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Surface Coupling between Mechanical and Electric Fields Empowering Ni-Rich Cathodes with Superior Cyclabilities for Lithium-Ion Batteries.

ABSTRACT: Ni-rich cathodes with high energy densities are considered as promising candidates for advanced lithium-ion batteries, whereas their commercial application is in dilemma due to dramatic capacity decay and poor structure stability stemmed from interfacial instability, structural degradation, and stress-strain accumulation, as well as intergranular cracks. Herein, a piezoelectric LiTaO₃ (LTO) layer is facilely deposited onto Li[Ni_x Co_y Mn_1- _x _- _y ]O₂ (x = 0.6, 0.8) cathodes to induce surface polarized electric fields via the intrinsic stress-strain of Ni-rich active materials, thus modulating interfacial Li⁺ kinetics upon cycling. Various characterizations indicate that the electrochemical performances of LTO-modified cathodes are obviously enhanced even under large current density and elevated temperature. Intensive explorations from in situ X-ray diffraction technique, finite element analysis, and first-principle calculation manifest that the improvement mechanism of LTO decoration can be attributed to the enhanced structural stability of bulk material, suppressed stress accumulation, and regulated ion transportation. These findings provide deep insight into surface coupling strategy between mechanical and electric fields to regulate the interfacial Li⁺ kinetics behavior and enhance structure stability for Ni-rich cathodes, which will also arouse great interest from scientists and engineers in multifunctional surface engineering for electrochemical systems.

SUBMITTER: Dai Z

PROVIDER: S-EPMC9218785 | biostudies-literature |

REPOSITORIES: biostudies-literature

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Project description:Sulfide electrolyte all-solid-state lithium-ion batteries (ASSLBs) that have inherently nonflammable properties have improved greatly over the past decade. However, determining both the stable and functional electrode components to pair with these solid electrolytes requires significant investigation. Solid electrolyte comprises 20-40% of the composite cathode electrode, which improves the ionic conductivity. However, this results in thick electrolyte that blocks the electron pathways in the electrode, significantly lowering the electrochemical performance. The application of conductive carbon material is required to overcome this issue, and, hence, determining the carbon properties that result in the most stable performance in the sulfide solid electrolyte is vital. This study analyzes the effect of the cathode conductive additive's morphology on the electrochemical performance of sulfide electrolyte-based ASSLBs. Carbon black (CB) and carbon nanotubes (CNTs), which provide electron pathways at the nanoscale and sub-micron scale, and carbon nanofiber (CNF), which provides electron pathways at the tens-of-microns scale, are all tested individually as potential conductive additives. When the CNF, with its high crystallinity, is used as a conductive material, the electrochemical performance shows an excellent initial discharge capacity of 191.78 mAh/g and a 50-cycle capacity retention of 83.9%. Conversely, the CB and the CNTs, with their shorter pathways and significantly increased surface area, show a relatively low electrochemical performance. By using the CNF to provide excellent electrical conductivity to the electrode, the polarization is suppressed. Furthermore, the interfacial impedance across the charge transfer region is also reduced over 50 cycles compared with the CB and CNT composite cells. These findings stringently analyze and emphasize the importance of the morphology of the carbon conductive additives in the ASSLB cathode electrodes, with improvements in the electrochemical performance being realized through the application of long-form two-dimensional crystalline CNFs.

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Surface Coupling between Mechanical and Electric Fields Empowering Ni-Rich Cathodes with Superior Cyclabilities for Lithium-Ion Batteries.

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