Unveiling low-tortuous effect on electrochemical performance toward ultrathick LiFePO4 electrode with 100 mg cm−2 area loading

Hierarchical Electrode Architecture Enabling Ultrahigh-Capacity LiFePO4 Cathodes with Low Tortuosity

“…For improving the ion diffusion capability in the thick electrode, one of the most straightforward approaches is to increase porosity and decrease tortuosity simultaneously. , Recently, numerous strategies, including laser etching, − three-dimensional (3D) printing, − and the template approach, − have been thoroughly researched to produce thick electrode topologies. Despite the capability to construct regular patterns and optimize ion transport channels through laser etching and 3D printing, these techniques would be prohibitively expensive for use in large-scale industrial manufacturing.…”

Enhancing the Reversibility of Lithium Cobalt Oxide Phase Transition in Thick Electrode via Low Tortuosity Design

“…To the best of our knowledge, LiCoO 2 thick electrodes suffer from extreme concentration polarization and low specific capacity, caused by sluggish lithium-ion transport kinetics. − Furthermore, the inhomogeneous local polarization of LiCoO 2 thick electrode inevitably induces the detrimental phase transition, aggravating the cyclability degradation. − This phenomenon is more severe in high-voltage LiCoO 2 thick electrodes due to excessive local operating potential. The LiCoO 2 particles operating at higher actual voltage exhibit serious irreversible phase transition and poor cyclability. , Thus, enhancing the reversibility of LiCoO 2 phase transition in thick electrode is critical to prolong cyclability.…”

Architected Low‐Tortuosity Electrodes with Tunable Porosity from Nonequilibrium Soft‐Matter Processing

“…Tailoring ratios between D p , t m and h e within low-tortuosity architectures to accommodate for the demanded in-plane supply of ions to the active material at a given current rate will allow for application-specific optimization between energy and power densities in this multidimensional parameter design space. [3,19,20,[24][25][26] Here we report the nonequilibrium soft matter processing technique of hybrid inorganic phase inversion (HIPI) that meets the challenge to fabricate free-standing and low-tortuosity composite electrode architectures. HIPI is a scalable manufacturing strategy that allows for individualized tuning of the most impactful structural features on relevant length scales.…”

“…A variety of electrodes of this type have been fabricated via freeze casting, magnetic templating, laser structuring, and soft‐matter phase separation, demonstrating the viability of low‐tortuosity electrodes to enhance power performance in energy storage devices. [ 2,3,12–23 ] To increase the energy density while maintaining a high power output, computational and experimental results suggest that the diameter of the low‐tortuosity pores and the thickness of the solid matrix with the active charge‐storing material should be in the range of 5–20 µm, smaller than what is obtained from many of the aforementioned fabrication methods. [ 3,24–26 ] Critical in the design of these electrodes is the aspect ratio between the pore diameter ( D p ) and overall thickness of the electrode ( h e ), as well as the material‐to‐pore ratio given by the thickness of the solid matrix ( t m ) and D p , which defines the electrode density and porosity ( Figure A).…”

“…Tailoring ratios between D p , t m and h e within low‐tortuosity architectures to accommodate for the demanded in‐plane supply of ions to the active material at a given current rate will allow for application‐specific optimization between energy and power densities in this multi‐dimensional parameter design space. [ 3,19,20,24–26 ]…”