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Abstract Intercalation has become a powerful approach to tune the intrinsic properties and introduce novel phenomena in layered materials. Intercalating van der Waals (vdW) magnetic materials is a promising route to engineer the low-dimensional magnetism. Recently, metal thiophosphates,MPX₃, has been widely studied because their magnetic orders are highly tunable and persist down to the two-dimensional limit. In this work, we used electrochemical technique to intercalate Li into NiPS₃single crystals and found the emergence of ferrimagnetism at low temperature in Li-intercalated NiPS₃. Such tuning of magnetic properties highlights the effectiveness of intercalation, providing a novel strategy to manipulate the magnetism in vdW magnets. 

Li dendrite formed in Li metal batteries can be categorized into two different types. One is the detrimental Li dendrite that heads towards the separator with a potential to short cell. The other is the ill-defined fibrous Li formed within bulk Li metal. The detrimental Li dendrite may cause cell short, while the other dendrites, covered by SEI, mainly increase cell impedance and terminate the cell operation, most often, before any “short” really happens. Without decoupling these two different Li dendrites, it is hard to develop any effective approach to realize both stable and safe Li metal batteries. Herein, a straightforward approach is proposed to induce the growth of detrimental dendritic Li so the cells are “shorted” frequently and consistently. Based on this new protocol, various electrolytes are revisited and the SEI derived are compared and quantified, providing new insights for addressing the challenges in rechargeable Li metal battery technologies. 

Lithium (Li) metal anodes have regained intensive interest in recent years due to the ever-increasing demand for next-generation high energy battery technologies. Li metal, unfortunately, suffers from poor cycling stability and low efficiency as well as from the formation of dangerous Li dendrites, raising safety concerns. Utilizing solid-state electrolytes (SSEs) to prevent Li dendrite growth provides a promising approach to tackle the challenge. However, recent studies indicate that Li dendrites easily form at high current densities, which calls for full investigation of the fundamental mechanisms of Li dendrite formation within SSEs. Herein, the origin and evolution of Li dendrite growth through SSEs have been studied and compared by using Li 6.1 Ga 0.3 La 3 Zr 2 O 12 (LLZO) and NASICON-type Li 2 O–Al 2 O 3 –P 2 O 5 –TiO 2 –GeO 2 (LATP) pellets as the separators. We discover that a solid electrolyte interphase (SEI)-like interfacial layer between Li and SSE plays a critical role in alleviating the growth of dendritic Li, providing new insights into the interface between SSE and Li metal to enable future all solid-state batteries.