently reported Na1+xZr2SixP3-xO12 electrolytes, as shown in Figure 3A,The Na+ conductivity of this electrolyte is as high as 10-4 and 10-1S·cm-1 at room temperature and 300 ° C, respectively[12,25,26]. It is generally believed that the size of the triangular "bottleneck" formed by three O atoms in the SiO4/PO4 tetrahedron and the ZrO6 octahedron is the key to determine the conductivity of SEs. Research reports have confirmed the above view by introducing ions with different radii at the Zr4+(0.72Å) site.For example, Sc3+(0.74Å), Y3+(0.89Å), Ca2+(1.0Å), La3+(1.06Å) and Sr2+(1.18Å) can expand their "bottleneck" size.And thus that conductivity of the Na+ is improve[40,55⇓~57]. In addition, Hu et al. Successfully constructed new phases of Na3La(PO4)2, La2O3 and LaPO4 at the grain boundary of Na3Zr2Si2PO12 by doping elements such as La, which improved the migration rate of Na+[58]. Imilarly, Mg dope that Na3Zr2Si2PO12 to form a grain boundary phase of the Na3-2δMgδPO4,Filling Na2SiO3 at the grain boundary of the Na3Zr2Si2PO12 by high temperature melt sintering and densifying the sintered Na3Zr2Si2PO12 by adding Na2B4O7 also proved to improve the grain boundary of the electrolyte and increase the conductivity of SEs[28,29,59].
图3 无机固体电解质Na+电导率随温度变化[87]:(a)NASICON;(b)硫化物固体电解质;(c)聚合物和复合固体电解质;(d)结晶态有机物、反钙钛矿和硼氢化物固体电解质

Fig.3 Temperature-dependent Na+ conductivities of inorganic solid electrolytes[87]: (a) NASICON; (b) sulfide solid electrolytes; (c) polymer and composite solid electrolytes; (d) crystalline organic, anti-perovskites and borohydrides solid electrolytes

Sulfide solid electrolytes include crystalline, glassy and glass-ceramic electrolytes. The radius of sulfur atom is larger than that of oxygen atom and the interaction between sulfur atom and sodium ion is weak, so the Na+ conductivity of sulfide solid electrolyte is higher than that of oxide solid electrolyte[60]. Because of their excellent ionic conductivity and good interfacial contact characteristics, more and more scientists have devoted themselves to the study of sodium-based sulfides in recent years, among which solid electrolysis of sulfides such as Na3PS4, Na3SbS4, Na11Sn2PS12 and Na4Sn0.67Si0.33S4 is the most common. As shown in fig. 2C,Tetragonal phase (P 4 2 ¯ 1c) and cubic phase (I 4 3 ¯ of Na3PS4 electrolyteM) materials have the advantages of low grain boundary impedance and high electrical conductivity of Na+ (~10-4S·cm-1),As shown in fig. 3B, and has been widely studied for easily forming a close contact with the electrode to improve the sodium ion transport at the interface[12,61⇓⇓⇓~65]. However, the poor stability of sulfide solid electrolyte in air limits its commercial application. Studies have shown that through cations (Sn4+, Si4+, Ge4+, Sb5+,As5+, etc.) replacing the P site of Na3PS4 or doping the S site with anions (Cl- and Se2-) can effectively enhance the stability of sulfide electrolyte to air and improve its sodium ion conductivity[66⇓⇓⇓~70].

