Статті в журналах: "Ni-rich NMC"

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Li, Tianyu, Xiao-Zi Yuan, Lei Zhang, Datong Song, Kaiyuan Shi, and Christina Bock. "Degradation Mechanisms and Mitigation Strategies of Nickel-Rich NMC-Based Lithium-Ion Batteries." Electrochemical Energy Reviews 3, no. 1 (October 21, 2019): 43–80. http://dx.doi.org/10.1007/s41918-019-00053-3.

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Abstract The demand for lithium-ion batteries (LIBs) with high mass-specific capacities, high rate capabilities and long-term cyclabilities is driving the research and development of LIBs with nickel-rich NMC (LiNixMnyCo1−x−yO2, $$x \geqslant 0.5$$x⩾0.5) cathodes and graphite (LixC6) anodes. Based on this, this review will summarize recently reported and widely recognized studies of the degradation mechanisms of Ni-rich NMC cathodes and graphite anodes. And with a broad collection of proposed mechanisms on both atomic and micrometer scales, this review can supplement previous degradation studies of Ni-rich NMC batteries. In addition, this review will categorize advanced mitigation strategies for both electrodes based on different modifications in which Ni-rich NMC cathode improvement strategies involve dopants, gradient layers, surface coatings, carbon matrixes and advanced synthesis methods, whereas graphite anode improvement strategies involve surface coatings, charge/discharge protocols and electrolyte volume estimations. Electrolyte components that can facilitate the stabilization of anodic solid electrolyte interfaces are also reviewed, and trade-offs between modification techniques as well as controversies are discussed for a deeper understanding of the mitigation strategies of Ni-rich NMC/graphite LIBs. Furthermore, this review will present various physical and electrochemical diagnostic tools that are vital in the elucidation of degradation mechanisms during operation to supplement future degradation studies. Finally, this review will summarize current research focuses and propose future research directions. Graphic Abstract The demand for lithium-ion batteries (LIBs) with high mass specific capacities, high rate capabilities and longterm cyclabilities is driving the research and development of LIBs with nickel-rich NMC (LiNixMnyCo1−x−yO2, x ≥ 0.5) cathodes and graphite (LixC6) anodes. Based on this, this review will summarize recently reported and widely recognized studies of the degradation mechanisms of Ni-rich NMC cathodes and graphite anodes. And with a broad collection of proposed mechanisms on both atomic and micrometer scales, this review can supplement previous degradation studies of Ni-rich NMC batteries. In addition, this review will categorize advanced mitigation strategies for both electrodes based on different modifications in which Ni-rich NMC cathode improvement strategies involve dopants, gradient layers, surface coatings, carbon matrixes and advanced synthesis methods, whereas graphite anode improvement strategies involve surface coatings, charge/discharge protocols and electrolyte volume estimations. Electrolyte components that can facilitate the stabilization of anodic solid-electrolyte interfaces (SEIs) are also reviewed and tradeoffs between modification techniques as well as controversies are discussed for a deeper understanding of the mitigation strategies of Ni-rich NMC/graphite LIBs. Furthermore, this review will present various physical and electrochemical diagnostic tools that are vital in the elucidation of degradation mechanisms during operation to supplement future degradation studies. Finally, this review will summarize current research focuses and propose future research directions.

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Teichert, Philipp, Gebrekidan Gebresilassie Eshetu, Hannes Jahnke, and Egbert Figgemeier. "Degradation and Aging Routes of Ni-Rich Cathode Based Li-Ion Batteries." Batteries 6, no. 1 (January 22, 2020): 8. http://dx.doi.org/10.3390/batteries6010008.

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Driven by the increasing plea for greener transportation and efficient integration of renewable energy sources, Ni-rich metal layered oxides, namely NMC, Li [Ni1−x−yCoyMnz] O2 (x + y ≤ 0.4), and NCA, Li [Ni1−x−yCoxAly] O2, cathode materials have garnered huge attention for the development of Next-Generation lithium-ion batteries (LIBs). The impetus behind such huge celebrity includes their higher capacity and cost effectiveness when compared to the-state-of-the-art LiCoO2 (LCO) and other low Ni content NMC versions. However, despite all the beneficial attributes, the large-scale deployment of Ni-rich NMC based LIBs poses a technical challenge due to less stability of the cathode/electrolyte interphase (CEI) and diverse degradation processes that are associated with electrolyte decomposition, transition metal cation dissolution, cation–mixing, oxygen release reaction etc. Here, the potential degradation routes, recent efforts and enabling strategies for mitigating the core challenges of Ni-rich NMC cathode materials are presented and assessed. In the end, the review shed light on the perspectives for the future research directions of Ni-rich cathode materials.

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Yang, Zhijie, and Feng Lin. "Synthesis and Size Control of Single Crystal Ni-Rich Layered Oxide Cathodes Using Statistical Analysis-Guided Molten Salt Method." ECS Meeting Abstracts MA2022-02, no. 3 (October 9, 2022): 282. http://dx.doi.org/10.1149/ma2022-023282mtgabs.

