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Solid composite electrolytes exhibit tremendous potential for practical all-solid-state lithium metal batteries (ASSLMBs), whereas the interfacial contact between cathode and electrolyte remains a long-standing problem. Herein, we demonstrate an integrated design of a double-layer functional composite electrolyte and cathode (ID-FCC), which effecti...
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... Solid-state Li-S batteries (SSLSBs) with inorganic solid electrolytes do not suffer from the capacity fade associated with the 'polysulfide shuttle' phenomenon in liquid electrolytes 8,9 . They involve direct conversion between S and Li 2 S during cycling 4,10 , and rely entirely on the interfaces between the solid electrolytes, conductive carbon and S species to transfer charge 11,12 . This reliance paired with the insulating nature of S (electrical conductivity of approximately 5 × 10 −18 S cm −1 ) is untenable. ...
Solid-state Li–S batteries (SSLSBs) are made of low-cost and abundant materials free of supply chain concerns. Owing to their high theoretical energy densities, they are highly desirable for electric vehicles1–3. However, the development of SSLSBs has been historically plagued by the insulating nature of sulfur4,5 and the poor interfacial contacts induced by its large volume change during cycling6,7, impeding charge transfer among different solid components. Here we report an S9.3I molecular crystal with I2 inserted in the crystalline sulfur structure, which shows a semiconductor-level electrical conductivity (approximately 5.9 × 10⁻⁷ S cm⁻¹) at 25 °C; an 11-order-of-magnitude increase over sulfur itself. Iodine introduces new states into the band gap of sulfur and promotes the formation of reactive polysulfides during electrochemical cycling. Further, the material features a low melting point of around 65 °C, which enables repairing of damaged interfaces due to cycling by periodical remelting of the cathode material. As a result, an Li–S9.3I battery demonstrates 400 stable cycles with a specific capacity retention of 87%. The design of this conductive, low-melting-point sulfur iodide material represents a substantial advancement in the chemistry of sulfur materials, and opens the door to the practical realization of SSLSBs.
... The variances in the electrochemical process have given rise to a multitude of distinct principles and experimental approaches to implement the interfacial strategies. In recent years, a number of high-quality review articles have summarized the evolution of SSEs and the electrode/electrolyte interfacial design in Li-S batteries [56][57][58][59]. Yu et al. [58] provided a survey of the research progress in the electrode/electrolyte interface in all-solid-state and hybrid electrolyte Li-S batteries. ...
The utilization of solid-state electrolytes (SSEs) presents a promising solution to the issues of safety concern and shuttle effect in Li–S batteries, which has garnered significant interest recently. However, the high interfacial impedances existing between the SSEs and the electrodes (both lithium anodes and sulfur cathodes) hinder the charge transfer and intensify the uneven deposition of lithium, which ultimately result in insufficient capacity utilization and poor cycling stability. Hence, the reduction of interfacial resistance between SSEs and electrodes is of paramount importance in the pursuit of efficacious solid-state batteries. In this review, we focus on the experimental strategies employed to enhance the interfacial contact between SSEs and electrodes, and summarize recent progresses of their applications in solid-state Li–S batteries. Moreover, the challenges and perspectives of rational interfacial design in practical solid-state Li–S batteries are outlined as well. We expect that this review will provide new insights into the further technique development and practical applications of solid-state lithium batteries.
... To date, there have been some professional and excellent review articles on the interface issues between electrolytes and electrodes in allsolid-state batteries. Generally, these articles summarize the interface improvement methods from the overall perspective of all-solid-state batteries, but they have not achieved in-depth and detailed effects [46,47]. Moreover, there are very few review articles specifically summarizing the interface issues between sulfide SEs and anode, and the few published articles on this topic have been around for some time. ...
... Due to ultra-high theoretical energy, sulfur is considered as one of the most promising cathodes, but both sulfur and its final discharge product Li2S exhibit poor electronic and ionic conductivity, resulting in sluggish kinetics and poor utilization of active materials. Therefore, the interface problem shown in Fig. 4 b plays a crucial role in improving the electrochemical performance of lithium-sulfur batteries [107]. Furthermore, the microstructure of electrode plays a vital role in controlling charge transport in the electrode composite, and a stable microstructure is essential for battery research. ...
Solid-state lithium batteries (SSLBs) are one of the most promising next-generation energy storage devices. Firstly, with the purpose of improving the stability of the passivation film on the electrode surface, this paper focuses on the effective methods to improve the overall performance of batteries. Secondly, the compatibility between different electrolytes and electrodes is analyzed, aiming to select an electrolyte suitable for promoting ion flow while improving the permeability of electrolytes and electrodes as well as the SEI film by inhibiting lithium dendrites. The basic content of this paper is shown in Fig. 1, in which the interfacial compatibility of SSLBs is determined by positive and negative electrodes, electrolyte, and SEI film, like a hamburger threaded on a bamboo stick. This paper also reviews major methods currently used to prepare SEI films. It can be concluded that Li dendrites are one of the most significant factors affecting the interfacial compatibility of SSLBs. To achieve good interfacial compatibility of SSLBs, it is necessary to increasingly serious lithium dendrites and to propose as many use schemes as possible.