2.2 Solid polymer electrolyte

Solid polymer electrolytes (SPEs) are composed of polymers and electrolyte salts, which have the advantages of good toughness, light weight and strong adaptability to the volume change of electrodes. At present, the common polymer solid electrolytes are mainly polyethylene oxide (PEO), polymethyl methacrylate (PMMA), polyvinylidene fluoride (PVDF), polyvinylidene fluoride-co-hexafluoropropylene (PVDF-HFP), polyvinyl chloride, polypropylene oxide, polyacrylonitrile (PAN), polypropylene carbonate (PPC), polyvinyl alcohol (PVA) and polyvinyl pyrrolidone (PVP). As shown in Fig. 2D, the ionic conduction mechanism of the polymer solid electrolyte is that the polar groups (such as — O —, — N —, — S —, C = O, C = N) are continuously "coordinated" and "dissociated" with the Na+, and the diffusion and migration of the Na+ are realized under the action of electric field driving and molecular thermal motion[71⇓~73]. Among many polymer solid electrolytes mentioned above, PEO has good solubility for sodium salt, but it is semi-crystalline at room temperature, resulting in low conductivity at low temperature Na+ (10-7~10-5S·cm-1); Compare with that PEO polymer, the nitrogen atom in the PAN polymer molecule has weaker interaction with the Na+, and the coordination compound for by the nitrogen atom and the Na+ is easy to dissociate, so the pan polymer has higher Na+ conductivity,The conductivity of Na+ can reach 10-4S·cm-1;PPC at room temperature. The Na+ has the characteristics of high conductivity, good thermal stability and wide electrochemical window, and the battery can operate stably at higher temperatures (≤ 120 ℃), but the interface impedance between the polymer and the electrode is large. PVDF-HFP has been widely used because of its high dielectric constant, low glass transition temperature, wide electrochemical window, high mechanical properties and thermal stability[26,74⇓⇓~77]. In addition to a single polymer as a polymer solid electrolyte, the composite of two or more polymers can also significantly improve the conductivity and electrochemical stability of polymer electrolytes. For example, oxidized polyethylene electrolyte and succinonitrile composite or polyvinylpyrrolidone and polyaniline composite have been used as polymer composite electrolytes[78⇓~80].

2.3 Composite solid electrolyte

Inorganic solid electrolyte has many advantages, such as good mechanical properties, high Na+ conductivity, wide electrochemical window, high safety and thermal stability, but it has large interface impedance and poor compatibility with electrodes. Solid polymer electrolytes have good flexibility, plasticity and close interface contact, but they have some problems such as low conductivity of Na+ at room temperature, poor chemical/electrochemical stability and mechanical stability of the interface. SEs with excellent performance can be obtained by compounding inorganic and polymer solid electrolytes, and its advantages are as follows:
(1) enhance that interface contact between the electrode and the SEs and reduce the interface impedance; (2) good toughness and mechanical strength, and can relieve that volume change of the electrode in the charge-discharge proces and inhibit the dendrite growth; (3) Inorganic solid electrolyte filler can reduce the crystallinity of polymer matrix and improve the conductivity of solid electrolyte Na+[81⇓⇓⇓~85]. For example, the SEs prepared by Song et al. By compounding 1-ethyl-3-methylimidazolium bis (trifluoromethanesulfonyl) imide ionic liquid (EmimFSI) with NaClO4-PEO-5%SiO2 have the advantages of good toughness, high mechanical strength, and high Na+ conductivity at room temperature (1.3×10-3S·cm-1)[86]. Kim et al. Enhanced the interfacial contact and conductivity of SSBs by compounding NASICON-type solid electrolyte with PVDF-HFP[88]. Ling et al. Compounded polyether-vinyl acid ester, NASICON, PVDF-HFP to significantly improve the interfacial mass transfer kinetics and mechanical properties of SEs of Na+[89]. However, the non-composite solid electrolyte still has the problems of low room temperature Na+ conductivity (Figure 3C), high interface impedance with the electrode, and poor interface stability.
In addition to oxides, sulfides, polymers and other SEs, eutectic materials, plastic crystals, gel polymers, borohydrides, perovskite/antiperovskite SEs are also commonly used in SSBs. The borohydride solid electrolyte has sodium vacancy and anti-perovskite structure, high room temperature Na+ conductivity, good thermal stability, wide electrochemical window and good compatibility with sodium metal,Such as the composite (Na2B10H10)0.25/(Na2B12H12)0.75 and Na2(B12H12)0.5/(B10H10)0.5 electrolytes, the Na+ conductivity at room temperature can be as high as 10-4 and 10-3S·cm-1, respectively (Figure 3D)[87,90]. Antiperovskite solid electrolytes (Na3OX,X=Cl, Br, I) have the characteristics of high carrier concentration, low raw material cost, and high Na+ conductivity at room temperature (>10-3S·cm-1), but the Na+ transport channels of antiperovskite materials are limited and the optimization technology is relatively single, and at present, methods such as heating or doping alkaline earth metals are often used to introduce defects to improve the ionic conductivity of antiperovskite electrolytes.