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Rechargeable Li ion batteries have been widely applied in daily lives. The demand for Li ion batteries with higher energy density has been increasing especially with the thriving development of electric vehicles in the past decade. Li(Ni1−x−yMnxCoy)O2 (NMC) is one of the most successful commercial cathodes with various transition metal (Ni, Mn, and Co) ratios. Higher Ni content in the composition of NMC gives rise to higher energy density but at the price of structural and thermal stability. Recently, synthesizing single-crystal cathode particles has been extensively investigated as a strategy to enhance the stability of NMC cathodes. Most commercial NMC cathode particles possess polycrystalline structure, which is prone to induce intergranular cracking and parasitic reactions with the electrolyte upon cycling due to grain boundaries and large surface area. In contrast, single crystal NMC cathodes show higher cycling stability than their polycrystalline counterparts. However, the synthesis of single crystal normally requires higher temperatures and longer calcination duration than that of the polycrystalline counterparts for solid state synthesis. Alternatively, molten salt synthesis of single crystals is less energy-intensive and capable of tuning particle morphology and size. However, there is not yet a systematic guideline for the molten salt synthesis of single crystal Ni-rich NMC cathodes. Herein, we studied the effect of different synthetic parameters on the performance of single crystal Ni-rich NMC cathodes. We applied statistical analysis tools to correlate the synthetic conditions with cathode properties and optimized the synthetic parameters. Furthermore, we investigated the effect of single crystal size on the cathode performance. Our findings provided new insights into the synthesis and understanding of single crystal Ni-rich cathodes.

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Doeff, Marca M. "(Invited) Thermal Properties of NMC Cathode Materials." ECS Meeting Abstracts MA2022-01, no. 2 (July 7, 2022): 378. http://dx.doi.org/10.1149/ma2022-012378mtgabs.

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NMC (LiNixMnyCozO2; x+y+z»1) materials deliver high capacity and excellent performance when used as cathodes in lithium-ion batteries. Increasing demand for higher energy density and concerns about the cost and ethics of using cobalt have prompted battery manufacturers to use Ni-rich formulations such as LiNi0.6Mn0.2Co0.2O2 (NMC622) and LiNi0.8Mn0.1Co0.1O2 (NMC811). The thermal stability of (partially) delithiated NMCs is known to decrease with increasing Ni content, however, so that scenarios of fires and other safety events become more distinct possibilities. To investigate the thermal properties of Ni-rich NMCs, we prepared partially and fully delithiated Ni-rich NMCs corresponding to various states-of-charge by chemical methods. We then studied the bulk and surface properties of these materials as they were heated or after they were heated, using a variety of ex situ and in situ synchrotron methods to understand the chemical changes that occur. Of particular concern are reactions that result in release of oxygen. Heated materials progress through a series of bulk structural changes from layered to spinel to rock salt as temperatures rise. Transition temperatures depend on both lithium and nickel content, with bulk changes evident at temperatures as low as 150°C. Surface-sensitive techniques such as soft X-ray absorption spectroscopy (sXAS) indicate that subtle changes that lead to oxygen release can happen well below these temperatures. The thermal behavior of the Ni-rich materials is very complex, and involves lattice transformation, transition metal migration and valence change and lithium redistribution. Moreover, these changes are dependent upon primary particle size, with smaller particles reacting at lower temperatures than larger ones. These observations suggest that materials can be engineered (through primary particle size manipulation, for example) to improve thermal robustness, and therefore, safety and reliability of lithium-ion batteries.

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Nguyen Le, Minh, Hoang Nguyen Van, Trang Bach Le Thuy, Man Tran Van, and Phung Le My Loan. "O3-type layered Ni-rich cathode: synthesis and electrochemical characterization." Vietnam Journal of Catalysis and Adsorption 10, no. 1S (October 15, 2021): 206–11. http://dx.doi.org/10.51316/jca.2021.123.

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Ni-rich layered oxides are currently the state-of-the-art material of Lithium-ion batteries due to the balance between the cost, power and energy density. In this work, Ni-rich O3-type NaxNi0.76Mn0.14Co0.10O2.04 (NMC) material was synthesized by the conventional solid-state reaction and investigated as a cathode material for sodium-ion batteries. Rietveld refinement shows that the material is high purity O3-type layered oxide of 91%. In the charge/discharge test, the material was provided the reversible capacity of 156 mAh.g-1 initially at 0.1 C with 50% capacity retention after 50 cycles in the voltage range of 2.0 – 4.2 V. In addition, this material also demonstrates great rate-capability with the discharge capacity of 50 mAh.g-1 even at 5 C. Therefore, NMC material could be a promising candidate for high energy sodium-ion batteries.

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Nisa, Shofirul Sholikhatun, Anisa Raditya Nurohmah, Cornelius Satria Yudha, Hanida Nilasary, Hartoto Nursukatmo, Endah Retno Dyartanti, and Agus Purwanto. "Utilization of Spent Nickel Catalyst as Raw Material for Ni-Rich Cathode Material." Jurnal Presipitasi : Media Komunikasi dan Pengembangan Teknik Lingkungan 18, no. 2 (July 30, 2021): 349–57. http://dx.doi.org/10.14710/presipitasi.v18i2.349-357.

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Spent nickel catalyst will be harmful to the environment if it is not processed or used properly. In fact, this waste still has a high nickel content. The treatment of spent nickel catalysts has been widely reported, but limited to nickel extraction. Since the lithium-ion batteries demand is continued to increase, then nickel is the most sought-after metal. Consequently, nickel from spent nickel catalysts could be developed as secondary source for lithium-ion battery cathode. This study aims to utilize spent nickel catalysts into more valuable materials. Nickel that has been extracted and mixed with Mn and Co has been used as raw material for nickel-rich cathode, namely NMC. Nickel extraction and NMC synthesis were using the acid leaching method followed by co-precipitation[WI1] [SSN2] . Based on the functional test performed in this work, nickel from spent nickel catalyst can be applied to Li-ion batteries. The sintering temperature that gives good characteristics and electrochemistry was found 820oC. The galvanostatic charge-discharge test gave specific capacity results for NMC of 110.4 mAh/g. The cycle test showed that NMC synthesized from spent nickel catalyst can be carried out up to 50 cycles with a capacity retention of 87.18%.

