Nickel-rich Cathode Materials Research Articles

Al, Zr dual-doped cobalt-free nickel-rich cathode materials for lithium-ion batteries

Nickel-rich and cobalt-free cathode materials have obvious advantages in the aspects of energy density and economic efficiency. However, these materials are restricted from being used in commercial lithium-ion batteries due to the problems of poor structural stability and rate capability. In this study, the aluminum and zirconium dual-doped Co-free Ni-rich LiNi0.96Mn0.04O2 cathode material (NMAZ) is prepared by a facile high-temperature solid-phase method. The obtained NMAZ shows low cation disordering degree owing to the stability of transition metal slabs induced by strong Al–O and Zr–O bonds. Besides, the kinetics of lithium-ion diffusion is significantly improved by larger c-axis and the fast lithium-ion conducting Li2ZrO3 layer on the interface. As a result, NMAZ shows an improved capacity retention of 70.3% at 1C after 100 cycles under an elevated temperature (45 ​°C), compared with 50.5% of pure LiNi0.96Mn0.04O2. In addition, it exhibits splendid rate performance even at higher C-rate and better thermal stability compared to bare LiNi0.96Mn0.04O2. Hence, the Al, Zr dual-doped modification is beneficial to improving the structural stability and electrochemical performance of the Ni-rich and Co-free layered oxide cathodes for Li-ion batteries.

Degradation of Nickel-Rich layered oxides in ambient air and its inhibition by surface coating and doping

Nickel-rich layered cathode materials [LiNixCoyMn1-x-yO2 (x ≥ 0.6), NCM] have been considered as one of the most promising cathode materials for high energy lithium-ion batteries (LIBs) due to the low cost and high energy density. However, NCM can easily degrade in the air·H2O and CO2 will react with NCM to produce surface impurities mainly consisting of LiOH and Li2CO3. These impurity species have a negative impact on LIBs, such as slurry gelation and side reactions, which hinder the practical application of NCM materials. Here, we use ambient pressure X-ray photoelectron spectroscopy (APXPS) to monitor the NCM surface reactions in air and identify the degradation mechanism. Then, surface coating and surface doping are deployed on NCM by the combination of atomic layer deposition (ALD) and post-annealing. We prove that ZrO2 surface coating and Zr4+ surface doping can significantly inhibit the formation of LiOH and Li2CO3 on NCM surface in air through thermogravimetric analysis (TGA) and titration and hence eliminate the electrochemical performance degradation of the battery. This simple modification method is expected to be a potential solution to the problem of residual lithium in the large-scale production of nickel-rich layered cathode materials.

W Modification of Nickel-Rich Ternary Cathode Material for Efficient Lithium-Ion Batteries

As one of the fastest-growing cathode materials, Nickel-rich layered cathode material has caused much attention in the “next-generation” Li-ion batteries (LIBs) owning to the high specific energy, high operating potential and long cycling life. However, it still encounters a great of complications to realize the improvement of poor cycle stability and structural defects. In an effort to emphatically investigate the obvious advantages of eco-friendly and low-cost W doping cathode material on the crystalline morphology and electrochemical properties, LiNi0.65−xCo0.15Mn0.20WxO2 (x = 0.5%, 1.0%, 2.0%) were synthesized by hydroxide coprecipitation and calcination crystallization method. Especially, when the amount of W is 1.0% molar ratio, the initial discharge capacity reaches 216.55 mAh g−1 and achieves a capacity retention of 95.95% after 100 cycles with the operation voltage of 2.7–4.4 V at 1C. The reliable results show that the primary particle size via doping appropriate content of W become significantly smaller which can effectively consolidate the stability of the crystal cathode material and improve the recycling performance evidently. In addition, the element of W was detected in the lattice of the crystal particle, which bring about somewhat increase of lattice spacing and expands the Li+ diffusion channels during charge/discharge cycles. This work provides a potential application prospect by the strategy of W modification in the cathode materials of micron-sized particles for efficient lithium-ion batteries.

