Skip to main content
NCBI home page
ACS Omega logoLink to ACS Omega
. 2025 Apr 1;10(14):14508–14513. doi: 10.1021/acsomega.5c01281

Reduced Graphene Oxide/LiMgPO4 Double Layer-Coated Li-Rich 0.4Li2MnO3·0.6LiMn1/3Ni1/3Co1/3O2 for High Performance Cathode

Fengying Wang 1,*, Wanxi Wang 1
PMCID: PMC12004286  PMID: 40256503

Abstract

graphic file with name ao5c01281_0005.jpg

Lithium-rich layered oxides (LLOs) have emerged as highly promising cathode materials for lithium-ion batteries due to their high specific capacity and cost-effectiveness. However, structural changes, oxygen release, and transition metal dissolution during cycling lead to irreversible voltage decay and capacity degradation, posing significant challenges for their practical application. While surface coatings with metal oxides offer partial mitigation, their poor electronic conductivity compromises rate capability and cycle stability. To tackle this challenge, we introduce an innovative dual-layer coating strategy by sequentially coating LLO (Li1.2Mn0.6Ni0.2Co0.2O2) particles with an ion-conductive LiMgPO4 (LMP) inner layer and a conductive reduced graphene oxide (rGO) outer layer. The LMP layer mitigates electrolyte-induced side reactions, while the rGO layer enhances electron transport, synergistically improving the performance. This synergistic design enables the optimized LLO@LMP@rGO cathode to achieve 80% capacity retention after 200 cycles at 1 C (vs 31% for pristine LLO) and an impressive high-rate capacity of 145 mA h g–1 at 8 C. The straightforward fabrication process, involving coprecipitation and thermal reduction, underscores its scalability for industrial production. Our work not only offers a viable pathway to enhance LLO cathodes but also inspires interfacial engineering strategies for advanced battery systems.

1. Introduction

The rapid development of electric vehicles and grid-scale renewable energy storage systems has imposed unprecedented demands on lithium-ion batteries (LIBs), particularly in terms of energy density and cost-effectiveness, which are crucial for the global transition toward sustainable energy solutions.1−3 As the core component of LIBs, cathode materials largely determine the battery’s energy ceiling. Among various candidates, lithium-rich layered oxides (LLOs) have emerged as the promising candidates due to their exceptional theoretical specific capacities and cost-effectiveness derived from manganese-rich compositions.4−6 However, the practical implementation remains hindered by critical challenges: (1) large irreversible capacity loss during the first cycle due to oxygen release,7,8 (2) severe capacity fading caused by transition metal (TM) dissolution and structural degradation,9,10 and (3) gradual voltage decay associated with phase transitions from layered to spinel-like structures.11,12 These issues stem from the inherent instability of oxygen redox chemistry, surface parasitic reactions with electrolytes, and cation migration during cycling.

To address these limitations, extensive efforts have been focused on surface modification strategies. Conventional approaches include elemental doping (e.g., Al, Mg, and F) to stabilize the lattice,13−16 electrolyte additives to suppress interfacial side reactions,17,18 and protective coatings to inhibit TM dissolution. Among these, surface coatings (e.g., Al2O3 and CeF3) have shown particular promise.19−21 Nevertheless, most oxide coatings suffer from poor electronic conductivity, inevitably increasing interfacial resistance and compromising the rate capability. This creates a fundamental dilemma: How can one simultaneously ensure ionic transport efficiency and electronic conductivity at the cathode–electrolyte interface?

Despite considerable progress in surface modification strategies, including doping, electrolyte additives, and protective coatings, a significant gap remains in simultaneously achieving high ionic and electronic conductivity at the cathode–electrolyte interface. Here, we introduce an innovative double-layer coating strategy that resolves this challenge by integrating an ionic conductor inner layer (LMP) with a highly conductive outer layer (grow). This unique approach not only addresses the inherent limitations of LLOs but also sets a new benchmark for future material design in advanced battery technologies.

