A Functional Electrolyte Containing P-Phenyl Diisothiocyanate (PDITC) Additive Achieves the Interphase Stability of High Nickel Cathode in a Wide Temperature Range.

The lithium-ion batteries (LIBs) with high nickel cathode have high specific energy, but as the nickel content in the cathode active material increases, batteries are suffering from temperature limitations, unstable performance, and transition metal dissolution during long cycling. In this work, a functional electrolyte with P-phenyl diisothiocyanate (PDITC) additive is developed to stabilize the performance of LiNi0.8 Co0.1 Mn0.1 O2 (NCM811)/graphite LIBs over a wide temperature range. Compared to the batteries without the additive, the capacity retention of the batteries with PDITC-containing electrolyte increases from 23 % to 74 % after 1400 cycles at 25 °C, and from 15 % to 85 % after 300 cycles at 45 °C. After being stored at 60 °C, the capacity retention rate and capacity recovery rate of the battery are also improved. In addition, the PDITC-containing battery has a higher discharge capacity at -20 °C, and the capacity retention rate increases from 79 % to 90 % after 500 cycles at 0 °C. Both theoretical calculations and spectroscopic results demonstrate that PDITC is involved in constructing a dense interphase, inhibiting the decomposition of the electrolyte and reducing the interfacial impedance. The application of PDITC provides a new strategy to improve the wide-temperature performance of the NCM811/graphite LIBs.

Air- and Moisture Robust Surface Modification for Ni-Rich Layered Cathode Materials for Li-Ion Batteries.

The mainstream of high-energy cathode development is focused on increasing the Ni-ratio in layered structured cathode materials. The increment of the Ni portion in the layered cathode material escalates not only the deliverable capacity but also the structural degradation. High-Ni layered cathodes are highly vulnerable to exposure to air that contains CO2 and H2 O, forming problematic residual lithium compounds at the surface. In this work, a novel air- and moisture robust surface modification is reported for LiNi0.8 Co0.1 Mn0.1 O2 (NCM811) via the sol-gel coating method that selectively coats the internal surface area of the polycrystalline morphology secondary particles. Bare-, Li2 SnO3 -coated and LiCoO2 -coated NCM811 are exposed to different ambient environments (air, hot-air, and moisture-air) to systematically investigate the correlation between the internal/external coating morphology and performance degradations. The LiCoO2 -coated NCM811s exhibit high-capacity retention after exposure to all environments, due to the internal surface coating that prevents the penetration of harmful compounds into the polycrystalline NCM811. On the other hand, the Li2 SnO3 -coated NCM811s exposed to the ambient environments show gradual capacity fading, implying the occurrence of internal degradation. This paper highlights the impact of the internal degradation of polycrystalline NCM811 after environmental exposure and the correct coating mechanisms required to successfully prevent it.

Interfacial Reviving of the Degraded LiNi0.8 Co0.1 Mn0.1 O2 Cathode by LiPO3 Repair Strategy.

Nickel-rich cathode materials, owing to their high energy density and low cost, are considered to be one of the cathodes with the most potential in next-generation lithium-ion batteries. Unfortunately, this kind of cathode with highly active surface is easy to react with H2 O and CO2 when exposed to ambient air, resulting in the formation of lithium impurities and interfacial phase transition as well as deterioration of the electrochemical properties. In this work, the evolution mechanism of the structure and interface of LiNi0.8 Co0.1 Mn0.1 O2 during air-exposure is systematically investigated. Furthermore, a facile reviving strategy is proposed to restore the degraded LiNi0.8 Co0.1 Mn0.1 O2 by using LiPO3 as the repair agent. The lithium impurities on the surface of the degraded sample can transform into the repair/coating layer, and part of the rock salt phase on the subsurface can revive to layered phase after repair heat treatment. As a result, the optimized cathode delivers an initial discharge capacity of 198.3 mAh g-1 at 0.1C and a capacity retention of 85.5% after 50 cycles. Although slightly lower than the bare sample (201 mAh g-1 and 88%), they are obviously higher than the exposed samples (166.5 mAh g-1 and 40.4%). The regenerated electrochemical properties should be attributed to the multifunctional repair layer that can efficiently reduce the surface lithium impurities, prevent the corrosion of electrolyte, and improve the interfacial Li+ diffusion kinetics. This work can effectively reduce the waste of the degraded Ni-rich ternary materials and realize the transformation of "waste" into wealth.

