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LiNi0.8Co0.1Mn0.1O2 (NCM811) has a high potential for using as the cathode material for lithium–ion batteries (LIBs) for electric vehicles owing to its high energy density and low cost. However, its poor rate capability and cycling performance have significantly hindered its application. In this study, we successfully design a uniform magnesium oxi...
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Citations
... [18][19][20][21] Several researchers focused on coatings such as ZrO 2 , Al 2 O 3 , WO 3, and MgO due to their high chemical and electrochemical stability. [22][23][24] However, Li-ion transport becomes compromised beyond the optimal thickness of these coatings on NMC. Also prolonged full cell (against graphite) cycling stability at high discharge rates such as 2 C is still questionable in the case of some of these coatings. ...
Nickel‐rich cathode materials such as LiNi0.9Co0.05Mn0.05O2 (NMC90) have gained attention due to their ability to deliver high energy densities while being cost‐effective for Lithium‐ion battery manufacturing. However, NMC90 cathodes suffer irreversible parasitic reactions such as electrolyte decomposition, severe capacity fading and impedance build‐up upon prolonged cycling. Herein, we synthesize a conformal ultrathin, surface protection layer on NMC90 powder using ZnxOy via atomic layer deposition technique (ZnxOy@NMC90). Prolonged electrochemical investigation of full cells at high discharge rates of 2 C shows that ZnxOy@NMC90 cells yielded ~31 % improvement in discharge capacity compared to pristine NMC90. Furthermore, operando electrochemical mass spectroscopy studies show that the ZnxOy@NMC90 cells have significantly suppressed electrolyte decomposition as compared to pristine NMC90 cells. Post‐cycling electrochemical impedance spectroscopy studies show that the ZnxOy@NMC90 full cells have significantly reduced impedance compared with pristine NMC90 cells. Additionally, post cycling manganese dissolution studies show that ZnxOy@NMC90 cells have greatly enhanced chemo‐mechanical integrity thereby contributing to improved electrochemical performances. Our results underscore the potential of tailored ZnxOy surface coatings on nickel‐rich cathode materials to address critical challenges in advanced energy storage systems, offering promising prospects for the development of high‐energy‐density lithium‐ion batteries.
... Surface modification is an effective approach to improve the electrochemical performance and overcome the limitations of NCM electrode materials [13,[18][19][20]. Thus far, metal oxides, fluorides, phosphates, and other coatings, such as MgO [21], ZrO 2 [16], SiO 2 [22], Al 2 O 3 [23,24], Nd 2 O 3 [25], LaFeO 3 [26], LiNbO 3 [27], LiAlO 2 [28], LBO (Li 2 O-2B 2 O 3 ) [16], Li 2 TiO 3 [29], Li 2 ZrO 3 [30], Li 2 WO 4 /WO 3 [12], Li 3 VO 4 [31], Li 4 Ti 5 O 12 [32], LiF [33], CaF 2 [34], FePO 4 [11], Li 3 PO 4 [35], polysiloxane [36], polyaniline [37], and dual coatings such as Li 3 PO 4 with polypyrrole (PPy) [38] have been applied to the surface of NCM811 to improve its electrochemical performance. Surface modification of bulk materials can segregate the bulk materials from the electrolyte, thus protecting the material surface from being attacked by the electrolyte during (de)lithiation [16]. ...
Ni-rich LiNi0.8Co0.1Mn0.1O2 (NCM811) is a promising high-performance cathode material for
large-scale Li-ion storage applications. However, devices consisting of Ni-rich materials are less
thermally stable, and several factors hinder their use in practical high-energy-density applications.
Herein, an approach for plasma-modified NCM811 with TiN is proposed to effectively improve
the electrochemical performance and stabilize the cathode–electrolyte interface reaction. In
addition, the following aspects are systematically investigated using different techniques: (i)
physicochemical properties; (ii) Li storage performance, particularly, cyclic/rate capacity, kinetic
behavior of the lithium-ion diffusivities, and electrical conductivity; and (iii) key factor for
improving the electrochemical performance through ex-situ/in-situ investigations. The NCM811-
TiN/graphite pouch cell displays a high reversible capacity of 17.5 mAh and sustains over 200
cycles at 1 C. Comprehensive characterization and probes indicate that the TiN interface with the
NCM electrode enhances thermal stability, cyclic capacity, and rate stability without changing the
bulk structure and morphology. Hence, these findings facilitate the practical use of safe and high-
energy-density Li-ion batteries.