In Situ Inducing Spinel/Rock Salt Phases to Stabilize Ni-Rich Cathode via Sucrose Heat Treatment

Nickel-rich cathode materials have attracted widespread interest due to their high capacity; however, the structure is prone to degradation and collapse during cycling, resulting in poor stability performance and safety, hindering the development of high-nickel cathode materials. Here, we propose a straightforward method to consume oxygen on the surface of primary particles during the high-temperature calcination process of precursors, inducing the coupled rearrangement of surface cations, resulting in the in situ generation of a nano-sized mixed spinel/rock salt defect phase, which is confirmed by high-angle annular dark-field scanning transmission electron microscopy. LiNi 0.8 Co 0.1 Mn 0.1 O 2 modified with mixed phase not only can reduce side reactions with the electrolyte, resulting in fewer by-products such as LiF and Li 2 CO 3 , preventing the formation of excessively thick cathode–electrolyte interface layers, but also can avoid irreversible phase transitions and prevents lattice mismatches. As a result, the cycling performance has been improved to some extent, benefiting from structural stability. In addition, the special 3-dimensional structure of the spinel phase allows the material surface to expand ion transport channels and enhance multiplicative performance. Therefore, this study provides a new perspective on the modification of high-nickel materials and extends the application of nickel-rich materials.

Heteroatomic dopants derived from coal fly-ash for the synthesis of nickel-rich Li-ion battery cathode material

Fly ashes often become an environmental problem and are difficult to process. Utilizing coal fly ash as a product is a promising approach to overcoming it. In response to this problem, the metal content in fly ash waste in the form of Al2O3 and Fe2O3 can be utilized by applying them as dopants on the nickel-rich cathode material to achieve LiNixCoyAlzFe(1-x-y-z)O2 (NCAF) which is a modified form of nickel-based cathode material or NCA. In this study, NCAF material was made in 3 stages: (i) Recovery of valuable metals Al and Fe from fly ash by leaching and precipitation processes to obtain Aluminum-iron (AF) precursor; (ii) Nickel-cobalt (NC) containing precursors were prepared by mixing nickel and cobalt salts using the coprecipitation method. This NC precursor and AF were mixed at a mass ratio of 90:10; (iii) Lithiation through heat treatments under an O2 atmosphere to form NCAF cathode material. The results of the NCAF material characterization are: (i) The XRD test showed the same diffraction pattern as the JCPDS 87-1562 reference; (ii) FTIR test of NCAF material showed that the storage condition affects the surface of NCAF powder; (iii) SEM-EDX test showed that the NCAF material has an agglomerated morphology and crystal-shape with a primary particle size of around 140 nm; (iv) Electrochemical test of Li-ion battery with NCAF cathode using graphite as anode showed charge and discharge capacity of 172 mAh/g and 144 mAh/g, respectively. Based on the results, implementing Al and Fe from fly ash as materials for Li-ion batteries should be considered for future energy storage technology developments.

Micro- and nano-structural design strategies towards polycrystalline nickel-rich layered cathode materials

The development of micro- & nano-structure engineering in recent years is reviewed. The synthesis methods and mechanisms of different microstructures are summarized, and the future development direction of microstructure modification is proposed.

Atomic-level insights into the first cycle irreversible capacity loss of Ni-rich layered cathodes for Li-ion batteries

Our study identifies that the first cycle IRC loss is strongly related to the irreversibility of the Ni charge state, which limits the capacity and energy density.

The genesis and control of microcracks in nickel-rich cathode materials for lithium-ion batteries

A schematic diagram of the formation, detrimental impacts of microcracks, and the corresponding modification strategies.

Crystallization of nickel sulfate and its purification process: towards efficient production of nickel-rich cathode materials for lithium-ion batteries.