Self-Reconstruction of Highly Degraded LiNi0.8 Co0.1 Mn0.1 O2 toward Stable Single-Crystalline Cathode.

The ever-growing demand for resources sustainability has promoted the recycle of spent lithium-ion batteries to a strategic position. Direct recycle outperforms either hydrometallurgical or pyrometallurgical approaches due to the high added value and facile treatment processes. However, the traditional direct recycling technologies are only applicable for Ni-poor/middle cathodes. Herein, spent Ni-rich LiNi0.8 Co0.1 Mn0.1 O2 (S-NCM) to performance-enhanced single-crystalline cathode materials is directly recycled using a simple but effective LiOH-NaCl molten salt. The evolution process of the Li-supplement and grain-recrystallization during regeneration is systematically investigated, and the successful recovery of the highly degraded microstructure is comprehensively proven, including significant elimination of Ni2+ and O vacancies. Beneficial from the favorable reconstructed single-crystalline particles, the regenerated NCM (R-NCM) represents remarkably enhanced structural stability, electrochemical activity, O2 and cracks suppression during charge/discharge, thus achieving the excellent performances in long-term cycling and high-rate tests. As a result, R-NCM maintains the 86.5% reversible capacity at 1 C after 200 cycles. Instructively, the present molten salt can be successfully applied for recycling spent NCMs with various Li and Ni compositions (e.g., LiNi0.5 Co0.2 Mn0.3 O2 ).

Improving the Rechargeable Li-CO2 Battery Performances by Tailoring Oxygen Defects on Li-Ni-Co-Mn Multi-Metal Oxide Catalysts Recycled from Spent Ternary Lithium-Ion Batteries.

Rechargeable Li-CO2 batteries are considered as a promising carbon-neutral energy storage technology owing to their ultra-high energy density and efficient CO2 capture capability. However, the sluggish CO2 reduction/evolution kinetics impedes their practical application, which leads to huge overpotentials and poor cyclability. Multi-element transit metal oxides (TMOs) are demonstrated as effective cathodic catalysts for Li-CO2 batteries. But there are no reports on the integration of defect engineering on multi-element TMOs. Herein, the oxygen vacancy-bearing Li-Ni-Co-Mn multi-oxide (Re-NCM-H3) catalyst with the α-NaFeO2-type structure is first fabricated by annealing the NiCoMn precursor that derived from spent ternary LiNi0.8Co0.1Mn0.1O2 cathode, in H2 at 300 °C. As demonstrated by experimental results and theory calculations, the introduction of moderate oxygen vacancy has optimized electronic state near the Fermi level (Ef), eventually improving CO2 adsorption and charge transfer. Therefore, the Li-CO2 batteries with Re-NCM-H3 catalyst deliver a high capacity (11808.9 mAh g-1), a lower overpotential (1.54 V), as well as excellent stability over 216 cycles at 100 mA g-1 and 165 cycles at 400 mA g-1. This study not only opens up a sustainable application of spent ternary cathode, but also validates the potential of multi-element TMO catalysts with oxygen defects for high-efficiency Li-CO2 batteries.

Invoking Interfacial Engineering Boosts Structural Stability Empowering Exceptional Cyclability of Ni-Rich Cathode.

The cycling stability of LiNi0.8Co0.1Mn0.1O2 under high voltages is hindered by the occurrence of hybrid anion- and cation-redox processes, leading to oxygen escape and uncontrolled phase collapse. In this study, an interfacial engineering strategy involving a straightforward mechanical ball milling and low-temperature calcination, employing a Se-doped and FeSe2&Fe2O3-modified approach is proposed to design a stable Ni-rich cathode. Se2- are selectively adsorbed within oxygen vacancies to form O─TM─Se bond, effectively stabilizing lattice oxygen, and preventing structural distortion. Simultaneously, the Se-NCM811//FeSe2//Fe2O3 self-assembled electric field is activated, improving interfacial charge transfer and coupling. Furthermore, FeSe2 accelerates Li+ diffusion and reacts with oxygen to form Fe2O3 and SeO2. The Fe2O3 coating mitigates hydrofluoric acid erosion and acts as an electrostatic shield layer, limiting the outward migration of oxygen anions. Impressively, the modified materials exhibit significantly improved electrochemical performance, with a capacity retention of 79.7% after 500 cycles at 1C under 4.5 V. Furthermore, it provides an extraordinary capacity retention of 94.6% in 3-4.25 V after 550 cycles in pouch-type full battery. This dual-modification approach demonstrates its feasibility and opens new perspective for the development of stable lithium-ion batteries operating at high voltages.