... Among them, the surface coating can prevent the surface of NCM cathode materials from directly contacting with organic electrolyte, reduce the interface side reaction, and thus improve the cycle stability of the NCM cathodes. The common coating agents mainly include oxides (AlO 3 [20,21], MgO [22,23]), phosphates (FePO 4 [24,25], Ni 3 (PO 4 ) 2 [26,27]), and fluorides (CaF 2 [28,29], AlF 3 [30,31]). However, these materials have poor ionic and electronic conductivity, which will hinder the migration of ions and electrons and increase the electrochemical polarization and interface impedance. ...
Ni-rich layered cathode materials LiNixCoyMn(1-x–y)O2 (x ≥ 0.8) suffer from capacity decay due to structural deterioration during electrochemical cycling. To overcome these problems, the fast-ion conductor Li0.33La0.56TiO3 (LLTO) is coated on the surface of LiNi0.83Co0.12Mn0.05O2 (NCM83) cathodes through the sol–gel method, which can stabilize the electrode/electrolyte interface of cathode materials and facilitate Li⁺ transport and charge transfer. As a result, the LLTO-coated NCM83 exhibits better cycle stability and higher rate performance. The NCM83 modified by 5 wt% LLTO has the discharge capacity of 185.9 mAh g⁻¹ at 1C rate after 100 cycles and with higher capacity retention of 92.9% than the pristine NCM83 of 86.2%, and as well as the 5 wt% LLTO-coated NCM83 has a higher Li⁺-insert diffusion coefficient of 1.143 × 10⁻¹¹ cm² s⁻¹ than the pristine NCM83 of 8.757 × 10⁻¹² cm² s⁻¹. Therefore, the fast-ion conductor LLTO coating strategy shows great potential in improving the performance of Ni-rich layered cathode materials.
... For decreasing the undesired reactions, the surface coating of cathode active materials has been investigated. According to the presented reports, this process protects the cathode electrode against side reactions with HF acid and reduces oxygen loss from cathode material [12]. Recently, synthesis and investigation of the electrochemical performance of Li-Ni 0.6 Mn 0.2 Co 0.2 O 2 (NMC666) have been carried out as the promising material for the cathode of Li-ion battery (Ref [13][14][15] The slurry of cathode material, binder, and carbon is coated on the Al foil as a current collector. ...
The surface of LiNi0.6Mn0.2Co0.2O2 particles and current collector was modified with Cr2O3, and NaOH solution, respectively, and the electrochemical performance of NMC622 as a cathode material of Li-ion battery was investigated. The contact angle test shows the more wettability of the modified Al foil, confirming the better adhesion of cathode material slurry on that. The cell with a modified current collector has more capacity (176.6 mAh g−1 at 0.1C) at the first cycle and better cyclic performance (capacity loss of 12.8% after 50 cycles) than the cell with the unmodified current collector (172.3 mAh g−1 at 0.1C, and capacity loss of 17% after 50 cycles). Moreover, modifying the surface of NMC622 particles as a cathode active material with 0.5 wt.% of Cr2O3 and surface treatment of the current collector leads to a high capacity (179.8 mAh g−1 at 0.1C) and improved cyclic stability; capacity loss of 9.1% after 50 cycles.
... Among the various methods mentioned above, surface modification is a feasible means to reduce direct contact between electrode material and electrolyte to improve its structural and electrochemical stabilities. Some kinds of metal oxides, such as MgO [16], Al 2 O 3 [17], SiO 2 [18], TiO 2 [19], ZrO 2 [20] and ZnO [21] have been applied in surface coating, aiming to decrease the decomposition of electrolyte and HF corrosion. Nowadays, the metal oxides were used as another surface stabilizer, which can effectively increase the cycling performance of cathode materials, and have been widely used in different cathode, such as LiCoO 2 [22], LiNi 0.5 Mn 1.5 O 4 [23], and Li 2 FeP 2 O 7 [24] for the lithium-ion batteries. ...
