In this work, we systematically study four different types of cell configuration, including Li/Li symmetric cells 33, Li/Cu cells, cathode/Li cells, and cathode/Cu anode-free cells, as an integrated protocol to unfold the intrinsic reasons and contributions of individual irr-CEs from not only Li anodes in Li/Cu cells, but also the cathodes in cathode/Li half-cells. Thus, there is still a lack of holistic methodology to identify and quantify the irr-CEs in LMBs and AFLMBs. However, the important information of the irr-CE or capacity loss from the cathode and cross-talk effects in cathode/Li or anode-free cathode/Cu cells could not be extracted from the TGC method. They comprehensively discussed the formation of inactive Li and determined the origin of irr-CE of Li anodes within Li/Cu cells by decoupling the dead Li and SEI formation, which provides strategies for more-efficient Li plating and stripping on Cu substrate. ![]() 32 demonstrated an analytical method of titration gas chromatography (TGC) to quantify the contribution of dead Li to the total irr-CE in Li/Cu cells, identifying dead Li as the major reason accounted for the capacity loss of Li/Cu cells. One efficient way is to study the irreversible coulombic efficiency (irr-CE), which may represent the side reactions and sources of capacity loss in the battery. More importantly, integrating all the unraveled phenomena and messages to have a better overall evaluation of the battery systems is essential. To systematically evaluate the electrochemical performance of both LMBs and AFLMBs, and unfold all the messages hidden within the battery, one has to comprehensively examine the information from all the possible perspectives. ![]() However, in most of the published works, the electrochemical performance of LMBs/AFLMBs is often discussed by comparing capacity retention, reversible capacity, or rate capability, which easily overlooks or even misunderstands the information that is concealed by the meretricious results when adopting only one or two points of view. Recently, anode-free lithium metal batteries (AFLMBs) are considered as phenomenal energy-storage systems owing to higher energy density than that of LMB, which with excess Li in the system, and greatly reduced safety risks since no Li metal is used during cell manufacturing, which remarkably increases the simplicity of cell fabrication and reduces the cost of cell assembly, too 26, 27, 28, 29, 30, 31. Meanwhile, several key factors would still affect the cycling performance of LMB and are crucial in achieving high specific energy of 500 Wh kg −1 demanded by electric vehicle energy-storage market such as electrolyte amount 21, temperature 22, pressure 23, amount of Li or cahode 24, 25, and current density applied 9, etc. Many works have also been done by using different electrolyte formulas 18, 3D architecture Li 19, and artificial coating layers 20 to study their effect on increasing the electrochemical performance of LMB. ![]() To overcome the aforementioned challenges, one has to systematically study Li metal stability/protection 12, SEI formation mechanism 13, 14, and suppression of Li dendrite growth in LMB 15, 16, 17. More specifically, the safety issues induced by Li dendrite growth and internal short circuit (ISC) 3, poor efficiency attributed to the formation of high surface area lithium (HSAL, dendrite) and dead Li 4, 5, and severe electrolyte decomposition at the negative electrode leading to electrolyte dry-up and the formation of thick solid electrolyte interphase (SEI) that increases the internal resistance and consumes the electrolytes 6, 7, 8, 9, 10, 11. However, lithium metal batteries (LMB) still suffer from several barriers and yet to be commercialized. standard hydrogen electrode), has already been extensively investigated over the four decades 1, 2. Lithium metal, with an ultrahigh theoretical specific capacity (3860 mAh g −1) and low redox potential (−3.040 V vs.
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