Surface engineering of LiNi0.8Mn0.1Co0.1O2 towards boosting lithium storage: Bimetallic oxides versus monometallic oxides

doi:10.1016/j.nanoen.2020.105034

Nano Energy

Volume 77, November 2020, 105034

https://doi.org/10.1016/j.nanoen.2020.105034 Get rights and content

Highlights

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A multi-functional bimetallic oxide coating was designed for NCM811 cathode.
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Bimetallic oxide coating shows the best modification performance.
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Bimetallic oxide coating balances all advantages of each monometallic oxide.

Abstract

Although conventional monometallic oxide coating on lithium nickel cobalt manganese oxide (NCM) cathode materials has been extensively investigated, there are still many issues, such as low electrical conductivity, poor mechanical properties and inferior chemical stability, that need to be addressed. Indeed, because of the single nature of monometallic oxides, it is difficult to achieve the synergistic effect of various properties. In this work, NiCo₂O₄ were rationally grown on the surface of commercial LiNi_0.8Mn_0.1Co_0.1O₂ (NCM811) to obtain a bimetallic oxide coated NCM811 as cathode material for Lithium ion batteries (LIBs). This cleverly designed coating with a higher electronic and ionic conductivity, better bulk modulus, and an outstanding interfacial stability, could improve the capacity retention to 90.97% after 200 cycles at 100 mA g⁻¹ and enhance the initial coulombic efficiency (CE) to 82.92%. The electrochemical characterization further clarifies the indisputable benefits of NiCo₂O₄ coating to enhancement of the cathode performance. Moreover, the theoretical calculations provide more explanations in three aspects, including mechanical stability, chemical stability and electrical properties, confirming the superiority of NiCo₂O₄ bimetallic oxide coating with multiple properties over the monometallic one. More importantly, this study has profound implications in the design of bimetallic and polymetallic oxide coatings for electrode materials, and even other bimetallic coatings, such as sulfides and selenides, in the future.

Graphical abstract

Introduction

The energy crisis is becoming a globally daunting issue due to the increasing demand for energy and the depletion of traditional fossil fuels, leading to a destructive impact on the environment. In order to solve this contradiction, great efforts have been made to develop green and sustainable energy sources, among which electrochemical storage and conversion technologies have proven to be very effective. Since the commercialization in 1991, LIBs have gradually shown great advantages in their application, occupying the largest market share among the rechargeable batteries. Because of the high energy, long cycle-life and other advantages, they have been widely employed in electric vehicles, grid energy storage, and electronic devices [1,2]. The performance of full batteries strongly depends on cathode materials, which are more difficult to develop and more expensive to produce than the widely used graphite or other more advanced anode materials [3,4]. Accordingly, Ni-rich NCM (LiNi_xMn_yCo_1-x-yO₂, 0.6 < x < 1, 0 < y < 0.2) originated from partial cation substitution of Ni atoms in LiNiO₂, is considered as a promising candidate because of its large capacity and low manufacturing cost compared to conventional LiFePO₄ and LiCoO₂ cathodes [[5], [6], [7], [8]]. However, Ni-rich NCM cathodes suffer from various types of electrochemical degradation phenomena such as cation disorder, phase transformation, and side reaction at the electrolyte-electrode interface, which are significant barriers for their further large-scale application and commercialization [[8], [9], [10], [11], [12]].

Surface coating is an efficient method to alleviate the degradation behaviors in Ni-rich NCMs by providing a physical barrier on the surface, which prevents the direct contact between the electrode and electrolyte [13]. For example, metal oxides such as Al₂O₃ [14,15], Co₃O₄ [16,17], SiO₂ [18], TiO₂ [19], ZnO [20] and WO₃ [21] are demonstrated to be successfully effective in improving the capacity retention of the layered cathode materials during electrochemical cycling. Metal phosphates [22], fluorides [23] and conducting polymers [24] are also popular and broadly applied as coating materials. In addition, for boosting the Li⁺ diffusion at the interface, Li-containing materials such as LiAlO₂ [25], Li₂MnO₃ [26,27], Li₂TiO₃ [28], Li₂ZrO₃ [29] and LiNbO₃ [30] have been investigated, exhibiting great rate capability and improved cycle-life. Among the various coating materials, oxides are the most widely studied and applied in both academia and industry. In spite of their great functionality, the aforementioned approaches have several drawbacks because the coating materials typically result in a lower initial capacity compared to the uncoated electrodes [31]. Another critical concern is the poor electronic and ionic conductivities of some coating layers, which may have a negative effect on the electrochemical kinetics of NCMs. Hence, the coating layer as a physical barrier with positive effects can simultaneously act as an electrochemical obstacle with negative effects. Hence, designing a multifunctional coating with both excellent physical and chemical properties is essential to achieve more efficient batteries.

Based on the critical aspects of surface coatings discussed above, an ideal coating material should possess the following functionalities: 1) excellent mechanical properties, buffering volume expansion during cycling; 2) high electronic and ionic conductivity, improving kinetics of extraction/insertion of Li⁺; 3) perfect chemical stability, reducing the erosion of cathode by electrolyte. Hence, in this work, a bimetallic oxide (i.e., NiCo₂O₄) as the coating layer for NCM811 is designed and compared with the monometallic oxides (i.e., NiO and Co₃O₄) and their mixture in order to achieve the above-mentioned modification effects and ameliorate the electrochemical performance of the cathode material. It also displays a high initial CE of 82.92% and a superb capacity retention of 90.97% after 200 cycles at 100 mA g⁻¹. Indeed, the theoretical calculations further verify the superior performance of the bimetallic oxide coating.