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Touag, Ouardia, Gael Coquil, Mathieu Charbonneau, Denis Mankovsky, and Mickaël Dollé. "One-Pot Synthesis of LiAlO₂-Coated LiNi_0.6Mn_0.2Co_0.2O₂ Cathode Material." ECS Meeting Abstracts MA2022-01, no. 2 (July 7, 2022): 336. http://dx.doi.org/10.1149/ma2022-012336mtgabs.

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The chemistry of lithium-ion batteries (LIBs) is an active area of research, notably through the increasing demand for high energy and power density in LIBs, especially for application in electric vehicles (EVs) and hybrid electric vehicles (HEVs). Among the various cathode materials, LiNixCoyMn1-x-yO2 (NMC) intercalation compounds are the best candidates for applications in high performance LIBs. However, Ni-rich NMC suffers mainly from parasitic side reactions at the interface with the electrolyte, which leads to a lower thermal and electrochemical stability. Surface modification via coating is an effective concept to counter the capacity degradation of NMC and to improve the particles’ structural stability for enhancing their cycle-life [1], [2]. Different processing techniques that usually requires several steps are presented in the literature. However, to facilitate the integration of a new product in the current battery market, it is preferable to reduce the number of steps during the synthesis process. In this work, we propose a one-pot synthesis of LiAlO2-coated LiNi0.6Mn0.2Co0.2O2 particles, by using a continuous stirred-tank reactor (CSTR). Firstly, the composition and morphology of the coated and uncoated cathode materials are characterized by SEM, TEM, EDX and XPS. Then, the structural characterization of our materials is validated by XRD analysis. Consequently, we will compare the electrochemical performance and thermal stability of coated and uncoated NMC particles. We will demonstrate that our approach provides an easy way to apply surface treatment onto Ni-rich NMC particles and simplifies the synthesis process at large scale production. KEYWORDS: Lithium-ion battery, Ni-rich NMC cathode, LiAlO2 coating, surface protection. Negi, R.S., et al., Enhancing the Electrochemical Performance of LiNi0.70Co0.15Mn0.15O2 Cathodes Using a Practical Solution-Based Al2O3 Coating. ACS Applied Materials & Interfaces, 2020. 12(28): p. 31392-31400. Kim, H.-S., et al., Enhanced electrochemical properties of LiNi1/3Co1/3Mn1/3O2 cathode material by coating with LiAlO2 nanoparticles. Journal of Power Sources, 2006. 161(1): p. 623-627.

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Sawangphruk, Montree, and Krisara Srimanon. "Dry Particle Fusion Assisted Ceramic Coatings for High Nickel Cathode for Scalable 18650 Lithium-Ion Batteries." ECS Meeting Abstracts MA2022-01, no. 2 (July 7, 2022): 416. http://dx.doi.org/10.1149/ma2022-012416mtgabs.

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Over the last several decades, energy storage has become one of the central tools for facilitating energy transformation from (electro)chemical reactions to electricity. Rechargeable lithium-ion batteries (LIBs) are among the most popular and promising mature technologies for portable electronics, grids, and transportation. The cathode, a working horse, mainly determines the overall capacity among the various components. Off-late layered Li-rich or Ni-rich material plays a vital role, especially Ni-rich LiNixMnyCo1-x-yO2; x ≥ 0.8 (NMC) get significant attention. However, it is unfortunate that such Ni-rich cathode materials encountered severe capacity degradation and poor thermal instability concerning the Ni-concentration. Several strategies have already been proposed to mitigate those issues, including electrolyte additive, cation doping, and coating or surface modification. Among them, the modification of the cathode surface, like core-shell construction, is a practical approach. Herein, a core-shell architecture was achieved by employing the cost-effective dry particle fusion method over Ni-rich (LiNi0.8Mn0.1Co0.1O2 (NMC811), where the nano aluminum oxide was used as a shell material with an average thickness of 150-200 nm. Such NMC@alumina core-shell exhibits excellent cycling stability compared with pristine NMC811. The chemical lithium diffusion coefficient was calculated using galvanostatic (GITT) and the potentio-dynamics process. Additionally, the control of parasitic reaction between the delithiated cathode and electrolyte was analyzed using the in-situ Differential Electrochemical Mass Spectrometry (DEMs) technique, where the onset potential and the amount of gas generated are compared with pristine material.

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Fung, Kuan-Zong, Shu-Yi Tsai, and Jen-Hao Yang. "(Digital Presentation) Performance Improvement of Nickel-Rich Layered Cathodes for Li Batteries Based on Modified Solid State Reaction." ECS Meeting Abstracts MA2022-01, no. 6 (July 7, 2022): 2500. http://dx.doi.org/10.1149/ma2022-0162500mtgabs.