3 All-solid-state sodium-ion battery challenge

3.1 SSBs interface and mechanical stability

In recent years, SEs have made a breakthrough in Na+ conductivity and electrochemical window, as shown in Fig. 4, but the solid-solid interface impedance caused by the interface between electrode and SEs, electrolyte grain boundary, the gap between cathode active particles, the gap between cathode active particles and binder or conductive agent, and the internal grain boundary of cathode materials has not been solved[20,91]. The new interface formed by the volume effect of the electrode, the fragmentation of the electrode active particles and the rupture of the interface layer during the charge-discharge process will also increase the interface impedance of the battery, reduce the charge-discharge efficiency and the stability of the battery. Therefore, an in-depth understanding of the interface characteristics of SEs/electrode, the mechanism of electrode volume change, and the interface modification strategy is essential to improve the cycling stability, capacity retention, and rate capability of SSBs.
图4 全固态钠离子电池示意图

Fig.4 Schematic illustration of the SSBs

3.2 Chemical and electrochemical stability of interface

Goodenough et al. Considered that when the electrochemical potential (μA) of the negative electrode is higher than the lowest unoccupied molecular orbital (LUMO) of the electrolyte, the electrons of the negative electrode are transferred to the electrolyte and reduced.However, when the electrochemical potential of the cathode (μC) is lower than the HOMO of the electrolyte, the electrolyte loses electrons and is oxidized, and only when both μA and μC are within the voltage window, the electrolyte and electrode are in a thermodynamically stable state[92]. Therefore, the construction of a laminated solid electrolyte thermodynamically stable to the positive or negative electrode at the electrode/SEs interface can improve the stability of the SEs and electrode interface and solve the problem of mismatch between the voltage window of SEs and electrode materials.

3.3 Interface space charge effect

The space charge layer caused by the chemical potential mismatch between different materials is one of the main sources of the interface impedance between the electrode and SEs. For example, when the chemical potentials of the electrodes and the SEs are not matched, the redistribution of charges at the interface minimizes the total energy of the interface, resulting in the enrichment of the same kind of charges on one side of the interface and the compensation of the opposite charges on the other side.So that an internal electric field opposite to the diffusion direction of a carrier is formed at the interface, and the electric field brings an additional charge migration energy barrier, thereby reducing the rate performance, the charge-discharge capacity and the cycle stability of the battery[93,94].

3.4 Ffect of dendrite on battery performance

The main reason for the deterioration of cycle performance and short circuit of SSBs is the growth of sodium dendrite caused by the uneven deposition of Na+ on the negative side during charge-discharge process. For the sodium metal anode, the continuous local growth of sodium dendrites during battery charging will lead to the rupture of the SEI layer, resulting in the contact of new sodium metal with the electrolyte and causing side reactions, thus reducing the coulombic efficiency of SSBs, and causing short circuit of the battery when the dendrites pierce the electrolyte. In addition, there are uneven charge, stress and sodium dendrite distribution on the surface of the negative electrode during discharge, which will lead to uneven stripping of sodium and the formation of "dead sodium", resulting in irreversible capacity loss of the negative electrode. In recent years, significant progress has been made in the study of dendrite growth of SSBs, but there are still great challenges in the in-situ tracking and observation of the growth law of SSBs sodium dendrites, and the mechanism and theory of the effect of dendrites on battery performance still need to be further improved.
To sum up, the study of SSBs interface should be devoted to revealing and solving the scientific problems of interface instability and poor kinetics of Na+ conduction, and it is urgent to make a breakthrough in the study of interface. However, there is still a lack of in-depth study of SSBs from the microscopic (or quantum) level to reveal their interfacial characteristics, such as how the physical, chemical, and electrochemical properties of the SEI layer affect the Na+ interfacial transport and the stability of SSBs. Therefore, it is extremely necessary to analyze the interface problems of SSBs from the micro level, and to explore the interface characteristics and solve the interface problems from multi-disciplinary and multi-scale by combining advanced interface characterization, simulation, simulation technology and computational methods.

4 Interface engineering of all-solid-state sodium-ion battery

SSBs have the advantages of high energy density, good safety and long life, but they still face great challenges in improving the interfacial chemical stability, electrochemical stability and interfacial mass transfer kinetics. The ideal electrode/SEs interface should have the following characteristics: (1) the electrode and SEs contact tightly and the interface layer has high Na+ conductivity, electronic insulation and uniform diffusion of Na+ to promote uniform sodium deposition and sodium ion interface transport; (2) excellent mechanical properties to mitigate positive electrode volume change and inhibit negative electrode dendrite growth; (3) Chemically/electrochemically and structurally stable with high interfacial compatibility and long cycling stability. Controlling the electrode/SEs interface, developing composite electrode materials, and designing the cell structure are the main ways to improve the thermodynamic stability and mass transfer kinetic performance of the interface.