Borate-Functionalized Disiloxane as Effective Electrolyte Additive for 4.5 V LiNi0.8Co0.1Mn0.1O2/Graphite Batteries.

Ni-rich LiNi0.8Co0.1Mn0.1O2 (NCM811) is considered the most prominent cathode material to establish a practical high energy density of lithium-ion batteries (LIBs) for future electric vehicles. The energy density of LIBs is greatly determined by the capacity of electrode materials and the operating voltage of the cells. To further improve the cycle lifespan of NCM811 batteries to meet the requirement of driving range for the electric vehicle market, it is vital to design a novel electrolyte additive that can enhance the stability of the cathode/electrolyte interface at a wide range of voltage. Herein, a novel borate functionalized disiloxane compound, 1,1,1,3,3-pentamethyl-3-(3-(4,4,5,5-tetramethyl-1,3,2-dioxaborolan-2-yl)propyl) disiloxane (PMBPDS), is synthesized as cathode electrolyte interphase (CEI) film-forming additive to improve the cycling performance of NCM811 batteries. Systematic studies reveal that PMBPDS can construct a stable CEI film on the NCM811 surface and efficiently scavenge hydrofluoric acid (HF). The PMBPDS-derived CEI prevents the dissolution of transmission metals in the NCM811 cathode and enhances the capacity retention of NCM811/graphite cells from 68.3 to 70.6% after 200 cycles at 1 C in the voltage window of 3-4.5 V. This work provides more understanding on designing the molecular structure of additive compounds for improving the electrochemical performance of LIBs.

Dual Modification for Low-Strain Ni-Rich Cathodes Toward Superior Cyclability in Pouch Full Cells.

Rapid capacity fading, interfacial instability, and thermal runaway due to oxygen loss are critical obstacles hindering the practical application and commercialization of Ni-rich cathodes (LiNi0.8Co0.1Mn0.1O2, NCM811). Herein, a Sn4+/F- codoping and LiF-coated Ni-rich cathode, denoted as NCM811-SF, is structurally fabricated that demonstrates very high cyclic and thermal stabilities. The introduction of Sn4+ regulates the local electronic structure and facilitates the conversion of the layered structure into a spinel phase; F- captures lithium impurities to form LiF coatings and forms TM-F bonds to reduce Ni/Li disordering. The compositionally complex codoping strategy reduces the internal structure strain, inhibits the Li+/Ni2+ intermixing during cycling and degradation of the nanoscale structure, and further improves the thermal stability and the crystal structure. The cathodic electrode showed a little volume shift at 2.8-4.5 V, which significantly decreased lattice flaws and fractures generated by local strain, based on detailed analyses performed using COMSOL simulations, X-ray diffraction, and scanning transmission electron microscopy. Benefiting from this, after 300 cycles, our as-prepared NCM811-SF cathode maintains 85.4% of its initial capacity at 4.5 V and has an excellent reversible capacity equal to 169 mAh·g-1 at 1 C. In addition, the NCM811-SF/graphite cell in a pouch-type complete cell retained 94.8% of its starting capacity following 500 cycles. These findings underscore the effectiveness of introducing the Sn-O and TM-F bonds in improving the durability and electrochemical efficiency of the cathode material, which makes it a good choice for high-efficiency Li-ion batteries.

Enhancing the Electrochemical Stability of LiNi0.8Co0.1Mn0.1O2 Compounds for Lithium-Ion Batteries via Tailoring Precursors Synthesis Temperatures.

LiNi0.8Co0.1Mn0.1O2 (LNCMO) cathode materials for lithium-ion batteries (LIBs) were prepared by the hydrothermal synthesis of precursors and high-temperature calcination. The effect of precursor hydrothermal synthesis temperature on the microstructures and electrochemical cycling performances of the Ni-rich LNCMO cathode materials were investigated by SEM, XRD, XPS and electrochemical tests. The results showed that the cathode material prepared using the precursor synthesized at a hydrothermal temperature of 220 °C exhibited the best charge/discharge cycle stability, whose specific capacity retention rate reached 81.94% after 50 cycles. Such enhanced cyclic stability of LNCMO was directly related to the small grain size, high crystallinity and structural stability inherited from the precursor obtained at 220 °C.