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Lithiated metal oxides with layered structure used as the cathode may provide a high capacity and stable cycle retention, which is a desired property for lithium-ion batteries. Among them, NMC composed of Ni, Mn and Co as transition metal ions is considered a promising positive electrode. Due to high cost and toxicity of Co, Ni-rich layered oxide with substitution of Ni for Co content shows high capacity and adequate cycling performance. Recently, the fabrication of NMC adopting single-crystal (grain size: 1~6 μm) process tends to give better long-term performance than ones with particles in nanometer range. In this study, LiNi0.8Mn0.1Co0.1O2 (NMC811) with substitution of Ni/Mn for Co were selected as the Ni-rich layered cathode investigated. Due to the low melting point of Li2CO3, the heating temperature/time of powder mixture become crucial to control the adequate grain size of to achieve better retention. The value of the I(003) /I(104) ratio in XRD pattern represent cation mixing in layered structure. And this parameter is closely related to its electrochemical properties. Discussion will be carried out based on the results of XRD analysis and the charge–discharge profiles and cycling performance.

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Bunyanidhi, Panyawee, and Montree Sawangphruk. "Investigation of Garnet Solid Electrolyte-Layered Oxide Cathode Interfaces Towards Cylindrical High-Performance Li-Ion Batteries." ECS Meeting Abstracts MA2022-01, no. 2 (July 7, 2022): 164. http://dx.doi.org/10.1149/ma2022-012164mtgabs.

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Even though the Ni-rich cathode materials (Ni content > 60%), providing high energy density and high capacity, can draw much attention for advanced lithium-ion battery (LIB) community and industry, several drawbacks such as poor structural stability, thermal stability, and capacity fading still restrict their scalable application. Herein, the trace amount of garnet Li7La3Zr2O12 (LLZO) oxide solid-state electrolyte was introduced on the LiNi0.8Mn 0.1 Co0.1O2 (NMC811) cathode as a scaffolding interfacial layer on NMC particles via a one-step solvent-free mechanofusion process. The interfacial La-Ni exchange after mechanofusion was investigated by the extended X-ray absorption fine structure (EXAFS) measurement. Subsequently, the in situ X-ray diffraction was used to investigate the crystallographic evolution during the charge-discharge process. The NMC-LLZO cathode exhibits excellent rate capability and cycling performance, especially at high current density. The LLZO interfacial layer was found to be able to delay Li insertion into NMC bulk which in turn led to a better Li distribution and higher rate capability over pristine NMC. The practical applications of NMC-LLZO are also presented in 2.5 Ah 18650-format lithium-ion batteries. The cells can perform from C/10 to 1C with only 16% capacity reduction and remain 80% retention after cycled up to 500 cycles at a high current density of 1C compared to 40% of NMC cells. Keywords: LiNi0.8Mn0.1Co0.1O2, Lithium-ion batteries, Oxide solid-state electrolyte, Scaffolding layer, High current density

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Chen, Heyin, Tove Ericson, Esko Kokkonen, Robert Temperton, Margit Andersson, Anastasiia Mikheenkova, William Brant, and Maria Hahlin. "Investigating Surface Sensitivity of Ni-Rich Cathode Material Towards CO₂ and H₂O." ECS Meeting Abstracts MA2022-01, no. 4 (July 7, 2022): 520. http://dx.doi.org/10.1149/ma2022-014520mtgabs.

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Layered Ni-rich transition metal oxide materials have been considered as the most promising cathode utilized in Li-ion batteries, e.g., LiNi0.8 Mn0.1 Co0.1 O2 (NMC 811). However, one of the drawbacks of NMC 811 is its high air sensitivity, leading to a degradation layer forming on the surface, and a lower cycling performance. Since the degradation mechanism is not fully understood, in this work, we use ambient pressure photoelectron spectroscopy (APPES)1 to investigate the surface sensitivity of NMC 811 towards CO2 and H2O in situ, aiming to determine the factor triggering the degradation. Before gas exposure, NMC 811 surface was Ar+ sputtered to remove the pre-existing boron oxide coating. The changes in surface chemical composition were monitored as a function of time and gas pressure. Results show that carbonate compounds are formed on the surface when NMC 811 is exposed to CO2. The carbonate compounds start to appear already within 2 minutes in CO2 at around 10-5 mbar. More interestingly, this reaction is reversed at around 3x10-6 mbar. Changes induced by water are slower, however, the water vapour effect on NMC 811 surface is irreversible. Results indicate that lithium hydroxide is formed, where Li+/H+ exchange on the surface is a possible route.2 Kokkonen, E.; Lopes Da Silva, F.; Mikkelã, M.-H.; Johansson, N.; Huang, S.-W.; Lee, J.-M.; Andersson, M.; Bartalesi, A.; Reinecke, B. N.; Handrup, K.; Tarawneh, H.; Sankari, R.; Knudsen, J.; Schnadt, J.; Såthe, C.; Urpelainen, S., Upgrade of the SPECIES beamline at the MAX IV Laboratory. Journal of Synchrotron Radiation 2021, 28 (2), 588-601. Hartmann, L.; Pritzl, D.; Beyer, H.; Gasteiger, H. A., Evidence for Li+/H+ Exchange during Ambient Storage of Ni-Rich Cathode Active Materials. Journal of The Electrochemical Society 2021, 168 (7), 070507. Figure 1

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Guyomard, Dominique, Angelica Laurita, Pierre Etienne Cabelguen, Liang Zhu, Nicolas Dupré, Vincent Fernandez, Jonathan Hamon, and Philippe Moreau. "(Invited) Surface Characterisation of Ni-Rich NMC Materials Stored in Various Environments." ECS Meeting Abstracts MA2020-02, no. 1 (November 23, 2020): 2. http://dx.doi.org/10.1149/ma2020-0212mtgabs.