NiSO4·6H2O is an important salt for the battery-making industry. The extraction of nickel sulfate relies on the hydrometallurgical processing of nickel ores as well as the recycling of nickel-containing products. The last step in hydrometallurgical processing is the crystallization of nickel sulfate. Because of the similar ionic radius and ionic charge between nickel and magnesium ions, magnesium undergoes isomorphous substitution and replaces nickel ions in the crystal lattice structure of NiSO4·6H2O. This poses a challenge as achieving the desired metal salt purity is difficult, resulting in an inferior cathode material for nickel-containing batteries. In this work, the removal of magnesium during the purification process of NiSO4·6H2O crystals via a repulping process was thoroughly investigated. Moreover, the impurity uptake mechanisms of magnesium into NiSO4·6H2O crystals were investigated. The results indicated that repulping NiSO4·6H2O crystals with a saturated NiSO4 solution results in 77% removal of magnesium. Using a second-stage repulping process is less effective with only 26% magnesium removal. The purification efficiency of the two repulping stages was quantified by the equilibrium distribution coefficient, which corroborates the trend of decreased removal of magnesium in the second stage of repulping compared with the first stage. The primary impurity uptake mechanisms of magnesium into NiSO4·6H2O crystals were identified to be surface adsorption and lattice substitution (isomorphous substitution).

Revealing the effect of Nb5+ on the electrochemical performance of nickel-rich layered LiNi0.83Co0.11Mn0.06O2 oxide cathode for lithium-ion batteries

The layered Nb5+-doped LiNi0.83Co0.11Mn0.06O2 (NCM) oxide cathode materials are successfully synthesized through introducing Nb2O5 into the precursor Ni0.83Co0.11Mn0.06(OH)2 during the lithiation process. The results refined by GSAS software present that the Nb5+-doped samples possess the perfect crystal structure with broader Li+ diffusion pathways. Moreover, the morphology characterized by scanning electron microscope displays the compact secondary particles packed by smaller primary particles under the effect of Nb5+. The excellent electrochemical properties are also acquired from the Nb5+-doped samples, in which the optimal rate performance and cycling stability are performed for NCM-1.0 when up to 1.0 mol % of Nb2O5 (based on the precursor) is added. Benefited from the introduction of Nb5+, the cell assembled with the NCM-1.0 electrode retains higher capacity retention of 86.6 % at 1.0 C and 25 °C, and 71.7 % at 1.0 C and 60 °C after 200cycles. Moreover, it also delivers higher discharge specific capacity of 154.6 mAh g−1 at 5.0 C. Therefore, the Nb5+-doping strategy may open an effective route for optimizing nickel-rich oxide cathode materials, which is worth popularizing for the enhancement of the electrochemical performance of nickel-rich cathodes for lithium-ion batteries.

Effects of the preheating temperature on flame-assisted spray pyrolysis of nickel-rich cathode materials

Reducing the cost and improving the performance of lithium-ion batteries (LIBs) are crucial for their applications in transportation electrification and grid energy storage. Much research effort has been devoted to develop novel synthesis methods for LIB cathodes, since traditional methods such as coprecipitation suffer long synthesis time and complex steps. In contrast, flame-based spray methods have great potential in manufacturing LIB cathode materials due to their features such as continuous, fast, and scalable operation. Nevertheless, flame-based spray methods also need improvement in controlling the morphology and improving the electrochemical performance of LIBs. The current work demonstrated a modified flame-assisted spray pyrolysis (FASP) method that used a preheating section for morphology control and electrochemical performance enhancement. The goal is to investigate the effect of preheating temperature on the particle morphology and electrochemical performance of Li(Ni0.8Co0.1Mn0.1)O2 (NCM811) cathode materials. Results showed that the preheating temperature could significantly alter the particle morphology by affecting the drying process. X-ray diffraction measurements demonstrated that the cation mixing level of NCM811 samples was sensitive to the preheating temperature, where introducing the preheating section was effective in inhibiting cation mixing and improving cation ordering at certain temperatures. However, a preheating temperature higher than 325 °C would notably encourage cation mixing. Moreover, the electrochemical tests showed that increasing the preheating temperature could improve the discharge capacity and stabilize the long-time cycling performance. Overall, carefully choosing the preheating temperature of FASP not only improved the particle uniformity by inhibiting the formation of hard-to-break agglomerations in calcinated powders, but also enhanced the electrochemical performance by hindering cation mixing.