Phosphate and Borate-Based Composite Interface of Single-Crystal LiNi0.8Co0.1Mn0.1O2 Enables Excellent Electrochemical Stability at High Operation Voltage.

The application of nickel-rich cathodes in lithium-ion batteries has been hampered by its rapid capacity/voltage fading and limited performance of rate. In this work, a passivation technique is used to create a stable composite interface on single-crystal LiNi0.8Co0.1Mn0.1O2 (NCM811) surface, which greatly improves the cycle life-span and high-voltage constancy of cathode with 4.5 and 4.6 V cut-off voltage. The improved Li+ conductivity of the interface enables a firm cathode-electrolyte interphase (CEI), which reduces interfacial side reactions, lowers the risk of safety hazards, and improves irreversible phase transitions. As a result, the electrochemical performance of single-crystal Ni-rich cathode are remarkably enhanced. The specific capacity of 152 mAh g-1 can be delivered at a charging/discharging rate of 5 C under 4.5 V cut-off voltage, much higher than 115 mAh g-1 of the pristine NCM811. After 200 cycles at 1 C, the composite interface modified NCM811 demonstrates outstanding capacity retention of 85.4% and 83.8% at 4.5 V and 4.6 V cut-off voltage, respectively.

Slurry-Coated LiNi0.8Co0.1Mn0.1O2-Li3InCl6 Composite Cathode with Enhanced Interfacial Stability for Sulfide-Based All-Solid-State Batteries.

The implementation of all-solid-state lithium batteries (ASSLBs) is regarded as an important step toward the next-generation energy storage systems. The sulfide solid-state electrolyte (SSE) is a promising candidate for ASSLBs due to its high ionic conductivity and easy processability. However, the interface stability of sulfide SSEs toward high-capacity cathodes like nickel-rich layered cathodes is limited by the interfacial side reaction and narrow electrochemical window of the electrolyte. Herein, we propose introducing the halide SSE Li3InCl6 (LIC) with high (electro)chemical stability and superior Li+ conductivity to act as an ionic conductive additive in the Ni-rich LiNi0.8Co0.1Mn0.1O2 (NCM) cathode mixture through a slurry coating, aiming to build a stable cathode-electrolyte interface. This work demonstrates that the sulfide SSE Li5.5PS4.5Cl1.5 (LPSCl) is chemically incompatible with the NCM cathode, and the indispensable role of the substitution of LPSCl with LIC in enhancing the interfacial compatibility and oxidation stability of the electrolyte is highlighted. Accordingly, this new configuration shows superior electrochemical performance at room temperature. It shows a high initial discharge capacity (136.3 mA h g-1 at 0.1C), cycling performance (77.4% capacity retention at the 100th cycle), and rate capability (79.3 mA h g-1 at 0.5C). This work paves the way for investigating interfacial challenges regarding high-voltage cathodes and provides new insights into possible interface engineering strategies.

Improving Fast Charging-Discharging Performances of Ni-Rich LiNi0.8Co0.1Mn0.1O2 Cathode Material by Electronic Conductor LaNiO3 Crystallites.

Fast charging-discharging is one of the important requirements for next-generation high-energy Li-ion batteries, nevertheless, electrons transport in the active oxide materials is limited. Thus, carbon coating of active materials is a common method to supply the routes for electron transport, but it is difficult to synthesize the oxide-carbon composite for LiNiO2-based materials which need to be calcined in an oxygen-rich atmosphere. In this work, LiNi0.8Co0.1Mn0.1O2 (NCM811) coated with electronic conductor LaNiO3 (LNO) crystallites is demonstrated for the first time as fast charging-discharging and high energy cathodes for Li-ion batteries. The LaNiO3 succeeds in providing an exceptional fast charging-discharging behavior and initial coulombic efficiency in comparison with pristine NCM811. Consequently, the NCM811@3LNO electrode presents a higher capacity at 0.1 C (approximately 246 mAh g-1) and a significantly improved high rate performance (a discharge specific capacity of 130.62 mAh g-1 at 10 C), twice that of pristine NCM811. Additionally, cycling stability is also improved for the composite material. This work provides a new possibility of active oxide cathodes for high energy/power Li-ion batteries by electronic conductor LaNiO3 coating.