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Cai, Jiyu, Natasha A. Chernova, Brad Prevel, Feng Wang, and Zonghai Chen. "Parasitic-Reaction-Triggered Performance Deterioration of Long-Term Cycling Nickel-Rich Cathodes." ECS Meeting Abstracts MA2022-02, no. 7 (October 9, 2022): 2441. http://dx.doi.org/10.1149/ma2022-0272441mtgabs.

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Ni-rich LiNi1-x-yMnxCoyO2 (NMC, x+y < 0.5) materials are widely regarded as the promising cathodes for high-energy-density and cost-effective lithium-ion batteries. Cycling performance deterioration is a long-standing challenge for Ni-rich NMC, especially at high potentials (>4.3V vs. Li/Li+). The fundamental understanding of failure mechanisms is crucial for the development of long-life lithium-ion technologies. In our investigation, full cells cycled to 4.35 V for 1000 cycles lose about 49% of their initial capacity, while the counterparts cycled to 4.15V lose only 27% of their initial capacity after 1000 cycles. The relatively low capacity loss of the low voltage cells (4.15 V) is dominated by the impedance hike, while the drastically increased (more than half of) capacity loss of high voltage cells (4.35 V) is contributed from the irreversible degradation of the electrode materials. The post-mortem diagnosis suggests that parasitic reactions are the primary driving force for severe deteriorations, including the irreversible phase transformation. The generally concerned transition metal dissolution and bulk phase transformation negligibly make direct contributions to the severe capacity loss, but the loss of active cathode materials has some substantially detrimental impacts on irreversible capacity loss. Our findings emphasize that mitigating parasitic reactions is crucial for enabling long life of Ni-rich cathodes. Figure 1

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Boz, Buket, Miljana Vuksanovic, Lukas Neidhart, Micheal Höchtl, Katja Fröhlich, and Marcus Jahn. "Aqueous Manufacturing of Ni-Rich Cathodes Using Polyacrylic Acid As Binder for Lithium-Ion Batteries." ECS Meeting Abstracts MA2022-02, no. 7 (October 9, 2022): 2542. http://dx.doi.org/10.1149/ma2022-0272542mtgabs.

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In the field of secondary batteries, the lithium-ion battery (LIB) is one of the most promising candidates for future electric vehicle (EV) applications, due to its high specific energy and good specific power [1]. However, to meet the demands in large scale storage, not only higher energy and power density and lower cost are needed, but environmentally friendly processing of LiBs is getting more in the focus of research. To meet the desirable requirements, one necessity is to tune the cathode in terms of sustainable production and materials. Ni-rich layered LiNi x Mn y Co1−x−y O2 (NMCs, x ≥ 0.8) cathodes are poised to be the dominating cathode materials for lithium-ion batteries for the foreseeable future due to its high energy density [2]. The state-of-the-art NMC based cathode production in both industrial and lab scale is with polyvinylidene fluoride (PVDF) in organic solvent N-methyl-2-pyrrolidone (NMP). NMP is a toxic, expensive, and highly flammable organic solvent [3]. Replacing NMP with water in the production of LiB cathodes is critical in terms of process cost savings and environmental concerns. Aqueous processes of NMC based cathodes are highly favorable as well as challenging due to the high reactivity of NMC particles. During the slurry preparation, the surface of Ni-rich particles undergoes Li leaching via exchange between H+ from water and Li+ from the active material which leads to increase in pH of the slurry. Li leaching leads to capacity fade and reduces the specific capacity of the cathode. The high pH of the slurry causes corrosion on the aluminum current collector. Surface treatment of NMC particles is a way to prevent Li leaching as well as using carbon coated Al current collector to resist the corrosion, but in terms of production cost these methods are not favorable. In this study, our fundamental aim is to demonstrate the manufacturing of large scale water based NMC811-PAA cathodes. We therefore employ a well-known binder material, polyacrylic acid (PAA), which is water soluble and an anionic polymer. During the mixing processes of the slurry, H+ from PAA can drive Li+ leaching, the leached Li+ reacts with carboxylic groups of PAA and binds to the PAA backbone. Thus, the reaction of H+ and OH- neutralizes the pH of the slurry. Bonded Li+ on PAA creates an active binder in which these Li ions can participate as an additional Li source to aid to prevent capacity decrease. This method has been successfully implemented in the lab scale [4]. Our main target is to investigate the slurry behavior and scalability of the cathodes with a PAA binder. Herein, we report high solid content of slurry behavior of NMC with PAA and the comparison to the conventionally produced slurry for the first time. Also, we show how the slurry behavior is affected by the mixing techniques from lab scale to pilot scale, which is an important parameter for later transfer to industrial production. The electrodes and successfully formed LiPAA as binder are shown by Fourier transformed infrared (FTIR) and Raman spectroscopy. The electrochemical tests are performed both in half and full cell configuration for NMC811-PAA and NMC811-PVDF cathodes. References [1] Tao, Yanqiu, et al. "Second life and recycling: Energy and environmental sustainability perspectives for high-performance lithium-ion batteries." Science advances 7.45 (2021): eabi7633. https://doi.org10.1126/sciadv.abi7633. [2] Lu, Yanying, et al. "Single‐crystal LiNixMnyCo1− x− yO2 cathodes for extreme fast charging." Small 18.12 (2022): 2105833. https://doi.org/10.1002/smll.202105833. [3] Zou, Feng, and Arumugam Manthiram. "A review of the design of advanced binders for high‐performance batteries." Advanced Energy Materials 10.45 (2020): 2002508. https://doi.org/10.1002/aenm.202002508. [4] Hawley, W. Blake, Harry M. Meyer III, and Jianlin Li. "Enabling aqueous processing for LiNi0. 80Co0. 15Al0. 05O2 (NCA)-based lithium-ion battery cathodes using polyacrylic acid." Electrochimica Acta 380 (2021): 138203. https://doi.org/10.1016/j.electacta.2021.138203.