The ionic conductor inner layer, LMP, is formed on the pristine LLO particles by a facile coprecipitation method. Then, a reduced graphene oxide (rGO) layer, which was thermally reduced from a GO layer, was applied to the LMP-modified LLO particles to improve their electronic conductivity. rGO films are widely believed to be a good electronic conducting two-dimensional material.22,23 Benefiting from the synergistic effect of the LMP protecting layer and the rGO layer, the modified LLOs exhibit dramatically enhanced electrochemical performance. By simultaneously optimizing the thickness of the LMP layer and the rGO layer, an LLO@LMP@rGO-based half-cell delivers an average capacity retention of 80% after 200 cycles at 1 C (250 mA g–1) with respect to its initial discharge capacity (208 mA h g–1), while the pristine material shows a much lower retention of only 31%. Meanwhile, the modified LLO materials show a dramatically improved rate capacity owing to the conductive rGO outer layers. Our results demonstrate a marked improvement in both cycle stability and rate capability, highlighting the potential of our method to facilitate the commercialization of LLOs for next-generation LIBs.

2. Materials and Methods

2.1. Materials

All of the chemical reagents were purchased from Sinopharm (Beijing, China).

2.2. Synthesis of LLO Particles

A coprecipitation method was used to prepare LLO precursors. MnSO4·H2O (1.014 g), NiSO4·6H2O (0.5257 g), and CoSO4·7H2O (0.5662 g) were added to 50 mL of water while continuously stirring, subsequent to which 25 mL of ethanol was added. After 1 h, an aqueous solution containing NH4HCO3 (0.8295 g) as a precipitant was gradually added to the solution as it was stirred. The solution’s temperature was maintained at 27 °C during the coprecipitation reaction. The resulting precipitant was separated using a centrifuge, washed thrice, and dried at 60 °C. The dried precipitant was then thoroughly mixed with LiOH·H2O (5% surfeit of lithium) and calcined in normal air at 800 °C for 5 h. Lastly, a black powder comprising pristine LLO particles was obtained.

2.3. Synthesis of LLO@LMP Particles

In this work, the pristine LLO particles were coated with different thickened LMP layers with LMP to LLO mass ratios fixed at 0.01, 0.02, and 0.03. Then, 0.5 g of prepared LLO particles were dispersed in 15 mL PVP solution (K 30, 1 g/mL) and stirred for 2 h. Subsequently, Mg(NO3)2·6H2O (10.5, 21.0, and 31.5 mg, respectively) was added to the solution, and NH4H2PO4 (4.8, 9.6, and 14.4 mg, respectively) was added after 15 min. Next, the solution was stirred for another 5 h at 60 °C. The resulting precipitant was separated using a centrifuge and then washed thrice and dried at 60 °C. Following this, CH3COOLi (3.1, 6.2, and 9.3 mg, respectively) was mixed with the precipitant and then sintered at 450 °C for 5 h under an argon atmosphere with a heating rate maintained at 2 °C/min. Lastly, LMP-coated LLO powders were obtained.

2.4. Synthesis of LLO@LMP@rGO Particles

In this work, the rGO coating amount was fixed at a mass ratio of GO to LLO@LMP of 0.005. Then, 0.01 g of PVP (K 30) was dispersed in 30 mL of deionized water and stirred for 30 min, subsequent to which 0.2 g of LLO@LMP powder was added to the PVP solution and stirred for another 10 min. The resulting solution was named solution A. Meanwhile, 0.541 mL of a GO solution (1.85 mg/mL) was added to 20 mL of deionized water to obtain a diluted GO solution that was named solution B. Subsequently, solution B was added to solution A, and the mixed solution was stirred for 10 min, following which the mixed solution was transferred to a bain-marie at 60 °C for 2 h. The particles in the solution were then separated, washed, and dried (at 80 °C for 12 h). The dried powder was then calcined at 400 °C for 5 h under an argon atmosphere to reduce the GO coating layers. The rate of heating was maintained at 2 °C/min. Lastly, rGO-coated LLO@LMP LLO powders were obtained.