4.1 Positive electrode/SEs interface

The positive electrode is composed of an active material, a binder, and a conductive agent. As shown in fig. 4, there are complex solid-solid interfaces between SEs and the positive electrode, and between different phases of the positive electrode. The main problems of the cathode side interface of SSBs are the poor thermodynamic stability of the interface between SEs and cathode, the mismatch of electrochemical windows, the mutual diffusion of interface elements, the poor contact of solid-solid interface, the space charge layer, and the electrode volume effect.

4.1.1 Adding interface wetting agent

It is an effective way to reduce the interfacial impedance by adding an interfacial sizing agent between the cathode and SEs to transform the "point" contact between solid particles into "surface" contact. Ionic liquids are often used as electrode/SEs interface modification materials due to their strong interfacial affinity, high Na+ conductivity at room temperature, and high thermal and electrochemical stability. As Zhang et al. Modified the interface between the cathode and SEs by adding nitromethyl-n-propylpiperidine bis (fluorosulfonyl) imide (PP13FSI) ionic liquid (IL), as shown in Figure 5A, the reversible capacity of the 10000 all-solid-state sodium-ion battery was still as high as 90 mA·h·g-1 after 10000 cycles at 10 C rate at room temperature[58]. However, the poor conductivity of ILs at low temperature Na+ limits their large-scale application in batteries.
图5 (a)NVP|IL/SE|Na电池界面示意图[58];(b)Na2S-Na3PS4-CMK-3复合正极示意图[95];(c)S-MSP20-Na3SbS4正极制备工艺[96];(d,e)正极活性材料与塑性晶体固体电解质复合正极示意图[97];(f)Na|PEO-SN-NaClO4/PAN-Na3Zr2Si2PO12-NaClO4|PB电池在0.2 C下循环性能图[98];(g)非对称固体电解质示意图

Fig.5 (a) Schematic of the interface for NVP|IL/SE|Na batteries[58]; (b) schematic of the Na2S-Na3PS4-CMK-3 composite cathode[95]; (c) preparation process for S-MSP20-Na3SbS4 cathode[96]; (d, e) schematic of plastic-crystal electrolyte and active material in composited cathode[97]; (f) cycling performance of the Na|PEO-SN-NaClO4/PAN-Na3Zr2Si2PO12-NaClO4|PB cell at 0.2 C[98]; and (g) illustration of the asymmetric solid electrolytes

4.1.2 Composite cathode material

The composite of cathode active material and electrolyte has good mechanical properties and high ion transmission performance, and the better toughness significantly enhances the contact between the cathode and SEs and reduces the interface impedance. Fan et al. Prepared the Na2S-Na3PS4-CMK-3 (mesoporous carbon material) composite cathode through a melt-casting-annealing-precipitation process, as shown in Fig. 5 B, which realized the close contact of Na2S cathode, Na3PS4 electrolyte, and CMK-3 conductive agent, and the reversible capacity of the solid-state sodium-ion battery was still as high as 650 mA·h·g-1 after 50 cycles at 60 ° C and 50 mA·g-1[95]. In addition to the composite cathode material, reducing the particle size of the cathode active material or improving the dispersion of the active material in the composite cathode can also effectively alleviate the cathode volume effect and improve the interface stability[100,101]. As shown in fig. 5C, reducing the particle size of the positive active material can weaken the influence of the volume change of the positive active particle on the mechanical stability of the positive electrode during the charge-discharge process. However, there is still a problem of poor solid-solid interface contact inside the positive electrode[96]. The study shows that the addition of plastic crystals composed of succinonitrile (SN) and NaClO4 to the Na3Zr2Si2PO12 and Na3V2(PO4)3 composite cathode can effectively improve the cathode material solid-solid contact and alleviate its volume effect, as shown in Fig. 5d, e, SSBs have excellent rate performance, capacity retention and cycling stability[97].