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Fung, Kuan-Zong, and Shu-Yi Tsai. "(Digital Presentation) Cost-Effective Processing of Nickel-Rich Layered Cathodes for Li Batteries." ECS Meeting Abstracts MA2022-02, no. 3 (October 9, 2022): 195. http://dx.doi.org/10.1149/ma2022-023195mtgabs.

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The layered structured cathode material can provide a higher capacity and stable cycle retention, which is a desired property for lithium-ion batteries. Among them, NMC composed of Ni, Mn and Co as transition metals is considered a promising positive electrode. However, because Co is slightly toxic and an expensive strategic resource, reducing the Co content and maintaining the capacitance and cycle stability are the objectives of this study. In this study, LiNi0.8Mn0.1Co0.1O2 were investigated. Adjust the amount of Li2CO3 and the temperature of calcination to control the size of the crystal grains to achieve better retention. The value of the I(003) and I(104) ratio in XRD pattern represent cation mixing in layered structure. And this parameter is closely related to its electrochemical properties. Discussion will be carried out based on the results of XRD analysis and the charge–discharge profiles and cycling performance. The layered structured cathode material may provide a high capacity and stable cycle retention, which is a desired property for lithium-ion batteries. Among them, NMC composed of Ni, Mn and Co as transition metals is considered a promising positive electrode. However, because Co is slightly toxic and an expensive strategic resource, reducing the Co content and maintaining high capacity and cycle stability are the objectives of this study. In addition, the fabrication of NMC adopting single-crystal (grain size: 1~6 mm) process tends to give better long-term performance than ones with particles in nanometer range. In this study, LiNi0.8Mn0.1Co0.1O2 (NMC811) with substitution of Ni/Mn for Co were selected as the Ni-rich layered cathode investigated. Due to the low melting point of Li2CO3, the heating temperature/time of powder mixture become crucial to control the adequate grain size of to achieve better retention. The value of the I(003) and I(104) ratio in XRD pattern represent cation mixing in layered structure. And this parameter is closely related to its electrochemical properties. Discussion will be carried out based on the results of XRD analysis and the charge–discharge profiles and cycling performance.

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Qian, Kun, Yuzi Liu, Xinwei Zhou, David J. Gosztola, Hoai Nguyen, and Tao Li. "Decoupling the degradation factors of Ni-rich NMC/Li metal batteries using concentrated electrolytes." Energy Storage Materials 41 (October 2021): 222–29. http://dx.doi.org/10.1016/j.ensm.2021.06.007.

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17

LIU, Xiang, Guiliang Xu, Liang Yin, Inhui Hwang, Minggao Ouyang, and Khalil Amine. "The Role of Cobalt and Manganese for the Safety of Ni-Rich NMC Cathode." ECS Meeting Abstracts MA2021-01, no. 5 (May 30, 2021): 304. http://dx.doi.org/10.1149/ma2021-015304mtgabs.

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18

Gomez‐Martin, Aurora, Friederike Reissig, Lars Frankenstein, Marcel Heidbüchel, Martin Winter, Tobias Placke, and Richard Schmuch. "Magnesium Substitution in Ni‐Rich NMC Layered Cathodes for High‐Energy Lithium Ion Batteries." Advanced Energy Materials 12, no. 8 (January 5, 2022): 2103045. http://dx.doi.org/10.1002/aenm.202103045.

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19

Dose, Wesley M., Amoghavarsha Mahadevegowda, Jędrzej K. Morzy, Caterina Ducati, Clare P. Grey, and Michael F. L. De Volder. "Origins of Capacity Fade and Material Degradation in Ni-Rich NMC Li-Ion Batteries." ECS Meeting Abstracts MA2020-01, no. 2 (May 1, 2020): 218. http://dx.doi.org/10.1149/ma2020-012218mtgabs.

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White, James L., Forrest S. Gittleson, Mark Homer, and Farid El Gabaly. "Nickel and Cobalt Oxidation State Evolution at Ni-Rich NMC Cathode Surfaces during Treatment." Journal of Physical Chemistry C 124, no. 30 (July 6, 2020): 16508–14. http://dx.doi.org/10.1021/acs.jpcc.0c04794.

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21

Dose, Wesley, Jędrzej K. Morzy, Amoghavarsha Mahadevegowda, Caterina Ducati, Clare P. Grey, and Michael F. L. De Volder. "Origins of Capacity Fade and Material Degradation in Ni-Rich NMC Li-Ion Batteries." ECS Meeting Abstracts MA2020-02, no. 45 (November 23, 2020): 3724. http://dx.doi.org/10.1149/ma2020-02453724mtgabs.