2.5. Material Characterizations

Field-emission scanning electron microscopy (SEM) images were obtained from Zeiss Sigma SUPRA-55(Carl Zeiss AG, Germany). Transmission electron microscopy (TEM) images were obtained from SUPRA-55 (Carl Zeiss AG, Germany). X-ray diffraction (XRD) measurements were conducted on a Rigaku Ultima VI (Rigaku, Tokyo, Japan) instrument with a Cu/K α source. X-ray photoelectron spectroscopy (XPS) curves were collected with a JEM-2100 instrument (JEOL, Japan).

2.6. Electrochemical Characterizations

Half-cells were fabricated for electrochemical tests. Typically, active material (80 wt %), acetylene black (10 wt %), and polyvinylidene fluoride (10 wt %) were mixed to form the slurry for cathode electrodes. The uniform slurry was then cast onto aluminum foil by the doctor blading method, achieving an electrode thickness of 150 μm, which was then kept in a vacuum oven at 80 °C for 12 h. The aluminum foil with active film was then punched to discs (12 mm) with the mass loading of active materials as approximately 1.3–1.6 mg cm–2. The electrolyte was obtained from CAPCHEM (Shenzhen, China). The separator was purchased from Clegard (Clegard 2400, America). The counter electrode was a metal Li plate. The devices were fabricated in an argon-filled glovebox, MB-10-G-V2A (M.Braun Inertgas-Systeme, GmbH, Germany).

Cycling and rate performance were measured on a Neware CT-4008 tester (Shenzhen, China). The charge and discharge voltage ranges are 2.0–4.8 V. Electrochemical impedance spectroscopy (EIS) was obtained from a CHI660E electrochemical workstation (Chenhua, Shanghai, China). The voltage amplitude and the frequency range for EIS measurements were 5 mV and 0.01 Hz–100 kHz, respectively.

3. Results and Discussion

The detailed experimental procedure is given in the Supporting Information. Figure 1a illustrates the synthesis routines of pristine LLO particles and modified LLO particles. The typical mass ratio of the LMP layer to LLO particles is 2%. For convenience, the 2% LMP-coated LLOs are noted as LLO@LMP. In the case of rGO coating, a rGO layer is obtained by thermal reduction of a GO conformal layer whose mass is 0.5% of the underneath LLO@LMP cores. The LLO@LMP particles with rGO coating are noted as LLO@LMP@rGO. The morphologies of pristine LLO particles, LLO@LMP particles, and LLO@LMP@rGO particles are shown in Figure 1b–d by SEM. It can be seen from Figure 1b that the pristine LLO particles, with diameters ranging from 1 to 3 μm, are composed of nanometer-sized primary particles of tens of nanometers, which is beneficial for a high-performance cathode. With the coating of the LMP layer, the modified LLO particles get smoother, as shown in Figure 1c. Further coating the LLO@LPM with a rGO layer results in a much more smoother surface, owing to the intrinsic two-dimensional morphology of intrinsic graphene materials.

Figure 1.

Figure 1

Open in a new tab

(a) Schematic images of the pristine LLO particle, LLO@LMP particle, and LLO@LMP@rGO particle. SEM images of (b) the pristine LLO particles, (c) the LLO@LMP particles, and (d) the LLO@LMP@rGO particles. TEM images of (e–g) the LLO@LMP particles and (h–j) the LLO@LMP@rGO particles.

TEM was used to determine the coating of the LMP layer and the rGO layer, presented in Figure 1e–j. A several nanometer thick layer can be observed in Figure 1f from a LLO@LMP particle, which means an effective coating of an ultrathin LMP layer. The details of the interface between the LLO and LMP are presented in Figure 1g. It can be seen that the well-ordered lattice fringes belong to the highly crystallized LLO particles with the typical (003) plane.24,25 Meanwhile, the enlarged image shows that the LMP layer is nonuniform and is composed of an ultrafine LMP layer, as shown in Figure 1g. The lattice fringes within the coating layer correspond to the (221) plane of the olivine structure.18 Similarly, an ultrathin rGO coating layer can be observed on the surface of a LLO@LMP@rGO particle, as shown in Figure 1h,i. In Figure 1j, the characteristic fringes can be easily distinguished, which belong to LLO, LMP, and rGO, respectively. The thickness of the rGO layer is approximately 3.5 nm. It can be concluded that the LLO surface is well protected by LMP and rGO simultaneously. The EDS mapping of the C and Mg elements for LLO@LMP@rGO particles is also shown in Figure S1 (Supporting Information), which reconfirms the well coating of the LMP and rGO double layer on the LLO surface. Moreover, the LMP particle is witnessed to fill in the void between two adjacent LLO particles, which no doubt explains the smoother surface of the LLO@LMP particles in Figure 1c.

