Guan Mingzhu, Wei Zengwu, Liu Rui, Yan Xufeng, Sun Shanshan, Zhou Mingjiong, Papović Snežana, Zheng Kun, Mandić Zoran, Xin Xing
School of Materials Science and Chemical Engineering, Ningbo University, Ningbo, 315211, P. R. China.
Ningbo Ronbay New Energy Technology Co., Ltd., Ningbo, 315400, P. R. China.
Small Methods. 2025 Jul 2:e2500923. doi: 10.1002/smtd.202500923.
Driven by the demand for high-energy-density storage, Lithium metal batteries (LMBs) and anode-free Lithium metal batteries (AFLMBs) have attracted significant attention due to their high theoretical capacity and low reduction potential. However, achieving reproducible Coulombic Efficiency (CE) measurements remains a challenge due to inconsistencies in electrochemical protocols and experimental conditions. This study systematically evaluates and compares three CE measurement methodologies, identifying key factors that influence reproducibility and accuracy. Unlike previous studies, which often report CE values without considering their methodological limitations, the impact of electrolyte composition, electrolyte concentration, and electrode surface properties are highlighted on CE variations. Furthermore, this study demonstrates that a pre-cycling Li reservoir method effectively minimizes substrate effects, leading to the most sensitive measurements across various testing conditions. This work provides a standardized framework for CE evaluation in LMBs and AFLMBs, offering valuable insights for optimizing Li-free anode interfaces and accelerating the commercialization of high-performance LMBs.
受高能量密度存储需求的驱动，锂金属电池（LMBs）和无阳极锂金属电池（AFLMBs）因其高理论容量和低还原电位而备受关注。然而，由于电化学协议和实验条件的不一致，实现可重复的库仑效率（CE）测量仍然是一个挑战。本研究系统地评估和比较了三种CE测量方法，确定了影响重现性和准确性的关键因素。与以往研究不同，以往研究常常在不考虑方法局限性的情况下报告CE值，本研究强调了电解质组成、电解质浓度和电极表面性质对CE变化的影响。此外，本研究表明，预循环锂储存器方法有效地最小化了基底效应，从而在各种测试条件下实现了最灵敏的测量。这项工作为LMBs和AFLMBs中的CE评估提供了一个标准化框架，为优化无锂阳极界面和加速高性能LMBs的商业化提供了有价值的见解。