Achieving a Highly Stable Electrode/Electrolyte Interface for a Nickel-Rich Cathode via an Additive-Containing Gel Polymer Electrolyte.

The nickel-rich cathode LiNi0.8Co0.1Mn0.1O2 (NCM811) is deemed as a prospective material for high-voltage lithium-ion batteries (LIBs) owing to its merits of high discharge capacity and low cobalt content. However, the unsatisfactory cyclic stability and thermostability that originate from the unstable electrode/electrolyte interface restrict its commercial application. Herein, a novel electrolyte composed of a polyethylene (PE) supported poly(vinylidene fluoride-co-hexafluoropropylene) (P(VdF-HFP)) based gel polymer electrolyte (GPE) strengthened by a film-forming additive of 3-(trimethylsilyl)phenylboronic acid (TMSPB) is proposed. The porous structure and good oxidative stability of the P(VdF-HFP)/PE membrane help to expand the oxidative potential of GPE to 5.5 V compared with 5.1 V for the liquid electrolyte. The developed GPE also has better thermal stability, contributing to improving the safety performance of LIBs. Furthermore, the TMSPB additive constructs a low-impedance and stable cathode electrolyte interphase (CEI) on the NCM811 cathode surface, compensating for GPE's drawbacks of sluggish kinetics. Consequently, the NCM811 cathode matched with 3% TMSPB-containing GPE exhibits remarkable cyclicity and rate capability, maintaining 94% of its initial capacity after 100 cycles at a high voltage range of 3.0-4.35 V and delivering a capacity of 133.5 mAh g-1 under 15 C high current rate compared with 68% and 75.8 mAh g-1 for the one with an additive-free liquid electrolyte. By virtue of the enhanced stability of the NCM811cathode, the cyclability of graphite||NCM811 full cell also increases from 48 to 81% after 100 cycles. The incorporation of P(VdF-HFP)-based GPE and TMSPB electrolyte additive points out a viable and convenient pathway to unlock the properties of high energy density and satisfactory safety for next-generation LIBs.

A Three in One Strategy to Achieve Zirconium Doping, Boron Doping, and Interfacial Coating for Stable LiNi0.8Co0.1Mn0.1O2 Cathode.

LiNi0.8Co0.1Mn0.1O2 cathodes suffer from severe bulk structural and interfacial degradation during battery operation. To address these issues, a three in one strategy using ZrB2 as the dopant is proposed for constructing a stable Ni-rich cathode. In this strategy, Zr and B are doped into the bulk of LiNi0.8Co0.1Mn0.1O2, respectively, which is beneficial to stabilize the crystal structure and mitigate the microcracks. Meanwhile, during the high-temperature calcination, some of the remaining Zr at the surface combined with the surface lithium source to form lithium zirconium coatings, which physically protect the surface and suppress the interfacial phase transition upon cycling. Thus, the 0.2 mol% ZrB2-LiNi0.8Co0.1Mn0.1O2 cathode delivers a discharge capacity of 183.1 mAh g-1 after 100 cycles at 50 °C (1C, 3.0-4.3 V), with an outstanding capacity retention of 88.1%. The cycling stability improvement is more obvious when the cut-off voltage increased to 4.4 V. Density functional theory confirms that the superior structural stability and excellent thermal stability are attributed to the higher exchange energy of Li/Ni exchange and the higher formation energy of oxygen vacancies by ZrB2 doping. The present work offers a three in one strategy to simultaneously stabilize the crystal structure and surface for the Ni-rich cathode via a facile preparation process.

A Rapid and Facile Approach for the Recycling of High-Performance LiNi1-x-y Cox Mny O2 Active Materials.