XRD measurements were performed to inspect whether there was any crystal phase difference between pristine LLO particles and modified LLO particles. The results are shown in Figure 2a. It can be seen that the XRD pattern of the LLO is similar to that of the LLO@LMP, indicating that the crystal phase is well maintained after the LMP coating. Both samples show a typical hexagonal α-NaFeO2 structure in the R3m space group. However, the LMP phase is not observed from the XRD pattern of the LMP-coated sample, which might be owing to the low content of LMP. While further coating the LLO@LMP with rGO, additional peaks belonging to the spinel LiMn2O4 phase can be seen in the XRD pattern in Figure 2a. It is speculated that the coating GOs would react with the oxygen from the inner particles at a high temperature during the thermal reduction of GOs, leading to a slight phase transformation.

Figure 2.

Figure 2

Open in a new tab

(a) XRD patterns of the pristine LLO particles and modified LLO particles and (b–f) high-resolution XPS features of different elements in the pristine LLO particles and modified LLO particles.

To confirm the speculation, XPS was used to monitor the evolution of the elemental chemical states in different LLOs, which can reflect the change of oxygen ions. As shown in Figure 2b–d, the chemical states of metal ions, Mn, Ni, and Co, have been changed. The detailed contents of different states for Mn, Ni, and Co are summarized in Figure 2e. It can be seen that the coating of the LMP layer barely affects the chemical state of transient metals. When annealed at high temperatures during the thermal reduction of GO coatings, the transient metals are partly reduced. It is owing to the reaction between oxygen from LLO@LMP particles and carbon from the GO, which would further lead to the formation of the spinel phase indicated in Figure 2a.4,26,27 Further study is needed to confirm that. Despite this, the formation of the spinel phase is favorable for the improved stability of cathode materials against those side reactions with the electrolyte.

The electrochemical performances of the pristine LLO and modified LLOs were systematically studied in coin half-cells using Li metal as an anode electrode. The initial charge and discharge specific capacities of the three samples are shown in Figure 3a. The pristine LLO shows a higher charge capacity of 398 mA h g–1 but a lower discharge capacity of 253 mA h g–1 with a poor initial Coulombic efficiency (iCE) of 63.5%. With the coating of the LMP layer (wt 2%), the charge capacity is slightly decreased, and the discharge capacity is increased with an enhanced iCE of 68.3%. (The dependence of device performance on different LMP amounts is given in Figure S5.) Such enhancement is ascribed to the improved lithium utilization and the reduced activity of lattice oxygen.28 When applying a double-layer coating, the iCE is increased to 80.9%. The decreased charge capacity and discharge capacity of LLO@LMP@rGO are ascribed to the reduced Li2O during the activation process. The voltage decay of modified LLO is also greatly suppressed, as shown in Figure 3b. The detailed values are given in Table S1. It can be seen that the LLO@LMP@rGO shows the lowest voltage decay as 3.8 mV per cycle, which proves the superiority of the double-layer coating.

Figure 3.

Figure 3

Open in a new tab

(a) LLOs initial charge and discharge curves (2.0–4.8 V, 0.1 C), (b) voltage decay curves of different LLOs (2.0–4.8 V, 1 C), and (c) cycling performance (2.0–4.8 V, 1 C) of modified-LLOs based half cells. (d) Rate performance of different LLOs.