4.1.3 Composite solid electrolyte

The composite of inorganic filler and polymer electrolyte has good toughness and high mechanical strength, which can not only enhance the interfacial contact between the electrode and SEs, but also effectively inhibit the dendrite growth, which is a hot topic in the field of SSBs[33,81,102⇓~104]. It is reported that the Na3Zr2Si2PO12-PVDF-HFP-NaFSI-TEGDME composite solid electrolyte has good contact performance and high stability with the electrode interface, and the capacity retention of the corresponding NaFePO4|Na3Zr2Si2PO12-PVDF-HFP-NaFSI-TEGDME|C (hard carbon) battery is as high as 96% after 200 cycles at 0.2 C. Goodenough et al. Stacked two electrolytes, PEO-SN-NaClO4, which is highly compatible with sodium metal, and PAN-Na3Zr2Si2PO12-NaClO4, which is highly matched with the cathode voltage window, to prepare a PEO-SN-NaClO4/PAN-Na3Zr2Si2PO12-NaClO4 double-layer solid electrolyte, as shown in Figure 5 f. The electrochemical window of the composite solid electrolyte was as high as 4.8 V and the cycle stability of the battery was improved[98]. The study shows that a thermodynamically stable electrode/SEs interface can be obtained by preparing an asymmetric laminated composite solid electrolyte (fig. 5g) with materials that are chemically and electrochemically stable to the positive and negative electrodes[99].

4.2 Anode/SEs interface

4.2.1 Surface coating modification

The interface problems between anode and SEs are mainly reflected in poor contact, poor compatibility and sodium dendrite growth. The introduction of a passivation layer or an interfacial buffer layer on the surface of the electrode or SEs is a common method to enhance the interfacial contact between the anode and SEs and to improve the interfacial compatibility on the anode side. Chemical vapor deposition and physical vapor deposition are that most common method to enhance the interfacial contact and stability of the anode and SEs. As a surface modification technique of chemical vapor deposition, atomic layer deposition (ALD) can coat materials on the substrate surface in the form of monoatomic films with controllable deposition thickness, so it is widely used in the interface modification of SSBs. For example, Luo et al. Used trimethylaluminum and oxygen as precursors to deposit Al2O3 layer by layer on the surface of sodium metal by low temperature plasma enhanced atomic layer deposition (PEALD) to enhance the stability of the anode/SEs interface, as shown in Figure 6A, the Na/Al2O3|EC/DEC/NaClO4|Na/Al2O3 battery showed excellent stability compared with the sodium metal anode without surface modification[105]. In addition, as shown in Figure 6B, the construction of graphene modification layer on the surface of NASICON by chemical vapor deposition technology can also effectively reduce the interface impedance and improve the stability of the battery[106].
图6 (a)PEALD构筑Al2O3钝化层示意图[105];(b)化学气相沉积石墨烯修饰NASICON表面示意图[106];(c)NaClO4/FEC溶液改性Na金属表面示意图[107];(d)Na|SnS2-Na3Zr2Si2PO12界面改性示意图[108];(e)固体电解质与金属Na界面接触模型[109];(f)Na-SiO2复合材料与NASICON界面[110]

Fig.6 (a) Schematic of PEALD process for Al2O3 layer[105]; (b) schematic of the CVD-grown graphene-like interlayer on NASICON surface[106]; (c) NaClO4/FEC modified surface of Na[107]; (d) schematic of the Na|SnS2-Na3Zr2Si2PO12 interface[108]; (e) contact model of SEs and sodium metallic[109]; (f) interfaces between Na-SiO2 composite and NASICON[110]

4.2.2 Solid electrolyte interface layer (SEI)

Lu et al. Reacted fluoroethylene carbonate (FEC) solution dissolved with NaClO4 with metallic sodium to obtain a NaF-rich SEI layer[107]. As shown in Figure 6C, the NaF-rich SEI can significantly reduce the impedance and enhance the interfacial stability of the Na|Na3V2(PO4)3 battery, and the capacity retention of the assembled battery is still 80% after 200 cycles at 2 C rate. However, the chemical reaction between electrolyte and sodium metal is difficult to obtain a uniform SEI layer, which can not fundamentally solve the problem of uneven deposition of Na+ at the interface. Wang et al. Constructed an ion/electron mixed conductive layer composed of Na-Sn alloy and Na2S in situ at the interface of anode and solid electrolyte by reacting SnS2 with Na anode, as shown in Fig. 6 d. The mixed conductive layer promoted the rapid diffusion and transport of electrons and Na+ at the interface of anode/SEs, resulting in high capacity retention and rate capability of Na3V2(PO4)3|Na3Zr2Si2PO12-SnS2|Na solid-state battery[108].