The LiNi0.5Mn1.5O4 (LNMO) is an ideal cathode material of lithium-ion battery due to its high operating voltage. However, the corrosion of the electrolyte at high voltage is also a key issue for the LNMO cathode. In current work, the CeF4 were used to coat LNMO pristine via a simple calcining synthesis process. The microstructure and morphology of the pristine and CeF4-coated samples were studied by XRD, FTIR, XPS SEM, and TEM. The microstructure and morphology analysis show that CeF4 successfully coats on the surface of LNMO and forms a uniform coating layer. The CeF4 layers have little effect on the crystal structure of the LNMO and surface characters keep stable. The electrochemical performance study revealed that the CeF4-coated samples owned higher rate capacity and galvanostatic change–discharge capacity at 5C because the CeF4 layer was benefit to Li+ diffusion that decrease the polarization resistance. Moreover, the CeF4-3 has best cycling performance and rate capacity among all samples. After 100 charge–discharge cycles, the specific discharge capacity of CeF4-3 is still maintained 120 mAh/g with 97.6% capacity retention, while the pristine LNMO is only 97 mAh/g with 94.0% capacity retention. Therefore, CeF4 can be regarded as a promising anode modification material to improve the electrochemical performance.
... This route resulted in a change in the crystal structure of the surface states at the interface with the coating and a change in cycling performance. 110 Initial charge and discharge capacities of the MgO coated NMC 811 particles were 225.6 mA·h·g −1 and 190.1 mA·h·g −1 , respectively, and the Coulombic efficiency was 84.1%. In contrast, the charge and discharge capacities for the uncoated NMC 811 particles were 235.2 mA·h·g −1 and 194.2 mA·h·g −1 , but the Coulombic efficiency was ∼83%. ...
... Cyclic voltammetry plots for the first three potential cycles from 2.8 to 4.3 V (vs Li/Li + ) for: (a) pristine NMC 811 particles; and (b) MgO coated NMC 811 cathode particles; reproduced with permissions. 110 modification suppressed an increase in resistance following repetitive Li + insertion and extraction up to 4.2 V (vs Li/Li + ). 112 The charge transfer resistances (R ct ) for bare and coated LCO films were found to be 250 Ω and 750 Ω, respectively. ...
Lithium ion batteries (LIBs) have dominated the energy industry due to their unmatchable properties, which include high energy density, compact design, and an ability to meet a number of required performance characteristics in comparison to other rechargeable systems. Both government agencies and industries are performing intensive research on Li-ion batteries for building an energy-sustainable economy. LIBs are single entities that consist of both organic and inorganic materials with features covering multiple length scales. Critical insights should be made for understanding the structure to property relationships and the behavior of components under the working condition of LIBs. Cathodes tend to react with the electrolytes and, hence, to undergo surface modifications accompanied by degradation. These side-reactions result in an erosion of battery performance, thereby causing a reduced battery life and power capacity. Recently, techniques for preparing surface coatings on cathode materials have been widely implemented as a measure to improve their stability, to enhance their electrochemical performance. This review will cover different types of surface coatings for cathode materials, as well as a comparison of the changes in electrochemical performance between those materials with and without an applied coating.
... 45 The potential difference (ΔV) between the largest anodic and cathodic peaks may be attributable to the generation of SEI films on the electrode surfaces, with the calculated value confirming the level of electrochemical reversibility. 52,53 Figure 8a−e reveals that the potential difference for L 4 -NCM (ca. 174 mV) was lower than those for L 0 -NCM (ca. ...
... Additionally, the doping of Mg 2+ can enhance the thermal stability of the layered oxide material [26]. Therefore, a small amount of magnesium ion bulk doping in the high nickel ternary cathode materials is considered as one of the effective ways to promote their electrochemical performance [27][28][29][30]. ...
