Toward High Performance All‐Solid‐State Lithium Batteries with High‐Voltage Cathode Materials: Design Strategies for Solid Electrolytes, Cathode Interfaces, and Composite Electrodes

Abstract

All-solid-state lithium batteries (ASSLBs) with nonflammable solid electrolytes (SEs) deliver greatly enhanced safety characteristics. Furthermore, ASSLBs composed of cathodes with high working voltages, such as LiCoO 2 , LiNi x Co y Mn z O 2 (x + y + z = 1, NCM), LiNi x Co y Al z O 2 (x + y + z = 1, NCA), LiMn x Fe y PO 4 (x + y = 1, LMFP), and LiNi 0.5 Mn 1.5 O 4 (LNMO), and a lithium metal anode can achieve comparable or better performance compared with that of LLBs in terms of energy density. Therefore, high-voltage ASSLBs have been regarded as the most promising next-generation batteries. Although significant progress has been achieved in high-voltage ASSLBs research, their development still faces multiple challenges. To facilitate further effective and target-oriented research on highvoltage ASSLBs, a summary of recent research progress is urgently needed. In this review, recent research progress in high-voltage ASSLBs is summarized from the perspectives of SEs modification, interfacial challenges and their corresponding solutions for cathodes, and high-voltage composite cathode design for practical applications. Finally, the authors' perspectives on the state of current ASSLBs research, aiming to propose possible research directions for the future development of high-voltage ASSLBs.

20 μ m-Thick Li 6.4 La 3 Zr 1.4 Ta 0.6 O 12 -Based Flexible Solid Electrolytes for All-Solid-State Lithium Batteries

“…The lithium transference number t(Li + ), reflecting the situation of lithium ion diffusion in the LLZTO-based film, was calculated to be as high as 0.81 (Figure 2(c)), contributing to homogeneous Li deposition [32]. The wide electrochemical window and high t(Li + ) can be attributed to the introduced high content single-ion conductor LLZTO ceramics [36], possessing excellent oxidative stability [37] and increasing the oxidative decomposition potential of the polymer component by dipole-dipole interactions [38] as well as immobilizing partial TFSIanions through Lewis acid-base interaction [39]. In addition, the time evolution of the impedance spectra of the Li|LLZTO-based film|Li symmetric cell is monitored at room temperature (Figure 2(d)).…”

Multiscale understanding of high-energy cathodes in solid-state batteries: from atomic scale to macroscopic scale

“…Compared with LLIBs (figure 2), the composite cathodes in SSBs faced more challenges, such as the continuous ionic/electronic conductivity networks, the influence of morphology/architecture and crystallographic orientations, etc. In addition, although several insightful reviews have been conducted on the cathode, [35][36][37][38] little attention has been paid to decoupling the intertwined multiscale issues within composite cathodes and summarizing multiscale effective strategies for high-energydensity SSBs.…”

Covalent Organic Framework for Rechargeable Batteries: Mechanisms and Properties of Ionic Conduction

“…In a typical battery system, as shown in Figure 1b, the liquid electrolyte includes protic solvent electrolyte and aprotic solvent electrolyte, while the solid conductors can be divided into electrode material and solid-state electrolyte. [53][54][55][56][57][58][59] Besides, the ionic conduction at the interface is also an important factor affecting the battery performance, mainly including solid electrolyte interphase (SEI), cathode electrolyte interphase (CEI), and electrode/solid-state electrolyte interface. [60][61][62][63][64] In condensed materials, the ionic diffusion can be achieved by the jumps of ions with their neighbors leading to the position exchange.…”