The circle stability of the pristine LLO and modified LLO materials is also evaluated, which is normally associated with side reactions between cathode materials and electrolytes. As shown in Figure 3c, LLO@LMP and LLO@LMP@rGO show capacity retentions of 62 and 80% after 200 cycles at 1 C (1 C = 250 mA g–1), which is much higher than 30.4% for pristine LLO. Rate performance is also an important factor for high-performance cathode materials, which is greatly affected by the electronic conductivity of the materials. Figure 3d shows the rate performances of different LLOs. It can be seen that the modifying layers, LMP and LMP@rGO, are beneficial for the improved rate capacities. The LLO@LMP@rGO retains 65.04% of its initial capacity (145 mA h g–1) at 8 C and is far higher than that of the pristine LLO as 31.3%. Such improvement might originate from two aspects: enhanced ionic conductivity by LMP and increased electronic conductivity by the rGO layer. Our results are outstanding among the reports on the LLO-based cathode materials synthesized by the coprecipitation method.

In order to unravel the mystery of the improved rate performance, EIS was carried out. As shown in Figure 4a, with the addition of the LMP layer or LMP@rGO layer, the semicircle in the high-frequency region, representing the interfacial charge-transfer resistance, is decreased, which hints that the interfacial side reactions are reduced by the LMP layer or LMP@rGO layer. The linear part of the curves at low frequency represents the diffusion of Li+ within the cathodes, named Warburg impedance, which can be calculated by fitting the linear relationship between the real part of the impedance, Zr, and ω–1/2 at the low frequency zone.29 As shown in Figure 4b, the slope of the fitting lines, named as the Warburg factor, decreases compared with that of the control sample. The diffusion coefficients of Li ions in pristine LLO, LLO@LMP, and LLO@LMP@rGO are 6.99 × 10–16, 9.85 × 10–16, and 1.48 × 10–15 cm2 s–1, respectively. Obviously, the double-layer coating can significantly improve the diffusion of Li ions within the modified LLOs. Such enhancement is ascribed to the improved ionic conductivity by the LMP layer and the improved electronic conductivity by the rGO layer. The results strongly support the superiority of our strategy to modify the LLO surface.

Figure 4.

Figure 4

Open in a new tab

(a) EIS spectra of pristine LLO and coated LLO-based half cells. (b) Dependence of the real part of Zre on the ω–1/2 at low frequency.

4. Conclusions

In conclusion, a novel double-layer coating was successfully applied to LLO cathode materials to improve their electrochemical performance. The LMP layer uniformly coats the LLO particles and fills in the voids between them. This effectively protects the LLO particles from electrolyte erosion. Additionally, when GO was added to the LMP surface and subsequently annealed, not only was a thin rGO layer obtained but also a minor amount of the spinel phase was observed. The resulting double-layer structure significantly enhances the stability of LLO particles during cycling while simultaneously improving electronic conductivity. These two beneficial effects undoubtedly contribute to the improved electrochemical performance of the LLOs. Specifically, the rGO@LMP@LLO-based cathode demonstrated an average capacity retention of 80% after 200 cycles at 1 C (with respect to its initial discharge capacity) and exhibited an outstanding rate capability with a discharge capacity of 145 mA h g–1 even at 8 C. Our method offers a scalable and effective approach for enhancing LLO cathode materials, with potential applications in next-generation LIBs.

Acknowledgments

This work was supported by Qinghai Provincial Science and Technology Plans (Grant No. 2023-ZJ-722 and Grant No. 2017-ZJ-750) and Qinghai Minzu University 2024 University-Level Innovation and Entrepreneurship Courses

Supporting Information Available

The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acsomega.5c01281.

  • Elemental mapping results of Mg and C distributions in LLO@LMP and LLO@LMP@rGO composite particles; X-ray diffraction patterns of LLO@LMP samples with varying LMP coating thicknesses; X-ray photoelectron spectroscopy spectra of pristine LLO, LLO@LMP, and LLO@LMP@rGO materials; high-resolution XPS spectra of characteristic elements in both unmodified and modified LLO samples; the electrochemical performance of modified LLO half-cells; and the discharge performance characteristics of cathode materials synthesized via the coprecipitation method (PDF)

The authors declare no competing financial interest.