4.2.3 Flexible electrolyte sandwich

Oxide solid electrolyte has high mechanical strength and thermodynamic stability, but the problems of large interface impedance between SEs and electrode and sodium dendrite growth need to be solved before its popularization and application. Zhou et al. Introduced a cross-linked polyethylene glycol methyl ether acrylate (CPMEA) interlayer at the anode/SEs interface to effectively enhance the Na-NASICON interface contact and interface stability, as shown in Fig. 6e, the impedance of the Na | CPMEA/NASICON/CPMEA | Na solid-state battery was reduced from 4000Ω·cm-2 to 1000Ω·cm-2,Na|NaTi2(PO4)3, and the coulombic efficiency of the solid-state battery was still as high as 99.7% after 70 cycles at 65 ° C[109]. Despite the good flexibility and interfacial wettability of the polymer electrolyte interlayer, the low room temperature Na+ conductivity and poor mechanical properties of the polymer make it difficult to effectively inhibit dendrite growth.

4.2.4 Composite anode material

In recent years, composite anodes and alloy anodes are often used to improve the interfacial ion transport and interfacial stability of SSBs anodes. For example, Fu et al. Prepared the Na-SiO2 electrode material by compounding amorphous SiO2 with sodium metal, as shown in Fig. 6 f, the Na-SiO2 electrode and NASICON electrolyte had excellent interfacial wettability and stability, and the impedance of the Na-SiO2|NASICON|Na-SiO2 battery was reduced from 1658 to 101Ω·cm-2[110]. In addition, composites of carbon materials and metal oxides, carbon materials and metal sodium, sodium-tin alloy have also been reported to have good interfacial wettability and stability in SSBs.

4.3 Battery Structure Design

The integral structure of SEs and electrode materials and the in-situ curing of the interface are the effective methods to achieve atomic-level contact between the electrode and SEs[111]. Zhao et al. Constructed a chemical crosslinking structure between the PEO electrolyte and the carbon-sodium composite anode to enhance the SEs/electrode interface contact, as shown in Fig. 7 a and B, and the capacity retention of the Na-C|PEO20NaFSI|Na3V2(PO4)3 solid-state battery was still higher than 80% after 5000 cycles at 0.1 C[112]. Chen et al. improved the interfacial contact between the electrode and SEs through the cathode-electrolyte integrated structure prepared by coating the composite solid electrolyte and the electrode material, as shown in Figure 7c, which can effectively reduce the interfacial impedance and enhance the electrochemical energy stability[113]. Yamauchi et al. Prepared a solid electrolyte-cathode integrated structure by co-sintering β"-Al2O3 as a matrix with Na2FeP2O7 cathode material at 550 ° C, as shown in Fig. 7 d, which realized the close contact between SEs and the cathode interface, and the assembled SSBs showed a high charge-discharge reversible capacity at room temperature[114]. Inoishi et al. Reported a Pt|Na3-xV2-xZrx(PO4)3|Pt“ single-phase "all-solid-state sodium-ion battery, as shown in Figure 7E, the V3+/V2+ (negative electrode) and V3+/V4+ (positive electrode) conversion reactions during battery charging and discharging were completed at the current collector and Na3-xV2-xZrx(PO4)3 interface, eliminating the electrode/SEs interface impedance."[115]. To sum up, the integrated structure of SEs and electrode can obtain SEs/electrode interface with close contact and high mechanical stability, which can effectively solve the problems of poor Na+ transmission performance and poor thermodynamic stability of SSBs interface.
图7 (a)金属钠-碳复合负极与固体聚合物化学交联界面示意图[112];(b)Na-C|PEO20NaFSI| Na-C和Na|PEO20NaFSI|Na电池在0.1、0.2和0.3 mA下循环电压曲线[112];(c)正极和固体电解质叠层薄膜示意图[113];(d)Na2FeP2O7正极与β''-Al2O3电解质一体化结构示意图[114];(e)Pt|Na3-xV2-xZrx(PO4)3|Pt单相全固态电池示意图[115]