Constructing an organic artificial cathode electrolyte interphase of multi-functions on single-crystal LiNi0.8Co0.1Mn0.1O2 cathode

Nickel-rich layered oxide materials are of great significance for high energy density lithium-ion batteries due to their high theoretical capacity. However, interfacial side reaction is known to be an important cause for their electrochemical degradation. Herein, we construct an organic artificial solid electrolyte interface with 4-cyanophenylboronic acid (4-CPBA) as a precursor on a single-crystal LiNi0.8Co0.1Mn0.1O2 (NCM811) surface. As a strong electron-absorbing group, cyano groups help to anchor the interfacial Ni2+ while the boronic acid groups contributes to remove the residual lithium and passivate the NCM811 surface. After wrapping the 11 nm thick artificial cathode electrolyte interface (CEI) precursor, the prepared NCM811 cathode exhibits an improved first coulomb efficiency of 93.5% at high temperature. A capacity retention of 82.5% after 200 cycles is obtained at 1C charge-discharge condition, significantly higher than that of 61.0% for the pristine cathode. The post analysis reveals that 4-CPBA is involved in the formation of CEI film and of many different functions on the cathode surface. The new interfacial modification strategy based on the synergistic interaction between the high nickel cathode material and functional organic molecules expands CEI technologies on nickel rich cathode materials.

Synthesis and Electrochemical Characterizations of Concentration-Gradient Structure Nickel-Rich Cathode Materials

Synthesis and Electrochemical Characterizations of Concentration-Gradient Structure Nickel-Rich Cathode Materials

Enhanced Structural Stability and Capacity Retention of Ni-Rich LiNi0.91Co0.06Mn0.03O2 Cathode Material By Dual Doping and Coating for Libs

Nickel-rich layered cathode material has been received a lot of attention due to their superior cycle-ability, high energy density and improved safety. However, there are some issues which are needed to be resolved to ensure the long term application. The hostile attack of electrolyte with the charged cathode electrode results in the growth of thick solid electrolyte interphase (SEI) at the expense of Li+ consumption and increase in interfacial resistance. In addition, de/intercalation of Li+ leads to the continuous contraction and expansion of lattice structure that leads to the crack formation in the active material particles during extended cycling.In this work, a facile technique has been adopted to resolve the mentioned problems. In this study, Li3BO3 has been coated on the NCM surface to protect the active material against the continuous attack of electrolyte and boron is doped to enhance the structural stability of LiNi0.91Co0.06Mn0.03O2 NCM cathode material. The samples were characterized by XPS, XRD, SEM and TEM and the electrochemical properties were measured by assembling the coin cells. The XRD results confirm the shifting of (003) diffraction peak towards low angle which validates the boron doping in the crystal structure. The presence of B1s is confirmed on the surface of modified NCM by XPS analysis. The FETEM images shows a uniform and distinct coating layer of 12 nm on the surface of 0.05 wt% coated NCM. The 0.05 wt% NCM samples offers the highest discharge capacity of 215.3 mAh g-1 at 0.1C and capacity retention of 81.6% at 0.5C (1C = 202 mA g-1) after 100 cycles. The reason behind enhanced cycling is the high bond dissociation energy of B−O (ΔHf298 = 402 kJ mol−1) than Ni–O (ΔHf298 = 391.6 kJ mol−1), Co–O (ΔHf298 = 368 kJ mol−1) and even Mn–O (ΔHf298 = 402 kJ mol−1). Even at 2C cycling, LBO-0.05 NCM sample demonstrated a capacity retention of 79.4% after 100 cycles while pristine shows only 67.3%. The modified samples displayed superior rate performance as compare to pristine NCM, especially at high current density. The cyclic voltammetry and EIS results are in-line with the cycling data. The presence of B3+ doping in host structure and Li3BO3 coating on the NCM surface results in the superior electrochemical performance of modified NCM.