Supplementary Material

ao5c01281_si_001.pdf (694.6KB, pdf)

References

  1. Han X.; Lu L.; Zheng Y.; Feng X.; Li Z.; Li J.; Ouyang M. A review on the key issues of the lithium ion battery degradation among the whole lifecycle. eTransportation 2019, 1, 100005 10.1016/j.etran.2019.100005. [DOI] [Google Scholar]
  2. Yalçin A.; Guler M. O.; Demir M.; Gönen M.; Akgün M. Enhanced Cycling Stability of Al-Doped Li1.20Mn0.52-xAlxNi0.20Co0.08O2 as a Cathode Material for Li-Ion Batteries by a Supercritical-CO2-Assisted Method. ACS Omega 2024, 9, 46813–46821. 10.1021/acsomega.4c05087. [DOI] [PMC free article] [PubMed] [Google Scholar]
  3. Dunn B.; Kamath H.; Tarascon J. Electrical Energy Storage for the Grid: A Battery of Choices. Science 2011, 334, 928–935. 10.1126/science.1212741. [DOI] [PubMed] [Google Scholar]
  4. Xia Q. B.; Zhao X. F.; Xu M. Q.; Ding Z. P.; Liu J. T.; Chen L. B.; Ivey D. G.; Wei W. F. A Li-rich Layered@Spinel@Carbon Heterostructured Cathode Material for High Capacity and High Rate Lithium-ion Batteries Fabricated via an in situ Synchronous Carbonization-reduction Method. J. Mater. Chem. A 2015, 3, 3995–4003. 10.1039/C4TA05848H. [DOI] [Google Scholar]
  5. Xie Y.; Jin Y.; Xiang L. Li-rich layered oxides: Structure, capacity and voltage fading mechanisms and solving strategies. Particuology 2022, 61, 1–10. 10.1016/j.partic.2021.05.011. [DOI] [Google Scholar]
  6. Jang H. Y.; Eum D.; Cho J.; Lim J.; et al. Structurally robust lithium-rich layered oxides for high-energy and long-lasting cathodes. Nat. Commun. 2024, 15, 1288. 10.1038/s41467-024-45490-x. [DOI] [PMC free article] [PubMed] [Google Scholar]
  7. Jin Y. L.; Zhao Z. R.; Ren P. G.; Zhang B. F.; Chen Z. Y.; Guo Z. Z.; Ren F.; Sun Z. F.; Liu S. H.; Song P.; Yang H. J.; Xu K. H.; Li X. F. Recent Advances in Oxygen Redox Activity of Lithium-Rich Manganese-Based Layered Oxides Cathode Materials: Mechanism, Challenges and Strategies. Adv. Energy. Mater. 2024, 14, 2402061. 10.1002/aenm.202402061. [DOI] [Google Scholar]
  8. Yin W.; Grimaud A.; Rousse G.; Abakumov A. M.; Senyshyn A.; Zhang L.; Trabesinger S.; Iadecola A.; Foix D.; Giaume D.; Tarascon J. M. Structural evolution at the oxidative and reductive limits in the first electrochemical cycle of Li1.2Ni0.13Mn0.54Co0.13O2. Nat. Commun. 2020, 11, 1252. 10.1038/s41467-020-14927-4. [DOI] [PMC free article] [PubMed] [Google Scholar]
  9. He W.; Guo W. B.; Wu H. L.; Lin L.; Liu Q.; Han X.; Xie Q. S.; Liu P. F.; Zheng H. F.; Wang L. S.; Yu X. Q.; Peng D. L. Challenges and Recent Advances in High Capacity Li-Rich Cathode Materials for High Energy Density Lithium-Ion Batteries. Adv. Mater. 2021, 33, 2005937. 10.1002/adma.202005937. [DOI] [PubMed] [Google Scholar]
  10. Xie H.; Xiao J.; Chen H.; Zhang B.; Hui K.; Zhang S.; Liu C.; Luo D.; Lin Z. Fundamental understanding of voltage decay in Li-rich Mn-based layered oxides cathode materials. AAPPS Bull. 2024, 34, 33. 10.1007/s43673-024-00138-2. [DOI] [Google Scholar]