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22

Zhao, Wengao, Jianming Zheng, Lianfeng Zou, Haiping Jia, Bin Liu, Hui Wang, Mark H. Engelhard, et al. "High Voltage Operation of Ni-Rich NMC Cathodes Enabled by Stable Electrode/Electrolyte Interphases." Advanced Energy Materials 8, no. 19 (March 30, 2018): 1800297. http://dx.doi.org/10.1002/aenm.201800297.

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23

Llewellyn, Alice V., Andrew S. Leach, Isabella Mombrini, Alessia Matruglio, Jiecheng Diao, Chun Tan, Thomas M. M. Heenan, et al. "Understanding the Degradation Mechanisms of Lithium Ion Batteries Using in-Situ Multi-Scale Diffraction Techniques." ECS Meeting Abstracts MA2022-01, no. 2 (July 7, 2022): 177. http://dx.doi.org/10.1149/ma2022-012177mtgabs.

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Анотація:

Advanced Li-ion batteries adopting new cathode chemistries are required for the successful widespread transition to electric vehicles (EVs) and renewable energy sources, aiming for high energy density, long cycle life, and good rate capability. Commercial candidates for EV batteries include Ni-rich Li(NixMnyCo1−x-y)O2 (NMC) cathodes, with Ni:Mn:Co ratios of 8:1:1 (NMC811) and higher. These are favored because of their high specific capacity (~ 200 mAh g-1)and reduced cobalt content. Despite all of the advantages, these materials suffer from a range of degradation modes, many of which are associated with the redox and crystallographic behavior at high states of charge. In particular, Ni-rich cathodes suffer from several limitations, such as rapid capacity fade in comparison to NMC stoichiometries with lower Ni content. In addition, they also have a lower onset voltage for oxygen release and subsequent surface reconstruction leading to the formation of spinel and rock salt phases which impede (de)lithiation and therefore the achievable capacity of the cell.1 Crystallographic properties of electrode materials are intrinsically linked to the electrochemical performance of the cell. NMC materials suffer from anisotropic changes in the crystal structure during cycling which induces strain and leads to issues such as crack formation, expediting degradation. One method to tackle capacity fade is to switch to single-crystal morphologies (particle size 1-3 μm) which have better mechanical stability than conventional polycrystalline morphologies (secondary agglomerate particles ~ 10 μm made up of primary particles which are 100 nm – 1 μm in size) and have less propensity to form extensive rock-salt layers. It is thought that the single-crystal morphology helps to reduce stress in the material as the anisotropic stress in polycrystalline cathodes is concentrated at grain boundaries. However, there is still a limited understanding of the subtle mechanistic differences between the two materials during cycling.2 A multi-scale approach is required to gain a more comprehensive understanding of the degradation mechanisms at play and how they initiate and propagate. In this work, synchrotron diffraction methods were employed at the crystal, particle and cell scale using a variety of techniques including in-situ Bragg Coherent Diffraction Imaging (BCDI), 3D-XRD and operando high-resolution XRD. Intra-particle, inter-particle and electrode level heterogeneities were observed during cycling, both in pristine and aged samples. It is believed that these heterogeneities accelerate the loss of performance at the cell level by inducing crack formation which can then be observed in X-ray computed tomography data acquired in simultaneous lab studies. The overarching goal of these investigations is to add to the understanding of complex degradation mechanisms for Ni-rich layered transition metal oxide cathodes, ultimately aiding in the informed development of future battery electrode materials. References: 1] Xu, C. et al., Phase Behaviour during Electrochemical Cycling of Ni‐Rich Cathode Materials for Li‐Ion Batteries. Adv. Energy Mater. 2021, 11, 2003404. 2] Yin, S. et al., Fundamental and solutions of microcracks in Ni-rich layered oxide cathode materials of lithium-ion batteries. Nano Energy, 2021, 83, 105854.

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West, Patrick J., Cavlin Quilty, Wenzao Li, Mikaela R. Dunkin, Garrett Wheeler, Christopher Kern, Killian Tallman, et al. "K-Edge and L-Edge Spectroscopy of Ni_0.8Mn_0.1Co_0.1O₂ Cathodes Under Expanded Voltage Conditions Via Soft X-Ray Absorption Spectroscopy." ECS Meeting Abstracts MA2022-02, no. 3 (October 9, 2022): 317. http://dx.doi.org/10.1149/ma2022-023317mtgabs.

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Mixed transition metal oxides, such as Ni0.8Mn0.1Co0.1O2 (NMC811), are intended to combine the high capacity of nickel oxides, the rate capability of cobalt oxides, and the structural stability of manganese oxides to meet the capacity and power demands of electric vehicles and commercial portable electronics. However, the capacity fade mechanisms in Ni-rich chemistries (x >y+z in NixMnyCozO2) can be elusive due to factors at the crystallographic, particle, or electrode level. In this study, bulk and surface x-ray spectroscopy characterization of NMC cathodes was used to explore cathode degradation mechanisms as influenced by cycling protocol, namely current rate and upper voltage limits. Soft x-ray absorption spectroscopy (sXAS) was used to probe the surface of recovered NMC electrodes via transition metal L-edge and O K-edge spectroscopy. The effect of rate and upper voltage potential under charge will be discussed to illustrate the versatility of sXAS for NMC cathode electrode characterization.