Section snippets

Material synthesis

Commercial NCM811 coated with NiCo₂O₄ was synthesized by a simple solvothermal method. In particular, 0.61 mg Ni(NO₃)₂·6H₂O, 1.21 mg Co(NO₃)₂·6H₂O and 0.29 mg HMTA, as a complexing agent, were dissolved into 40 mL ethanol, then transferred into a Teflon-lined stainless-steel autoclave which was sealed and kept at 120 °C for 12 h, and then cooled down to room temperature. The as-obtained black product was washed with ethanol several times, followed by drying at 90 °C for 1 h. The obtained black

Results and discussion

According to Fig. 1a, the XRD patterns of the pristine and coated NCM with different coatings all show the same diffraction peaks, perfectly matched LiNiO₂ (PDF # 89–3601), which is a typical layered structure transition metal (TM) oxide [34]. It indicates that the phases of NCM after coating via solvothermal method have not been changed, and perfectly maintained its original layered form. To confirm the phases of coating layers, the XRD test was conducted for each of them before coating the

Conclusions

In this work, bimetallic oxide coatings on NCM811 were proved to have a superior performance over monometallic oxides which were used as the control groups. Specifically, as a result of the coatings, the electrochemical characteristics achieved different levels of improvement, among which the bimetallic oxide Ni&Co-NCM displayed the best performance. Ni&Co-NCM delivered a high initial CE of 82.92% and a high capacity retention of 90.97% after 200 cycles at 100 mA g⁻¹. Among the coatings, NiCo₂O₄

Declaration of competing interest

This manuscript has not been published or presented elsewhere in part or in entirety and is not under consideration by another journal. All study participants provided informed consent, and the study design was approved by the appropriate ethics review boards. All the authors have approved the manuscript and agree with submission to your esteemed journal. There are no conflicts of interest to declare.

Acknowledgement

The authors gratefully acknowledge the financial support by the National Natural Science Foundation of China (51672189, 51772051 and 51801153), China Postdoctoral Science Foundation (2019M653705), Project 2019JPL-04 supported by Joint Foundation of Shaanxi, Natural Science Foundation of Shaanxi Province (2020JQ-638) and Xi'an Science and Technology Project of China (201805037YD15CG21(20)).

Quan Xu is currently a graduate student in the Institute of Advanced Electrochemical Energy at Xi'an University of Technology. He received B.S. degree in School of Materials Science and Engineering, Xi'an University of Technology in 2016. His research interests focus on the modification and application of cathode materials for lithium ion batteries.

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Xifei Li is currently a full professor at Xi'an University of Technology, and a fellow of Royal Society of Chemistry. He was awarded as 2018 & 2019 Highly Cited Researchers of Clarivate Analytics. He is an executive editor-in chief of Electrochemical Energy Reviews, a vice-president of International Academy of Electrochemical Energy Science, and a vice-director of Full Cell Engine Sub-society of Chinese Society of Internal Combustion Engines. Dr. Li's research group is working on optimized interfaces of the anodes and the cathodes with various structures for high performance rechargeable batteries. Dr. Li has authored/ co-authored 230 articles with 12000 citations.

Hirbod Maleki Kheimeh Sari is currently a Ph.D. candidate in the Institute of Advanced Electrochemical Energy at Xi'an University of Technology. He received his Master's degree from the College of Mechanical Engineering, Malaysia University of Technology in 2014. His research interests primarily focus on the design and synthesis of novel nanomaterials for energy storage, especially cathode materials for lithium/sodium ion batteries.

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Surface engineering of LiNi0.8Mn0.1Co0.1O2 towards boosting lithium storage: Bimetallic oxides versus monometallic oxides

Highlights

Abstract

Graphical abstract

Introduction

Section snippets

Material synthesis

Results and discussion

Conclusions

Declaration of competing interest

Acknowledgement

Nano Energy

J. Power Sources

Electrochim. Acta

J. Power Sources

J. Power Sources

Appl. Surf. Sci.

Electrochim. Acta

Mater. Lett.

Nano Energy

Solid State Ionics

Electrochim. Acta

J. Energy Chem.

J. Alloys Compd.

Electrochim. Acta

J. Power Sources

J. Alloys Compd.

The current move of lithium ion batteries towards the next phase

Adv. Energy Mater.

Challenges facing lithium batteries and electrical double-layer capacitors

Angew Chem. Int. Ed. Engl.

30 Years of lithium-ion batteries

Adv. Mater.

Nickel-rich layered lithium transition-metal oxide for high-energy lithium-ion batteries

Angew Chem. Int. Ed. Engl.

Intrinsic origins of crack generation in Ni-rich LiNi0.8Co0.1Mn0.1O2 layered oxide cathode

Mater. Sci. Rep.

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ACS Energy Lett.

Degradation mechanisms and mitigation strategies of nickel-rich NMC-based lithium-ion batteries

Electrochem. Energy Rev.

formation and inhibition of metallic lithium microstructures in lithium batteries driven by chemical crossover

ACS Nano

The impact of electrolyte additives and upper cut-off voltage on the formation of a rocksalt surface layer in LiNi0.8Mn0.1Co0.1O2 electrodes

J. Electrochem. Soc.

Surface engineering of LiNi_0.8Mn_0.1Co_0.1O₂ towards boosting lithium storage: Bimetallic oxides versus monometallic oxides

Intrinsic origins of crack generation in Ni-rich LiNi_0.8Co_0.1Mn_0.1O₂ layered oxide cathode

Structural and electrochemical aspects of LiNi_0.8Co_0.1Mn_0.1O₂ cathode materials doped by various cations

The impact of electrolyte additives and upper cut-off voltage on the formation of a rocksalt surface layer in LiNi_0.8Mn_0.1Co_0.1O₂ electrodes