The demand for lithium-ion batteries has risen dramatically over the years. Unfortunately, many of the essential component materials, such as cobalt and lithium, are both costly and of limited abundance. For this reason, the recycling of lithium-ion battery electrodes is crucial to ensuring the availability of such resources and protecting the environment. Herein, a simple and scalable recycling process was developed for the prototypical cathode active material Li1.02 (Ni0.8 Co0.1 Mn0.1 )0.98 O2 (NCM-811). By a combination of thermal decomposition and dissolution steps, spent NCM could be converted into Li2 CO3 and a transition metal oxalate blend, which served as precursors for new NCM. Importantly, it was also possible to individually separate each transition metal during the recycling process, thereby extending the utility of this method to a wide variety of NCM compositions. Each intermediate in the process was investigated by scanning electron microscopy and X-ray diffraction. Additionally, the elemental composition of the recycled NCM-811 was confirmed using inductively coupled plasma optical emission spectroscopy and energy-dispersive X-ray spectroscopy. The electrochemical performance of the recycled NCM-811 exhibited up to 80 % of the initial capacity of pristine NCM-811. The method presented herein serves as an efficient and environmentally benign alternative to existing recycling methods for lithium-ion battery electrode materials.

Improvement of the Electrochemical Performance of LiNi0.8Co0.1Mn0.1O2 via Atomic Layer Deposition of Lithium-Rich Zirconium Phosphate Coatings.

Owing to its high energy density, LiNi0.8Co0.1Mn0.1O2 (NMC811) is a cathode material of prime interest for electric vehicle battery manufacturers. However, NMC811 suffers from several irreversible parasitic reactions that lead to severe capacity fading and impedance buildup during prolonged cycling. Thin surface protection films coated on the cathode material mitigate degradative chemomechanical reactions at the electrode-electrolyte interphase, which helps to increase cycling stability. However, these coatings may impede the diffusion of lithium ions, and therefore, limit the performance of the cathode material at a high C-rate. Herein, we report on the synthesis of zirconium phosphate (ZrxPOy) and lithium-containing zirconium phosphate (LixZryPOz) coatings as artificial cathode-electrolyte interphases (ACEIs) on NMC811 using the atomic layer deposition technique. Upon prolonged cycling, the ZrxPOy- and LixZryPOz-coated NMC811 samples show 36.4 and 49.4% enhanced capacity retention, respectively, compared with the uncoated NMC811. Moreover, the addition of Li ions to the LixZryPOz coating enhances the rate performance and initial discharge capacity in comparison to the ZrxPOy-coated and uncoated samples. Using online electrochemical mass spectroscopy, we show that the coated ACEIs largely suppress the degradative parasitic side reactions observed with the uncoated NMC811 sample. Our study demonstrates that providing extra lithium to the ACEI layer improves the cycling stability of the NMC811 cathode material without sacrificing its rate capability performance.

Constructing a High-Energy and Durable Single-Crystal NCM811 Cathode for All-Solid-State Batteries by a Surface Engineering Strategy.

Single-crystal LiNi0.8Co0.1Mn0.1O2 (S-NCM811) with an electrochemomechanically compliant microstructure has attracted great attention in all-solid-state batteries (ASSBs) for its superior electrochemical performance compared to the polycrystalline counterpart. However, the undesired side reactions on the cathode/solid-state electrolyte (SSE) interface causes inferior capacity and rate capability than lithium-ion batteries, limiting the practical application of S-NCM811 in the ASSB technology. Herein, it shows that S-NCM811 delivers a high capacity (205 mAh g-1, 0.1C) with outstanding rate capability (175 mAh g-1 at 0.3C and 116 mAh g-1 at 1C) in ASSBs by the coating of a nano-lithium niobium oxide (LNO) layer via the atomic layer deposition technique combined with optimized post-annealing treatment. The working mechanism is verified as the nano-LNO layer effectively suppresses the decomposition of sulfide SSE and stabilizes the cathode/SSE interface. The post-annealing of the LNO layer at 400 °C improves the coating uniformity, eliminates the residual lithium salts, and leads to small impedance increasing and less electrochemical polarization during cycling compared with pristine materials. This work highlights the critical role of the post-annealed nano-LNO layer in the applications of a high-nickel cathode and offers some new insights into the designing of high-performance cathode materials for ASSBs.

Assembly of MXene/PP Separator and Its Enhancement for Ni-Rich LiNi0.8Co0.1Mn0.1O2 Electrochemical Performance.

