Dense All‐Electrochem‐Active Electrodes for All‐Solid‐State Lithium Batteries

Abstract

The energy density presents the core competitiveness of lithium (Li)‐ion batteries. In conventional Li‐ion batteries, the utilization of the gravimetric/volumetric energy density at the electrode level is unsatisfactory (<84 wt% and <62 vol%, respectively) due to the existence of non‐electrochemical active parts among the 3D porous electrodes, including electrolytes, binders, and carbon additives. These are regarded as indispensable and irreducible components of the electronic and ionic transport network. Here, a dense “all‐electrochem‐active” (AEA) electrode for all‐solid‐state Li batteries is proposed, which is entirely constructed from a family of superior mixed electronic–ionic‐conducting cathodes, to minimize the energy density gap between the accessible and theoretical energy density at the electrode level. Furthermore, with the ionic–electronic‐conductive network self‐supported from the AEA cathode, the dense hybrid sulfur (S)‐based AEA electrode exhibits a high compacted filling rate of 91.8%, which indicates a high energy density of 777 W h kg−1 and 1945 W h L−1 at the electrode level based on the total cathodes and anodes when at 70 °C.

All-in-One Ionic–Electronic Dual-Carrier Conducting Framework Thickening All-Solid-State Electrode

“…Those problems can be partially resolved by optimizing the multiphase electrode system, but this does not address the root cause of the issue. To overcome this challenge, we proposed a new family of an all-electrochemically active electrode using the intrinsic conductive network inside the electrode to achieve charge transport, thus avoiding the generation of a multiphase interface caused by conductive additives …”

“…Considering that σ eff should meet the required kinetics performance of a real battery cathode, a series of cathodes with different Mo 6 S 8 volume fractions (Φ DCC ) were constructed to measure the corresponding σ eff . Here, an approximate porosity of 10% is considered, and the Φ DCC is approximately 81%, 67%, 54%, 40%, and 27%, denoted as MS/S81, MS/S67, etc.…”

Challenges and Opportunities for Fast Charging of Solid-State Lithium Metal Batteries

“…Creating sufficient ionic and electronic percolating pathways in thick cathodes may demand new cathode chemistries and architectures. For example, one approach is to create thick, dense cathodes that intrinsically possess higher electronic and ionic conductivity; this has been recently demonstrated using a thick electrodeposited LiCoO 2 cathode with no conductive diluents . Electrodeposited cathodes can be grown with preferred crystallographic facets that allow optimized ion transport pathways and charge transfer to enable fast charge, although the limits of the charge/discharging rate need to be determined.…”

“…For example, one approach is to create thick, dense cathodes that intrinsically possess higher electronic and ionic conductivity; this has been recently demonstrated 134 using a thick electrodeposited LiCoO 2 cathode with no conductive diluents. 135 Electrodeposited cathodes can be grown with preferred crystallographic facets that allow optimized ion transport pathways and charge transfer to enable fast charge, although the limits of the charge/discharging rate need to be determined. Another approach 136 is to fabricate 3D templates that provide bi-continuous electronic and ionic pathways, to minimize tortuosity and simultaneously enable high active material loading.…”

N-doped engineering of a high-voltage LiNi0.5Mn1.5O4 cathode with superior cycling capability for wide temperature lithium–ion batteries

“…Lithium–ion batteries (LIBs) have been the dominant energy storage devices in both portable equipment and large scale energy storage fields. 1–8 In recent years, the fast increasing demand for higher energy density Li–ion power packs has promoted the research of high-voltage cathodes. 2,9–14 Among these high-voltage cathode materials, Ni-substituted spinel (LiNi 0.5 Mn 1.5 O 4 ) is attractive due to its 5 V level high-voltage, cost-effectiveness, ease of preparation, and eco-friendliness compared to other conventional cathodes such as LiCoO 2 (4.0 V), LiMn 2 O 4 (4.0 V), and LiFePO 4 (3.4 V).…”