... [1][2][3] However, the following defects have hampered the application of Li-S batteries: (1) the large volume expansion (80%) that occurs in cathodes when the conversion reaction occurs; (2) the shuttle effect of Li polysulphides (LiPSs); and (3) the electrical insulation nature of S and its process products (Li 2 S 2 /Li 2 S). [4][5][6] Commendable progress has been made in the study of both modied separators and cathodes to ameliorate the lifespans and energy density of Li-S batteries. ...
Lithium-sulphur (Li-S) batteries are high-energy-density and cost-effective batteries. Herein, petal-like Ni1-x Mn x (OH)2 (x ≈ 0.04) nanosheets were synthesised using a hydrothermal method and the electrical conductivity of Ni(OH)2 was improved by applying the cathode functional materials in Li-S batteries. With up to 5 mg cm-2 of S content in the cathode, the fabricated Ni1-x Mn x (OH)2 electrode exhibited specific discharge capacities up to 1375 and 1150 mA h g-1 at 0.2 and 0.5C, and retained this capacity at 813 and 714 mA h g-1 after 200 cycles, respectively. Electrochemical measurement results show that Ni1-x Mn x (OH)2 plays a critical role in Li-S batteries as it has a larger specific surface area than Ni(OH)2, which has superior adsorption performance toward lithium polysulphides. Moreover, the conductivity performance of Ni1-x Mn x (OH)2 is significantly better than that of Ni(OH)2, which improves the electrochemical reaction kinetics of the Li-S batteries.
... However, several electro-chemo-mechanical challenges exist as sulfur cathodes undergo severe volume changes and microstructure evolution during electrochemical cycling [65][66][67][68]. ...
The development of next-generation batteries, utilizing electrodes with high capacities and power densities requires a comprehensive understanding and precise control of material interfaces and architectures. Electro-chemo-mechanics plays an integral role in the morphological evolution and stability of such complex interfaces. Volume changes in electrode materials and the chemical interaction of electrode/electrolyte interfaces result in non-uniform stress fields and structurally-different interphases, fundamentally affecting the underlying transport and reaction kinetics. The origin of this mechanistic coupling and its implications on degradation is uniquely dependent on the interface characteristics. In this review, the distinct nature of chemo-mechanical coupling and failure mechanisms at solid-liquid interfaces and solid-solid interfaces is analyzed. For lithium metal electrodes, the critical role of surface/microstructural heterogeneities on the solid electrolyte interphase (SEI) stability and dendrite growth in liquid electrolytes, and on the onset of contact loss and filament penetration with solid electrolytes (SEs) is summarized. With respect to composite electrodes, key differences in the microstructure-coupled electro-chemo-mechanical attributes of intercalation- and conversion-based chemistries are delineated. Moving from liquid to solid electrolytes in such cathodes, we highlight the significant impact of solid-solid point contacts on transport/mechanical response, electrochemical performance, and failure modes such as particle cracking and delamination. Lastly, we present our perspective on future research directions and opportunities to address the underlying electro-chemo-mechanical challenges for enabling next-generation lithium metal batteries.
... Since their discovery at the end of the 20 th century, lithium (Li)-ion batteries (LIBs) have been widely applied in many fields such as portable electrical devices, electric vehicles (EVs), and grid storage stations, because of their advantages including high energy density, high operating voltage, and excellent cycle stability [1,2]. Traditional LIBs can offer volumetric and gravimetric energy densities of up to ~ 770 Wh•L −1 and ~ 300 Wh•kg −1 , respectively [2][3][4][5][6][7][8]; however, these levels are still not enough to meet the consumers' requirements [9]. ...
... In order to facilitate the dissociation of the lithium salts in the polymer hosts, the lithium salts should have low lattice energy and the polymers should have high dielectric constant [30]. The ionic conductivity (σ) of the polymer electrolytes can be expressed as follows [31] σ = ∑niqiμ i (1) in this formula, ni is the concentration of carriers, qi is the charge number of the mobile ions, and μi is the mobility of the carriers. It can be seen from this formula that, for a certain ion species, the charge qi is fixed, then the ionic conductivity is proportional to the number of mobile ions and the ion mobility. ...
