power and energy densities are the imperative units for these cutting-edge energy harvesting and storage. [3] The state-ofthe-art commercial batteries are prepared with graphite anodes and lithium transition-metal oxide cathodes that reversibly intercalate lithium (Li) ions with moderate stability and energy densities. [4] The intrinsic physicochemical properties and ion insertion mechanisms of conventional materials limits the energy capacity of devices, which will not be quantified for unprecedented demand of modern electronics. [5] Other than the insertiontype electrode materials, there exist some conversion-type electrode materials with higher energy storage capability and faster electrochemical conversion dynamics, including transition-metal dichalcogenide (TMD) and silicon materials. [6] TMD materials demonstrate strong chemical interaction and high catalytic effect with active species in batteries, which is critical to suppress shuttle effects and promote conversion kinetics. [7] But lithiation of TMD materials inevitably gives rise to phase transformation and causes severe damage for the structural integrity of electrodes. [8] Silicon materials emerge as promising conversion-type substitute in recent years due to the high theoretical capacity of 4200 mAh g −1 , but silicon materials exit severe volume expansion effect in conversion processes, which will lead to rapid capacity degradation within several cycles. [9] These two typical conversion-type materials are both semiconductor materials with poor conductivity and unsatisfactory structural stability under electrochemical conditions. Construction of composition architectures with carbon materials is a common strategy to address these drawbacks for purpose of increasing conductivity and maintaining structural integrity. [10] Even if some synthetic methods have been deliberately considered and rationally designed, their attractive theoretical capacities have not fully expressed with long-term cycling performances. Thus, novel battery chemistries other than traditional insertion and conversion-type electrode materials need to be developed to address these issues.With the ever-increasing development of material science and engineering, lots of alternative materials with high energy capacities and stabilities have stood out as the electrode materials from the competition with conventional counterparts. For instance, sulfur material-based batteries gives high theoretical Advanced battery systems with high energy density have attracted enormous research enthusiasm with potential for portable electronics, electrical vehicles, and grid-scale systems. To enhance the performance of conversiontype batteries, various catalytic materials are developed, including metals and transition-metal dichalcogenides (TMDs). Metals are highly conductive with catalytic effects, but bulk structures with low surface area result in low atom utilization, and high chemical reactivity induces unfavorable dendrite effects. TMDs present chemical adsorption with active species and ...

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The increasing demand for safe and dense energy storage has shifted research focus from liquid electrolyte-based Li-ion batteries toward solid-state batteries (SSBs). However, the application of SSBs is impeded by uncontrollable Li dendrite growth and short circuiting, the mechanism of which remains elusive. Herein, we conceptualize a scheme to visualize Li deposition in the confined space inside carbon nanotubes (CNTs) to mimic Li deposition dynamics inside solid electrolyte (SE) cracks, where the high-strength CNT walls mimic the mechanically strong SEs. We observed that the deposited Li propagates as a creeping solid in the CNTs, presenting an effective pathway for stress relaxation. When the stress-relaxation pathway is blocked, the Li deposition-induced stress reaches the gigapascal level and causes CNT fracture. Mechanics analysis suggests that interfacial lithiophilicity critically governs Li deposition dynamics and stress relaxation. Our study offers critical strategies for suppressing Li dendritic growth and constructing high-energy-density, electrochemically and mechanically robust SSBs.

Atomic scale imaging revealed that the deposition/stripping of Na from the β′′-Al2O3 solid electrolyte causes delamination cracks and the closure of the conduction planes.