Comparative Study of NCM and NCA Electrode Material for Capacity-Fade Using 1-D Modeling

Today, Lithium-ion (Li-ion) batteries are one of the most emerging power sources for almost all modern consumer electronic products. LiNi0.8Co0.15Al0.05O2 (NCA) and LiNi0.3Co0.3Mn0.3O2 (NCM) are projected to be utilized in lithium-ion power batteries as two typical layered nickel-rich ternary cathode materials. Moreover, there is still a need for systematic study from an industrial aspect as to the advantages and drawbacks of these two nickel-rich materials. Hence, a comparative study of NCM and NCA electrode material for capacity-fade has been explored using a 1-D simulated model constructed in the multi-physics software. The capacity of a battery depends on the cell potential, discharge rate, state of charge (SoC), and state of health (SoH). Therefore, the comparison of these parameters and the cycle number of a battery is extremely important. During this comparative study of NCM and NCA electrode material, the capacity fade based on discharge rate, SoC, and SoH over cycle number of a battery has been reported.

Correlating Morphological and Structural Evolution with the Electrochemical Performance of Nickel-Rich Cathode Materials: From Polycrystal to Single Crystal

Nickel-rich layered oxides (Ni ≥ 90%) have been recognized as a promising cathode material for Lithium-ion batteries (LIBs) owing to their high energy density and low cost. Herein, we prepared 20 LiNi0.90Co0.06Mn0.04O2 (Ni90) samples with various morphologies by regulating sintering temperature and the lithium to transition metal ratio. The correlation between the synthesis conditions, structural properties, and electrochemical performance of Ni90 materials was thoroughly investigated during the evolution from polycrystal to single crystal. A positive and linear relationship was found between sintering temperature and primary particle size (PPS), which affect the electrochemical performance profoundly. Polycrystals with small PPS show a high discharge capacity and low polarization, while single crystals with large PPS have low discharge capacity but excellent cycling stability. Moreover, the sluggish kinetic properties of Ni90 materials at the end of discharge (a sharp drop in lithium-ion diffusion coefficient at the end of discharge) lead the morphology factors to a critical feature that dominates the total discharge capacity. Taking discharge capacity and cycling stability into integrated consideration, the quasi-single crystal Ni90 materials with moderate PPS and the lowest cation disordering is the first choice. These findings contribute to a better understanding of polycrystalline and single-crystal Nickel-rich cathode materials for LIBs.

Nanoscale surface modification to suppress capacity fade of Ni-Rich layered oxide material at high cut-off voltage

Ni-rich layered oxide is a promising cathode material for future advanced lithium-ion batteries (LIBs). However, the nickel-rich layered cathode material exhibits insufficient high-voltage cycling stability ascribing to the phase transformation, surface side reactions, and lattice oxygen evolution. This work developed an effective inorganic coating strategy to construct LiNiO2/Na1-xNi1-yPO4 surface hybrid coating layer and Na bulk doping simultaneously by a simple wet-chemical method, improving the high-voltage performance of LiNi0.8Co0.1Mn0.1O2 (NCM) effectively. It is found that the surface oxygen vacancy and surface residual lithium on NCM reacts with NaNiPO4 precursors at 500 °C to form LiNiO2 inner layer in addition to the Na1-xNi1-yPO4 outer layer, which is structurally coherent to the layered lattice of NCM. In the constructed hybrid layer, layered phase LiNiO2 firmly fixes on the NCM surface. At the same time, highly chemical stable Na1-xNi1-yPO4 with lattice tunnels can enable lithium-ion transport and act as a protecting layer to inhibit surface side reactions. In addition, Na bulk doping could enlarge lithium-ion diffusion channels and stabilize lattice structure. All these advantages contribute to improving the electrochemical performance of NCM. The results show that the surface treatment NCM cathode exhibit excellent cycling stability with a higher capacity retention of 88 % after 200 cycles under 25 °C and 86 % after 100 cycles under 55 °C, both at 1C. This method provides a feasible strategy to promote the high-voltage cycling performance of electrode material, thus improving the service life, energy density, and safety performance of Li-ion batteries.