  11. Pechen L.; Makhonina E.; Rumyantsev A.; Koshtyal Y.; Goloveshkin A.; Volkov V.; Politov Y.; Eremenko I. Synthesis and electrochemical performance of Li-rich xLi2MnO3•(1-x)LiMn1/3Ni1/3Co1/3O2 (x = 0.2–0.5) cathode materials for lithium-ion batteries. Mater. Sci. Eng. 2019, 525, 012042 10.1088/1757-899X/525/1/012042. [DOI] [Google Scholar]
  12. Liu Z.; Zeng Y.; Tan J.; et al. Revealing the degradation pathways of layered Li-rich oxide cathodes. Nat. Nanotechnol. 2024, 19, 1821–1830. 10.1038/s41565-024-01773-4. [DOI] [PubMed] [Google Scholar]
  13. Lei T. W.; Yang Y. Q.; He H.; Liang T. Q. F-ion doping enhance the cycling stability of Li1.2Mn0.54Ni0.13Co0.13O2 cathode in lithium battery. Inorg. Chem. Commun. 2025, 173, 113857 10.1016/j.inoche.2024.113857. [DOI] [Google Scholar]
  14. Guo L.; Ren L.; Wan L.; Li J. Heterogeneous carbon/N-doped reduced graphene oxide wrapping LiMn0.8Fe0.2PO4 composite for higher performance of lithiumion batteries. Appl. Surf. Sci. 2019, 476, 513–520. 10.1016/j.apsusc.2018.12.227. [DOI] [Google Scholar]
  15. Li Y.; Zhao Q.; Zhang M. K.; Qiu L.; Zheng Z.; Liu Y.; Sun Y.; Zhong B. H.; Song Y.; Guo X. D. Fabricating Heterostructures for Boosting the Structure Stability of Li-Rich Cathodes. ACS Omega. 2023, 8 (7), 6720–6728. 10.1021/acsomega.2c07313. [DOI] [PMC free article] [PubMed] [Google Scholar]
  16. Xu Y.; Xiang W.; Wu Z.; Xu C.; Li Y.; Guo X.; Lv G.; Peng X.; Zhong B. Improving cycling performance and rate capability of Ni-rich LiNi0.8Co0.1Mn0.1O2 cathode materials by Li4Ti5O12 coating. Electrochim. Acta 2018, 268, 358–365. 10.1016/j.electacta.2018.02.049. [DOI] [Google Scholar]
  17. Jiang B.; Li H.; Luo B.; Liu L.; Chu L.; Zhang Q.; Li M. Vinyltrimethylsilane as a novel electrolyte additive for improving interfacial stability of Li-rich cathode working in high voltage. Chin. Chem. Lett. 2024, 35, 108649 10.1016/j.cclet.2023.108649. [DOI] [Google Scholar]
  18. Li J.; Xing L.; Zhang L.; Yu L.; Fan W.; Xu M.; Li W. Insight into self-discharge of layered lithium-rich oxide cathode in carbonate-based electrolytes with and without additive. J. Power Sources. 2016, 324, 17–25. 10.1016/j.jpowsour.2016.05.074. [DOI] [Google Scholar]
  19. Yang F.; Li Y. L.; Wang Z.; Chen C. G.; Guo Z. M. Preparation and coating modification of lithium-rich layered oxides Li1.2Mn0.54Ni0.13Co0.13O2 via Al2O3. J. Appl. Electrochem. 2023, 53 (1), 1–8. 10.1007/s10800-022-01752-4. [DOI] [Google Scholar]
  20. Bei Y. Y.; Zhang Y.; Li Y. Y.; Song Y.; Liu L.; Ma J. J.; Liu J. Controlled preparation of nano-Al2O3/PPy composite coatings to compensate surface structural defects of lithium-rich layered oxides. J. Alloys Compd. 2022, 928, 167140 10.1016/j.jallcom.2022.167140. [DOI] [Google Scholar]
