Lithium‐Diffusion Induced Capacity Losses in Lithium‐Based Batteries

Abstract

Rechargeable lithium‐based batteries generally exhibit gradual capacity losses resulting in decreasing energy and power densities. For negative electrode materials, the capacity losses are largely attributed to the formation of a solid electrolyte interphase layer and volume expansion effects. For positive electrode materials, the capacity losses are, instead, mainly ascribed to structural changes and metal ion dissolution. This review focuses on another, so far largely unrecognized, type of capacity loss stemming from diffusion of lithium atoms or ions as a result of concentration gradients present in the electrode. An incomplete delithiation step is then seen for a negative electrode material while an incomplete lithiation step is obtained for a positive electrode material. Evidence for diffusion‐controlled capacity losses is presented based on published experimental data and results obtained in recent studies focusing on this trapping effect. The implications of the diffusion‐controlled Li‐trapping induced capacity losses, which are discussed using a straightforward diffusion‐based model, are compared with those of other phenomena expected to give capacity losses. Approaches that can be used to identify and circumvent the diffusion‐controlled Li‐trapping problem (e.g., regeneration of cycled batteries) are discussed, in addition to remaining challenges and proposed future research directions within this important research area.

Bridging Multiscale Characterization Technologies and Digital Modeling to Evaluate Lithium Battery Full Lifecycle

“…Without enough time or driving force to fully extract lithium ions from the electrode, a portion of lithium ions will be trapped within electrodes, which will accumulate gradually in the following cycles and finally lead to capacity fade. [61] For example, Nyholm and co-workers monitored the capacity and accumulated capacity loss in nanosilicon electrodes. [62] ICP-AES confirmed that the lithium ions can be trapped within electrodes during cycling.…”

Assessing ternary materials for fluoride-ion batteries

“…3 The discrepancy between the theoretical and experimental values of LiCoO2 has been attributed to the incomplete deintercalation of Li from LiCoO2. 26 Although our dataset may encourage researchers to focus on materials with energy densities above those of current LIB technology, we also note that other characteristics can be important. These include ionic and electrical conductivity, chemical compatibility with an electrolyte, electrochemical stability, and material recyclability.…”

Construction of Lithium-Rich Manganese-Based Cathodes Based on Activated Manganese Dioxide for Enhanced Energy Storage Performances

“…2,3 Moreover, the cathode material plays a decisive role in the performance of lithium-ion batteries. 4 Among the available cathode materials, the lithium-rich layered cathode material xLi 2 MnO 3 -(1− x)LiTMO 2 (where TM = Ni, Co, Mn, etc.) has the advantages of high discharge specific capacity, high operating voltage, low cost, and environmental friendliness, compared with the traditional lithium-ion battery cathode materials (lithium iron phosphate cathode material, lithium manganate cathode material, lithium cobaltate cathode material), and is considered to have high potential for application.…”

“…In recent years, people are actively developing devices that utilize renewable energy sources and their efficient energy conversion and storage, in which lithium-ion batteries are rapidly becoming the main form of chemical energy storage with the advantages of high specific energy, good cycling performance, and environmental friendliness. , Moreover, the cathode material plays a decisive role in the performance of lithium-ion batteries . Among the available cathode materials, the lithium-rich layered cathode material x Li 2 MnO 3 -(1– x )­LiTMO 2 (where TM = Ni, Co, Mn, etc.)…”