A Mini Review on Ni-rich Layered Oxide Cathode Materials

The global energy demand and increasing global warming are threats to the planet; therefore, replacing internal combustion engine vehicles to electric vehicles is prerequisite. Rechargeable batteries are key component to operate electric vehicles, among which lithium-ion batteries are governing the industry. After the successful discovery of Goodenough’s LiCoO2, layered oxides are emerging and are considered to be the next-generation cathodes. Ni-rich layered oxides are the new-generation cathode material owing to high specific capacity, high energy density, high operating voltage and low cost. Substitution of Co, Mn and Al is advantageous to compensate for the loss of the storage capacity and structural degradation. This review aims to discuss the characteristics, structure and preparation methods for nickel-rich layered oxide cathode material.

The Role of Gas Evolution in Particle Surface Cracking in Nickel-Rich Lithium-Ion Cathode Materials

Nickel-rich layered oxide cathode materials (LiNixTM(1-x)O2 where x > 0.8) are of great interest because they offer increased capacity compared to current commercial materials while maintaining compatibility with supply chain and production processes already in place. However, recent studies have shown that these materials in their current form are unsuitable for commercial applications due to the accelerated degradation caused by replacing more stable transition metals with the relatively unstable nickel. While various strategies have already been proposed to mitigate this issue, the fundamental degradation mechanism still needs to be better understood to inform the design of the next generation of nickel-rich cathode materials. In this work, differential electrochemical mass spectrometry (DEMS) is combined with titration mass spectrometry (TiMS) to measure gases evolved in a lithium half-cell during cycling as well as surface species which evolve gas upon addition of strong acid to an extracted cathode. Along with qualitative observations of particle cracking by scanning electron microscopy (SEM), these results reveal correlations between particle cracking, electrolyte reactivity, and carbonate oxidation and deposition on the changing cathode surface in nickel-rich cathode materials.

The Effect of Annealing on the Structure, Composition and Electrochemistry of NMC811 Coated with Al2O3 Using an Alkoxide Precursor