  21. Ji X.; Dai X.; Wu F.; Jin H. Liquid-Phase Integrated Surface Modification to Construct Stable Interfaces and Superior Performance of High-Voltage LiNi0.5Mn1.5O4 Cathode Materials ACS Sustainable. Chem. Eng. 2022, 10 (30), 9850–9859. 10.1021/acssuschemeng.2c01711. [DOI] [Google Scholar]
  22. Xia W. C.; Zheng Z.; Zhou L.; Sun J. T.; Bei F. L. A novel coating strategy for graphene-modified Li1.2Mn0.54Ni0.13Co0.13O2 as cathode material for LIBs. Int. J. Electrochem. Sci. 2023, 18 (10), 100280 10.1016/j.ijoes.2023.100280. [DOI] [Google Scholar]
  23. Luo D.; Fang S.; Yang L.; Hirano S. In-situ preparation of novel layered-spinel-microsphere/reduced-graphene-oxide heterostructured cathode for ultrafast charge-discharge Li-ion batteries. ChemSusChem 2017, 10 (22), 4845–4850. 10.1002/cssc.201701207. [DOI] [PubMed] [Google Scholar]
  24. Zhou L. J.; Yin Z. L.; Ding Z. Y.; Li X. H.; Wang Z. X.; Wang Y. Bulk and surface reconstructed Li-rich Mn-based cathode material. J. Electroanal. Chem. 2018, 829, 7–15. 10.1016/j.jelechem.2018.09.043. [DOI] [Google Scholar]
  25. Zou W.; Xia F. J.; Song J. P.; Wu L.; Chen L.; Chen H.; Liu Y.; Dong W.; Wu S.; Hu Z.; Liu J.; Wang H.; Chen L.; Li Y.; Peng D.; Su B. Probing and suppressing voltage fade of Li-rich Li1.2Ni0.13Co0.13Mn0.54O2 cathode material for lithium-ion battery. Electrochim. Acta 2019, 318, 875–882. 10.1016/j.electacta.2019.06.119. [DOI] [Google Scholar]
  26. Pei Y.; Xu C.; Xiao Y.; Chen Q.; Huang B.; Li B.; Li S.; Zhen L.; Cao G. Phase transition induced synthesis of layered/spinel heterostructure with enhanced electrochemical properties. Adv. Funct. Mater. 2017, 27 (7), 1604349 10.1002/adfm.201604349. [DOI] [Google Scholar]
  27. Ku L.; Cai Y.; Ma Y.; Zheng H.; Liu P.; Qiao Z.; Xie Q.; Wang L.; Peng D. Enhanced electrochemical performances of layered-spinel heterostructured. Chem. Eng. J. 2019, 370, 499–507. 10.1016/j.cej.2019.03.247. [DOI] [Google Scholar]
  28. Liu P.; Zhang H.; He W.; Xiong T.; Cheng Y.; Xie Q.; Ma Y.; Zheng H.; Wang L.; Zhu Z.; Peng Y.; Mai L.; Peng D. Lithium deficiencies engineering in Li-rich layered oxide Li1.098 Mn0.533Ni0.113Co0.138O2 for high-stability cathode. J. Am. Chem. Soc. 2019, 141 (27), 10876–10882. 10.1021/jacs.9b04974. [DOI] [PubMed] [Google Scholar]
  29. He W.; Zheng H.; Ju X.; Li S.; Ma Y.; Xie Q.; Wang L.; Qu B.; Peng D. Multistage Li1.2Ni0.2Mn0.6O2 micro-architecture towards high-performance cathode materials for lithium-ion batteries. ChemElectroChem. 2017, 4 (12), 3250–3256. 10.1002/celc.201700727. [DOI] [Google Scholar]

Associated Data

This section collects any data citations, data availability statements, or supplementary materials included in this article.

Supplementary Materials

ao5c01281_si_001.pdf (694.6KB, pdf)

Articles from ACS Omega are provided here courtesy of American Chemical Society

RESOURCES