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Lithium–sulfur batteries (LSBs) are considered one of the most promising candidates for next-generation energy storage owing to their large energy capacity. Tremendous effort has been devoted to overcoming the inherent problems of LSBs to facilitate their commercialization, such as polysulfide shuttling and dendritic lithium growth. Pouch cells present additional challenges for LSBs as they require greater electrode active material utilization, a lower electrolyte–sulfur ratio, and more mechanically robust electrode architectures to ensure long-term cycling stability. In this review, the critical challenges facing practical Li–S pouch cells that dictate their energy density and long-term cyclability are summarized. Strategies and perspectives for every major pouch cell component—cathode/anode active materials and electrode construction, separator design, and electrolyte—are discussed with emphasis placed on approaches aimed at improving the reversible electrochemical conversion of sulfur and lithium anode protection for high-energy Li–S pouch cells.

Ceramic composite separator is more competitive than traditional polyolefin separator in the field of power supply for superior thermal stability and wettability of liquid electrolyte. In this study, we develop a two-steps method that modifies SiO2 with acrylamide (AM) by grafting process and prepare a functional SiO2 composite separator (PE/SiO2-AM). This kind of composite separator exhibits similar size-shrinkage (8.8%) to that of PE/ SiO2 composite separator at the tested temperature, lower than 18.1% of bare PE separator, and is electrochemically stable below 4.5 V (vs. Li/Li+). In addition, the Li-symmetric cells employing PE/SiO2-AM composite separator have the lowest overpotential and an improved lithium-ion transference number of 0.44. It is demonstrated from DFT calculation that the electron-rich species of imide group is able to uniformly disperse lithium-ion flux at the interface of electrolyte/lithium anode, and contributes to lithium-ion transport process. After assembling the LiCoO2/Li half cells, the cell with PE/SiO2-AM composite separator displays better cycle performance and higher discharge capacity when compared with other separators. Therefore, functional ceramic separator would be more attractive for next-generation lithium metal battery with high energy density.

Hybrid silica-based nanofillers were synthesised by grafting short chains of poly(ethylene glycol) (PEG) with different molecular weight on the surface of SiO2 porous nanoparticles. Based on this approach, homogeneous poly(ethylene oxide) (PEO)-based ceramic-in-polymer solid-state electrolytes with SiO2 loadings up to 23 wt% were obtained, thanks to the high compatibility between the two phases endowed by the grafted PEG chains. These electrolytes showed satisfying ionic conductivity and excellent resistance against dendrite piercing that enabled long operation, for more than 350 h, under continuous stripping/plating of lithium in symmetric Li/electrolyte/Li cells. Additionally, the operating life of these devices was improved by the self-healing reaction between Li dendrites and silica fillers, being able to reinstate the cycling after short circuit. Finally, a lithium metal full cell, equipped with LiFePO4 positive material and the solid-state electrolyte containing 18 wt% of SiO2, demonstrated high stability against dendrite penetration and discharge capacity at 70 °C comparable to cells based on liquid analogues.

LiNO3 has been widely used as an effective electrolyte additive in lithium-sulfur (Li-S) batteries to suppress the polysulfide shuttle effect. To better understand the mechanism of suppressed shuttle effect by LiNO3, herein we report a comprehensive investigation of the influence of LiNO3 additive on the formation process of the solid electrolyte interphase (SEI) layer on lithium anode of Li-S batteries by operando X-ray absorption spectroscopy (XAS). We observed that a compact and stable SEI layer composed of Li2SO3 and Li2SO4 on top of lithium anode is formed during the initial discharge process due to the synergetic effect of shuttled polysulfides and LiNO3, which can effectively suppress the subsequent reaction between polysulfides in electrolyte and lithium metal and thus result in the alleviation of polysulfide shuttle effect. In contrast, when using electrolyte without LiNO3, the shuttled polysulfides continuously react with lithium metal to form insulating Li2S on lithium anode, leading to the irreversible capacity loss. Our present operando XAS study provides a valuable insight into the important role of LiNO3 for the protection of lithium anodes, which will be beneficial for the further development of new electrolyte additives for high-performance Li-S batteries.

Amorphous lithium phosphorous oxynitride film was coated directly on pre-treated lithium metal as anode of lithium air battery by radio-frequency sputtering technique from a Li 3 PO 4 target. The structure and composition of modified anode was analyzed before and after charge/discharge test in a lithium-air battery, which comprises 0.5 M LiNO 3 /TEGDME as the electrolyte and super P carbon as cathode. Batteries were galvanostatically discharged by an Arbin BT-2000 battery tester between open current voltage and 2.15 V vs. Li + /Li at various current regimes ranging from 0.1–0.4 mA/cm 2 . Compared with fresh lithium, LIPON-coated anode exhibited better electrochemical performance. Good charging efficiency of 90% at a narrower voltage gap with high ionic conductivity of 9.4 × 10 −5 S/cm was achieved through optimizing lithium pre-treated conditions, sputtering N 2 flows and suitable solute for electrolyte.

In the last decade, dealloying has become a popular and effective strategy to fabricate nanoporous metals used in electrochemical applications such as electrocatalysis and energy storage. This review article summarizes the recent literature on dealloyed non-noble metals and oxides evaluated as lithium-ion battery anode materials. The importance of dealloying parameters to achieve desired pore and ligament sizes is emphasized. A future research roadmap is also provided.