Achieving a highly stable structure is the key to successfully enhancing the cycling stability and safety performance of LiNi0.8Co0.1Mn0.1O2 (NCM811) cathode material for Li-ion batteries at a high cutoff voltage (4.5 V). In this work, the co-precipitation method is applied to prepare the precursor of the full concentration gradient (FCG) NCM811, and Mg2+ is doped into bulk phase to prepare LiNi0.8-xCo0.1Mn0.1MgxO2 (x = 0.01, 0.02, 0.03, and 0.04) for modification. Influences of magnesium doping direction and magnitude on electrochemical performance are investigated. It is found that Li(Ni0.8Co0.1Mn0.1)1-xMgxO2 shows low Li+/Ni2+ cation mixing in the voltage of 2.7–4.5 V with high structural stability and improves cycling stability because of the pillaring effect of inactive Mg in the crystal structure. In terms of the doping direction, compared with the uniform magnesium doping material, the specific discharge capacity with a forward concentration gradient doping is increased by 5.96%, and the cycle stability can be promoted as high as 6.33%. For the magnitude of the doping concentration gradient, the specific discharge capacity compared to pristine (Ni0.8Co0.1Mn0.1O2) material can be increased by 10.1%, and correspondingly the cycle stability can be promoted as high as 13.7%. After doping 3% Mg2+ with the optimal forward concentration gradient direction and cycling for 200 cycles at 2.7 ~ 4.5 V and 1 C, the specific discharge capacity is up to 163.5 mAh/g, and the capacity retention rate can keep 82.99%. Additionally, LiNi0.8Co0.1Mn0.1O2 doped with 3% Mg2+ along the forward concentration gradient direction has a positive effect on reducing the material impedance.
... Various metal oxides are being used for surface modification of cathodes in LiBs such as MgO [132], ZnO [133], Al 2 O 3 [134], TiO 2 [135], ZrO 2 [136], RuO 2 [137], CeO 2 [138], SiO 2 [139], etc. Among the materials, Al 2 O 3 , MgO, and TiO 2 are frequently being used for surface coating in LiBs. ...
With an advanced understanding of cathode materials in Li-ion batteries (LiBs) and supercapacitors, it has been observed that the surface structures of cathodes play an important role in these devices and significantly affects the whole system's performance e.g. maintain the structural stability and material's conductivity. Various approaches are being applied to enhance the electrochemical performances of batteries and supercapacitors e.g. Doping of transition metal ions, synthesis of composite materials, synthesis of nanomaterials, and surface modification of materials. Among these techniques, surface modification of the electrode materials is widely used because of ease of synthesis and cost effectiveness. In the present article, the recent advancements in surface modifications of the energy storage electrode materials and their electrochemical performances are summarized. First, coating strategies and their effects on cathode are discussed and then the current research progress focusing on the surface coating materials are covered. At last, the challenges faced are discussed to improve the performances of cathode materials. In this study, we are presenting that the selection of coating materials and technologies plays a vital role in the advancement of cathode materials.
... NCM111 (LiNi 1/3 Co 1/3 Mn 1/3 O 2 ) has the best layer structure, with the increasing content of Ni, the worse of layer structure, and the worst of electrochemical performance at the same time. Generally, the ratio of X-ray diffraction peak intensity of crystal plane (003) to crystal plane (104) is used to judge the Li/Ni disordering degree of layered structure [25]. The higher the ratio, the better the layered structure (Table 1). ...
... Ma et al. [25] used wet chemical method to coat NCM811 with MgO. XRD test shows that the MgO-coated NCM811 corresponds to the X-ray diffraction peaks of each crystal face of pristine NCM811, which proves that the two samples have the same layer structure. ...
... As a matter of fact, coating may reduce the electrical conductivity of the material; in the process of industrial production, controlling the thickness of the cladding is Fig. 15 The XRD pattern of uncoated NCM811 and coated NCM811 with MgO. Reproduced with permission [25], copyright, 2019, Journal of Solid State Electrochemistry Fig. 16 (a) The first charge-specific capacity and discharge-specific capacity at the current density of 0.1 C. (b) The cycle performance and coulombic efficiency of pristine and MgO-coated. Reproduced with permission [25], copyright, 2019, Journal of Solid State Electrochemistry J Solid State Electrochem more difficult. ...
LiNi0.8Co0.1Mn0.1O2 (NCM811), as one of the most promising cathode materials for lithium ion batteries, has gained a huge market with its obvious advantages of high energy density and low cost. It has become a competitive material among various cathode materials. However, in NCM811, the phenomenon of “cationic mixed discharge” is serious, resulting the cyclic performance performing badly. In addition, the thermal stability of ternary material will also be poor with the increase of nickel when temperature is high. In view of the above-mentioned situation, researchers come up with different methods to modify LiNi0.8Co0.1Mn0.1O2 by doping and coating to reduce mixing effect and improve its electrochemical performance. Here, we sketch out the structure, properties, and existing problems of NCM811 and summarize some cutting-edge modification methods. Finally, the development direction and commercial application of NCM811 cathode materials are prospected to accelerate its commercialization process.