Fig.7 (a) Illustration of the interfaces between solid-state polymer and Na-C anode[112]; (b) voltage curves of the Na-C|PEO20NaFSI| Na-C and Na|PEO20NaFSI|Na batteries at a current density of 0.1, 0.2, and 0.3 mA[112]; (c) schematic of the cathode-supported solid electrolyte membrane[113]; (d) illustration of the Na2FeP2O7 and β''-Al2O3 integrated structure[114]; (e) schematic illustration of the Pt|Na3-xV2-xZrx(PO4)3|Pt battery[115]

5 Conclusion and prospect

All-solid-state sodium-ion batteries, with solid electrolyte as the core material, have the advantages of abundant raw materials, low cost and high energy density, and are excellent candidates for large-scale energy storage. In this paper, the research progress of inorganic solid electrolytes, polymer solid electrolytes and composite solid electrolytes is summarized, the challenges and countermeasures of SSBs interface are discussed, and the research and achievements of full SSBs interface characteristics and interface engineering are reviewed. In recent years, significant progress has been made in the study of SSBs, but practical applications still need to solve the problems of low ionic conductivity, poor interface compatibility and large interface impedance of cells.
The room temperature ionic conductivity, electrochemical stability, and mechanical properties of SEs are the key parameters of SSBs. The composition modification and structure design of SEs are the common methods to improve their ionic conductivity and electrochemical stability. For example, inorganic solid electrolytes can improve their ionic conductivity and electrochemical stability by element substitution or doping, while the room temperature ionic conductivity of polymer electrolytes can be improved by chain blending, copolymerization or crosslinking. PolySEs composed of polymer and solid filler can give consideration to both the flexibility of organic polymer and the rigidity of inorganic solid filler, thus improving its mechanical properties. In the future study of SEs, we suggest the following four breakthroughs: (1) using atomic-scale characterization and modeling techniques to deeply understand the electrochemical and mechanical stability of SEs and enrich the Na+ transport kinetics of SEs; (2) to improve the low temperature Na+ conductivity of SEs by deeply studying the Na+ conduction mechanism, material composition and structural characteristics of SEs through the intersection of physics, electrochemistry and material science; (3) optimize that topology of the SEs and ensure optimal sodium coordination in the material; (4) Combining density functional theory and machine learning to carry out theoretical research to obtain appropriate SEs.
The bottleneck of SSBs is to improve the interface impedance, interface compatibility, dendrite growth and electrode volume effect between electrodes and SEs. At present, methods such as introducing interfacial wetting agents, SEI/CEI layers, interfacial flexible interlayers, or designing composite solid electrolytes, composite electrode materials, interfacial in-situ curing, and designing new battery structures are usually used to reduce the interfacial impedance between electrodes and SEs and improve the interfacial stability and compatibility. SEs with low elastic modulus, active materials with small volume change during charge-discharge process, and SEs nanoparticles with short ion diffusion path will also help to improve the stability and electrochemical performance of SSBs. Dendrite is the main reason for the poor stability and short circuit of SSBs. Generally, the electrode/SEs interface layer with high conductivity, electronic insulation and good mechanical properties of Na+ can promote the uniform deposition of sodium or inhibit dendrite. In addition, by designing a flat anode surface, the dendrite growth induced by protrusions can be slowed down, or new materials and interface modification technologies can be developed to induce uniform sodium deposition. In a word, interface compatibility and interface impedance are the main factors that hinder the development and application of SSBs. We suggest the following methods to study the battery interface. (1) Low cost, scalable and simple operation process is the premise of large-scale application of SSBs interface engineering technology; (2) Advanced analysis and characterization techniques of SSBs interface are very important for the study of SSBs interface stability, interface ion transport kinetics, space charge layer and other scientific issues, as well as the study of interface chemistry, sodium deposition and stripping behavior; (3) Adopt advanced battery structure and material design to improve the performance of SSBs; (4) The study of the structural evolution of the interface during the charge-discharge process by combining kinetic simulation and thermodynamic calculation will contribute to the development of SSBs.
In summary, the study of the interfacial Na+ transport properties and thermodynamic stability of SSBs is essential to improve the electrochemical performance of batteries. At present, the study of SSBs still faces many challenges and needs further exploration. Researchers should combine experimental and theoretical calculation methods to solve the interface problem of SSBs, break through the design bottleneck of key materials and devices of SSBs, and promote their practical application.

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