A "solo-solvent de novo liquid-phase" method for synthesizing sulfide solid electrolyte Li6PS5Cl.

We report a "solo-solvent de novo liquid-phase" method of synthesizing a highly-favored sulfide electrolyte (Li6PS5Cl) for developing all-solid-state lithium batteries. The key chemistry for such a successful method is that tetrahydropyrrole enables in situ synthesis of the critical precursor Li2S from cheap and air-stable precursors of lithium chloride and sodium sulfide.

Performance Enhancement of the Li6PS5Cl-Based Solid-State Batteries by Scavenging Lithium Dendrites with LaCl3-Based Electrolyte.

Li6PS5Cl (LPSC) is a very attractive sulfide solid electrolyte for developing high-performance all-solid-state lithium batteries. However, it cannot suppress the growth of lithium dendrites and then can only tolerate a small critical current density (CCD) before getting short-circuited to death. Learning from that a newly-developed LaCl3-based electrolyte (LTLC) can afford a very large CCD, a three-layer sandwich-structured electrolyte is designed by inserting LTLC inside LPSC. Remarkably, compared with bland LPSC, this hybrid electrolyte LPSC/LTLC/LPSC presents extraordinary performance improvements: the CCD gets increased from 0.51 to 1.52 mA cm-2, the lifetime gets prolonged from 7 h to >500 h at the cycling current of 0.5 mA cm-2 in symmetric cells, and the cyclability gets extended from 10 cycles to >200 cycles at the cycling rate of 0.5 C and 30 °C in Li|electrolyte|NCM721 full cells. The enhancing reasons are assigned to the capability of LTLC to scavenge lithium dendrites, forming a passive layer of Ta, La, and LiCl.

Making the Unfeasible Feasible: Synthesis of the Battery Material Lithium Sulfide via the Metathetic Reaction between Lithium Sulfate and Sodium Sulfide.

Lithium sulfide (Li2S) is a highly desired material for advanced batteries. However, its current industrial production is not suitable for large-scale applications in the long run because the process is carbon-emissive, energy-intensive, and cost-ineffective. This article demonstrates a new method that can overcome these challenges by reacting lithium sulfate (Li2SO4) with sodium sulfide. This approach, which seems unfeasible initially because Li2SO4 is barely soluble in ethanol at room temperature, becomes feasible when heated ethanol and an excess amount of Li2SO4 are used. More interestingly, product purification is easier than that in other metathetic reactions, thanks to the poor solubility of Li2SO4. In order to further minimize the overall costs of producing Li2S, the concomitant byproduct LiNaSO4 and the unfinished precursor Li2SO4 are converted into more valuable materials, Li2CO3 and Na2SO4. Moreover, the homemade Li2S is competitive with the commercial Li2S in cathode performance and gains further enhancement when being composited with the Co9S8 catalyst. Thus, this Li2SO4-based metathesis of Li2S has great potential for practical applications.