... In contrast, the additions of low-dielectric-constant EtAc (donor number: 17.1, ε = 6) and ClBz (donor number: 2, ε = 5.6) can decrease the Tg, but cannot decrease the A and the activation energy, and therefore they had little effect on the ionic conductivity of the electrolyte (Fig. 14(c)). 1 H NMR characterizations showed that the addition of DMF into the PTHF5 electrolyte (dissolved in chloroform) caused the alpha proton peak to shift back upfield, indicating the weakened O-Li + interaction, while the addition of EtAc had little effect on the alpha proton peak and the O-Li + interaction (Fig. 14(d)). The additions of DMF and EtAc into the PTHF5 system also caused strong and poor deshieldings of Li + , respectively, indicating a loosening of the strong O-Li + interaction by DMF (Fig. 14(e)). ...
Solid polymer electrolytes (SPEs) possess comprehensive advantages such as high flexibility, low interfacial resistance with the electrodes, excellent film-forming ability, and low price, however, their applications in solid-state batteries are mainly hindered by the insufficient ionic conductivity especially below the melting temperatures, etc. To improve the ion conduction capability and other properties, a variety of modification strategies have been exploited. In this review article, we scrutinize the structure characteristics and the ion transfer behaviors of the SPEs (and their composites) and then disclose the ion conduction mechanisms. The ion transport involves the ion hopping and the polymer segmental motion, and the improvement in the ionic conductivity is mainly attributed to the increase of the concentration and mobility of the charge carriers and the construction of fast-ion pathways. Furthermore, the recent advances on the modification strategies of the SPEs to enhance the ion conduction from copolymer structure design to lithium salt exploitation, additive engineering, and electrolyte micromorphology adjustion are summarized. This article intends to give a comprehensive, systemic, and profound understanding of the ion conduction and enhancement mechanisms of the SPEs for their viable applications in solid-state batteries with high safety and energy density.
... SIEs, such as Li7La3Zr2O12, have high lithium-ion conductivity (>1×10 −4 S cm −1 ) at room temperature [13,14] and usually can be integrated with the cathode through high pressure to improve the interface compatibility [15]. But the pores and cracks at the interfaces of inorganic ceramic conductor block the lithium-ion conduction and lead to carrier depletion and battery polarization [16]. Out of expectation, inorganic ceramic conductors with high electron conductivity (~10 −7 S cm −1 ) can induce the formation and migration of lithium dendrites in the ceramic [17,18]. ...
... The assimilation of SEs in Li-S batteries is focused as one of the impressive tactics to mitigate the high volume expansion that occurs in sulfur cathode in Li-S batteries. The shuttle effect that developing at the cathode-electrolyte interfaces, lethargic cathode kinetics due to lower conductivity of the sulfur cathode and its final discharge product Li 2 S, makes supplementary hindrances to the ASS Li-S battery (ASS-LSB) research [53]. The SE can play a pivotal role in Li-S batteries to alleviate the shuttle effect due to the natural absence of organic solvents. ...
All-Solid-State Batteries (ASSBS) are considered as one of the mesmerizing technologies for next-generation energy storage with its inherent safe nature. The versatility of nanomaterials can roadmap to the high power/energy storing ASSBs for transferable, bendable, foldable electronics, transportation, and grid-scale energy storage. The most challenging part of designing a comprehensive-nanoscale ASSB assembly, is the down scaling of the particle size of solid electrolyte, upholding its super ionic conductivity. In this context, materials with nanoscale-sized structural features and a large electrochemically active surface can change the paradigm for energy storage that transpire manifold improvement in power and cycle life characteristics. This review primarily provides an outlook on recent progress in the application of the concept of ‘nano’ for energy harvesting in different dwellings of ASSB assemblies. The review also deliberate successful strategies for the exploitation of nanomaterials deployable at the most challenging solid-solid interfaces of ASSBs. Attention is focused on the importance of designing ‘nanoscale particle articulated’, electrode-solid electrolyte interfaces and their aspects in lithium-ion movements.
... Lithium sulfur (Li-S) battery is attractive due to high theoretical energy-density [1,2]. Meanwhile, the high abundance of sulfur in the crust makes it to be attractive for electric vehicles and future energy-storage system [3][4][5]. Nevertheless, in the Li-S battery cathode, sulfur has some issues, which lead to capacity decay, poor rate-performance and Coulombic efficiency [6][7][8]. ...
Lithium-sulfur battery is of great interest because of high theoretical energy-density and low cost. While the large volumetric change of sulfur and shuttle effect restrict its development. Here, we develop a one-dimensional chain-like Fe3O4 prepared through the self-assembly of magnetic particles as sulfur host. The Fe3O4@S cathode shows a capacity 457 mAh g⁻¹ after 150 cycles, and a 99% Coulombic efficiency. In addition, rate-performance after three rounds delivers stable capacities after repeated measurements. The electrochemical performance is ascribed to the one-dimensional nano-chain structure provides fast pathways for electron transportation, and accommodates volumetric change of sulfur in charge-discharge. Those findings provide a potential strategy to develop high-performance nanocomposite for secondary batteries.