In this work, a few-layer MXene is prepared and sprinkled on a commercial polypropylene (PP) separator by a facile spraying method to enhance the electrochemistry of the Ni-rich LiNi0.8Co0.1Mn0.1O2 (NCM811) cathode. Scanning electron microscope (SEM) and X-ray diffraction (XRD) are used to characterize the morphology and structure of MXene. Fourier transform infrared spectroscopy (FT-IR) and a contact angle tester are used to measure the bond structure and surface wettability PP and MXene/PP separator. The effect of the MXene/PP separator on the electrochemical performance of ternary NCM811 material is tested by an electrochemical workstation. The results show that the two-dimensional MXene material could improve the wettability of the separator to the electrolyte and greatly enhance the electrochemical properties of the NCM811 cathode. During 0.5 C current density cycling, the Li/NCM811 cell with MXene/PP separator remains at 166.2 mAh/g after the 100 cycles with ~90.7% retention. The Rct of MXene/PP cell is measured to be ~28.0 Ω. Combining all analyses results related to MXene/PP separator, the strategy by spraying the MXene on commercial PP is considered as a simple, convenient, and effective way to improve the electrochemical performance of the Ni-rich NCM811 cathode and it is expected to achieve large-scale in high-performance lithium-ion batteries in the near future.

Multifunctional Integration of Double-Shell Hybrid Nanostructure for Alleviating Surface Degradation of LiNi0.8Co0.1Mn0.1O2 Cathode for Advanced Lithium-Ion Batteries at High Cutoff Voltage.

Ni-rich LiNi0.8Co0.1Mn0.1O2 (NCM811) cathode is considered to be among the most promising candidates for high-energy-density lithium-ion batteries (LIBs). However, both capacity fading and structural degradation occur during long-term cycling, which extremely limit the commercial applications of NCM811, especially at a high cutoff voltage (>4.3 V). Here, we design a double-shell hybrid nanostructure consisting of a Li2SiO3 coating layer and a cation-mixed layer (Fm3̅m phase) to improve its electrochemical performance. Consequently, the Si-modified NCM811 electrode shows outstanding cycling stability with a 95.2% capacity retention at 4.3 V after 100 cycles and 87.3% at a 4.5 V high cutoff voltage after 100 cycles. This designed double-shell hybrid nanostructure alleviates side reactions, structural degradation, and internal cracking, effectively enhancing the surface structural stability. This efficient strategy provides a valuable step toward further commercial applications of the LiNi0.8Co0.1Mn0.1O2 cathode and enriches the fundamental understanding of layered cathode materials.

Constructing a Low-Impedance Interface on a High-Voltage LiNi0.8Co0.1Mn0.1O2 Cathode with 2,4,6-Triphenyl Boroxine as a Film-Forming Electrolyte Additive for Li-Ion Batteries.

Compared with other commercial cathode materials, the LiNi0.8Co0.1Mn0.1O2 cathode (NCM811) has high specific capacity and a relatively low cost. Nevertheless, the higher nickel content in NCM811 leads to an extremely unstable interface between the electrode and the electrolyte, resulting in inferior cyclic stability of the corresponding cell. Use of film-forming additives is regarded as the most feasible and economic approach to construct a stable interface on the NCM811 cathode. However, less effective electrolyte additives have been reported to date. Herein, we propose a valid film-forming electrolyte additive, 2,4,6-triphenyl boroxine (TPBX), for application in a high-voltage NCM811 cathode. Experimental and computational results reveal that the TPBX additive can be preferentially oxidized to generate a highly stable and conductive cathode electrolyte interface (CEI) layer on the NCM811 cathode, which efficiently suppresses the detrimental side reaction and improves the electrochemical performance eventually. In detail, the cyclic stability of the Li/NCM811 half-cell is enhanced from 57% (without additive) to 78% (with 5% TPBX) after 200 cycles at 1C between 3.0 and 4.35 V. At a high current rate of 15C, the TPBX-containing electrode delivers a capacity of about 135 mAh g-1, which is much higher than that of the electrode without the additive (80 mAh g-1). Interestingly, the TPBX is also reduced earlier than the ethylene carbonate (EC) solvent to form an ionically conductive solid electrolyte interface (SEI) film on the graphite anode. Due to the CEI layer on the cathode and the SEI film on the anode simultaneously formed by the TPBX additive, the cyclic performance of the graphite/LiNi0.8Co0.1Mn0.1O2 full cell is enhanced. Therefore, the incorporation of the TPBX additive into the electrolyte provides a convenient method for the commercial application of the high-energy-density NCM811 cathode in high-voltage lithium-ion batteries.