Pre‐Lithiation Strategies for Next‐Generation Practical Lithium‐Ion Batteries

Abstract

Next‐generation Li‐ion batteries (LIBs) with higher energy density adopt some novel anode materials, which generally have the potential to exhibit higher capacity, superior rate performance as well as better cycling durability than conventional graphite anode, while on the other hand always suffer from larger active lithium loss (ALL) in the first several cycles. During the last two decades, various pre‐lithiation strategies are developed to mitigate the initial ALL by presetting the extra Li sources to effectively improve the first Coulombic efficiency and thus achieve higher energy density as well as better cyclability. In this progress report, the origin of the huge initial ALL of the anode and its effect on the performance of full cells are first illustrated in theory. Then, various pre‐lithiation strategies to resolve these issues are summarized, classified, and compared in detail. Moreover, the research progress of pre‐lithiation strategies for the representative electrochemical systems are carefully reviewed. Finally, the current challenges and future perspectives are particularly analyzed and outlooked. This progress report aims to bring up new insights to reassess the significance of pre‐lithiation strategies and offer a guideline for the research directions tailored for different applications based on the proposed pre‐lithiation strategies summaries and comparisons.

Investigating the energy storage performance of the ZnMn 2 O 4 anode for its potential application in lithium‐ion batteries

“…A typical disadvantage of these high-capacity metal oxide-based anode materials, when applied practically, is their relatively low initial CE, which can be mitigated by the pre-lithiation strategy. 45 The ZMO-BM electrode also demonstrated an outstanding rate capability apart from the high capacity and good cycling. Figure 3D shows the rate capability of the ZMO-BM electrode.…”

3D Correlative Imaging of Lithium Ion Concentration in a Vertically Oriented Electrode Microstructure with a Density Gradient

“…[7,8] Theoretical studies have attributed battery capacity loss to a Li + ion concentration gradient in the electrodes with a higher concentration near the separator but a lower concentration near the current collector which in turn increases the overpotential and polarization of the cell, [9][10][11][12] but the relationship between Li + chemical stoichiometry distribution and electrode microstructural properties is less understood. [13][14][15] Most battery electrodes are made by a highly productive slurry casting (SC) method which makes electrodes of 150-200 μm thickness and 20-30 vol% porosity, [16] containing a random porous microstructure with highly tortuous pores that restrict Li + ion diffusion through the electrode thickness, [17,18] which in turn causes the steep Li + ion concentration gradient in the electrodes [19,20] and reduces the accessibility of electrode active material and battery capacity. [21] Thick electrodes (≥300 μm) can reduce the proportion of inactive components (current collectors and separators) in a battery cell-stack and increase the proportion of active components (electrodes) that contributes to energy storage, [22] but thick electrodes with the conventional tortuous porous microstructure would amplify the problem of restricted Li + ion diffusion and lead to under-utilization of active materials and loss of battery capacity even with an extremely small current.…”

Stable and Reversible Lithium Storage Properties of LiTiOx Nanotubes for Electrochemical Recovery from Aqueous Solutions

“…In this case, the metal substrate work as current collector and the highly ordered structure of the NTs ensures a one‐dimensional electronic and ionic conductivity [36] . Pre‐lithiation is a well‐known strategy in the battery world to improve the electrochemical energy storage as is the use of spinels [37–41] . Similarly, lithiated titanium oxide structures have recently been investigated to recover lithium from aqueous solutions as an alternative to lithium manganese oxide adsorbents due to their better stability in acidic solutions [42–46] …”

“…[36] Pre-lithiation is a well-known strategy in the battery world to improve the electrochemical energy storage as is the use of spinels. [37][38][39][40][41] Similarly, lithiated titanium oxide structures have recently been investigated to recover lithium from aqueous solutions as an alternative to lithium manganese oxide adsorbents due to their better stability in acidic solutions. [42][43][44][45][46] To the best of the authors' knowledge, this is the first systematic study on the stable and reversible lithium storage properties from ordered hydrothermally lithiated nanotubes obtained by anodic oxidation.…”