Increasing capacities and lowering costs of the cathode material is a key challenge in lithium ion-battery research. Towards this end, nickel-rich layered oxides of the formula Li[NixMnyCoy]O2 (NMC) with x ≥ 0.8 were developed. Compared to previously used cathodes such as LiCoO2 , nickel-rich NMCs reach lower costs by replacing most of the cobalt with nickel and they enable higher discharge capacities.1 Despite the presence of small amounts of cobalt and manganese as dopants to improve stability and rate-capability, these materials still show fast capacity fade during electrochemical cycling which cannot be overcome by modifying the ratio of their elements.2 New strategies to mitigate this degradation are therefore urgently needed for the use of these materials in practical applications such as electric vehicles.3 Most of the degradation that occurs in nickel-rich NMCs upon cycling starts at the cathode-electrolyte interface via surface reactions,oxygen evolution followed by rock-salt formationand transition metal dissolution.4–6 One way to slow down or stop these processes is by changing the nature of this interface through coatings. Although there is a large number of studies showing the benefits of using them, knowledge on the design of coatings with specific properties is still lacking.7,8 In this work, we develop a new solution-based deposition method for the synthesis of aluminium oxide coatings onto LiNi0.8Mn0.1Co0.1O2 (NMC811) secondary particles (Figure 1) and study the effect of annealing on their structure and electrochemical lifetime as new-generation cathode for lithium-ion batteries. Using energy dispersive X-ray spectroscopy (EDS) and X-ray fluorescence spectroscopy (XRF) we quantify the amount and distribution of aluminium oxide on the cathode particles. By using solid-state nuclear magnetic resonance (SS-NMR) and X-ray photoelectron spectroscopy (XPS), we track changes in the coating phase and composition as a function of annealing temperature. 27Al NMR spectroscopy provides direct evidence of the diffusion of the coating into the bulk of the particles leading to surface-layer doping. Finally, we evaluate the electrochemical performance of the coated materials in half cells using long-term galvanostatic cycling. This work provides insight on the effects of surface coating and doping on battery degradation and shows how, by carefully selecting synthetic conditions, coatings of cathode particles with tailored properties can be prepared.(1) Myung, S.-T.; Maglia, F.; Park, K.-J.; Yoon, C. S.; Lamp, P.; Kim, S.-J.; Sun, Y.-K. Nickel-Rich Layered Cathode Materials for Automotive Lithium-Ion Batteries: Achievements and Perspectives. ACS Energy Letters 2017, 2 (1), 196–223. https://doi.org/10.1021/acsenergylett.6b00594.(2) Noh, H.-J.; Youn, S.; Yoon, C. S.; Sun, Y.-K. Comparison of the Structural and Electrochemical Properties of Layered Li[NixCoyMnz]O2 (x = 1/3, 0.5, 0.6, 0.7, 0.8 and 0.85) Cathode Material for Lithium-Ion Batteries. Journal of Power Sources 2013, 233, 121–130. https://doi.org/10.1016/j.jpowsour.2013.01.063.(3) Kim, J.; Lee, H.; Cha, H.; Yoon, M.; Park, M.; Cho, J. Prospect and Reality of Ni-Rich Cathode for Commercialization. Advanced Energy Materials 2018, 8 (6), 1702028. https://doi.org/10.1002/aenm.201702028.(4) Rinkel, B. L. D.; Hall, D. S.; Temprano, I.; Grey, C. P. Electrolyte Oxidation Pathways in Lithium-Ion Batteries. J. Am. Chem. Soc. 2020, 142 (35), 15058–15074. https://doi.org/10.1021/jacs.0c06363.(5) Wandt, J.; Freiberg, A.; Thomas, R.; Gorlin, Y.; Siebel, A.; Jung, R.; Gasteiger, H. A.; Tromp, M. Transition Metal Dissolution and Deposition in Li-Ion Batteries Investigated by Operando X-Ray Absorption Spectroscopy. J. Mater. Chem. A 2016, 4 (47), 18300–18305. https://doi.org/10.1039/C6TA08865A.(6) Xu, C.; Märker, K.; Lee, J.; Mahadevegowda, A.; Reeves, P. J.; Day, S. J.; Groh, M. F.; Emge, S. P.; Ducati, C.; Layla Mehdi, B.; Tang, C. C.; Grey, C. P. Bulk Fatigue Induced by Surface Reconstruction in Layered Ni-Rich Cathodes for Li-Ion Batteries. Nat. Mater. 2020. https://doi.org/10.1038/s41563-020-0767-8.(7) Shi, Y.; Zhang, M.; Qian, D.; Meng, Y. S. Ultrathin Al2O3 Coatings for Improved Cycling Performance and Thermal Stability of LiNi0.5Co0.2Mn0.3O2 Cathode Material. Electrochimica Acta 2016, 203, 154–161. https://doi.org/10.1016/j.electacta.2016.03.185.(8) Neudeck, S.; Strauss, F.; Garcia, G.; Wolf, H.; Janek, J.; Hartmann, P.; Brezesinski, T. Room Temperature, Liquid-Phase Al2O3 Surface Coating Approach for Ni-Rich Layered Oxide Cathode Material. Chemical Communications 2019, 55 (15), 2174–2177. https://doi.org/10.1039/C8CC09618J. Figure 1