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25

Kitsche, David, Aleksandr Kondrakov, Jürgen Janek, and Torsten Brezesinski. "(Invited) ALD Coatings for Li-Ion Battery and All-Solid-State Battery Applications." ECS Meeting Abstracts MA2022-02, no. 31 (October 9, 2022): 1138. http://dx.doi.org/10.1149/ma2022-02311138mtgabs.

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Lithium-ion batteries (LIBs) are essential for modern life, and their improvement is crucial for the more widespread adoption of electric vehicles.[1] Layered lithium transition metal oxides, such as LiNixCoyMnzO2 (often referred to as NCM or NMC), are among the most widely used cathode active materials (CAMs) for automotive applications, owing to their technological maturity and high energy density. However, they typically require a surface coating for stabilizing interfaces, both in liquid-electrolyte based LIBs and in solid-state battery (SSB) environments. For the preparation of protective CAM coatings, atomic layer deposition (ALD) stands out with its ability to produce conformal films on complex substrates. This presentation encompasses several examples of successful improvements in cycling performance of Ni-rich NCM CAMs in LIBs and SSBs by ALD of binary oxides. The low-temperature deposition of AlxOy onto ready-to-use cathode sheets will be discussed.[2] ALD or ALD-related surface protection enables increased stability by suppressing detrimental surface corrosion and metal leaching (side reactions) in LIBs.[2,3] Moreover, we report about the application of ALD coatings to Ni-rich NCM CAMs in SSBs with lithium thiophosphate solid electrolytes. Specifically, the effect that both HfO2 and ZrO2 have on the cell cyclability will be shown, with emphasis placed on the role of post annealing.[4] [1] Goodenough et al. J. Am. Chem. Soc. 2013, 135, 1167. [2] Neudeck et al. Sci. Rep. 2019, 9, 5328. [3] Neudeck et al. Chem. Commun. 2019, 55, 2174. [4] Kitsche et al. ACS Appl. Energy Mater. 2021, 4, 7338.

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Lyu, Peizhao, Yutao Huo, Zhiguo Qu, and Zhonghao Rao. "Investigation on the thermal behavior of Ni-rich NMC lithium ion battery for energy storage." Applied Thermal Engineering 166 (February 2020): 114749. http://dx.doi.org/10.1016/j.applthermaleng.2019.114749.

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27

Bi, Yujing, Qiuyan Li, Ran Yi, and Jie Xiao. "To Pave the Way for Large-Scale Electrode Processing of Moisture-Sensitive Ni-Rich Cathodes." Journal of The Electrochemical Society 169, no. 2 (February 1, 2022): 020521. http://dx.doi.org/10.1149/1945-7111/ac4e5d.

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Анотація:

High-capacity Ni-rich cathode such as LiNi0.8Mn0.1Co0.1O2 (NMC811) has a great potential to enable high energy lithium-ion batteries (LIBs) for long-range electrical vehicles. However, the utilization of NMC 811 in large-scale application is still challenging. While many published papers on NMC811 focus on materials modification, the moisture sensitivity of NMC811 and its implications in storage and large-scale electrode coating are not well explored, not to mention how to overcome those challenges for industry application. This work discusses the key parameters impacting the rheological properties of NMC811 slurries and their correlations to the properties of dried electrodes. Effective solutions are proposed to address the gelation issue of NMC811 slurry during large-scale coating to hopefully inspire more effective and practical approaches to tackle the grand challenges in electrochemical energy storage.

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28

Tsai, Ya-Ting, Che-Ya Wu, and Jenq-Gong Duh. "Synthesis of Ni-rich NMC cathode material by redox-assisted deposition method for lithium ion batteries." Electrochimica Acta 381 (June 2021): 138244. http://dx.doi.org/10.1016/j.electacta.2021.138244.

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29

Jung, Roland, Fabian Linsenmann, Rowena Thomas, Johannes Wandt, Sophie Solchenbach, Filippo Maglia, Christoph Stinner, Moniek Tromp, and Hubert A. Gasteiger. "Nickel, Manganese, and Cobalt Dissolution from Ni-Rich NMC and Their Effects on NMC622-Graphite Cells." Journal of The Electrochemical Society 166, no. 2 (2019): A378—A389. http://dx.doi.org/10.1149/2.1151902jes.

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30

Ronduda, Hubert, Magdalena Zybert, Anna Szczęsna-Chrzan, Tomasz Trzeciak, Andrzej Ostrowski, Damian Szymański, Władysław Wieczorek, Wioletta Raróg-Pilecka, and Marek Marcinek. "On the Sensitivity of the Ni-rich Layered Cathode Materials for Li-ion Batteries to the Different Calcination Conditions." Nanomaterials 10, no. 10 (October 13, 2020): 2018. http://dx.doi.org/10.3390/nano10102018.

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Ni-rich layered oxides, i.e., LiNi0.6Mn0.2Co0.2O2 (NMC622) and LiNiO2 (LNO), were prepared using the two-step calcination procedure. The samples obtained at different calcination temperatures (750–950 °C for the NMC622 and 650–850 °C for the LNO cathode materials) were characterized using nitrogen physisorption, PXRD, SEM and DLS methods. The correlation of the calcination temperature, structural properties and electrochemical performance of the studied Ni-rich layered cathode materials was thoroughly investigated and discussed. It was determined that the optimal calcination temperature is dependent on the chemical composition of the cathode materials. With increasing nickel content, the optimal calcination temperature shifts towards lower temperatures. The NMC-900 calcined at 900 °C and the LNO-700 calcined at 700 °C showed the most favorable electrochemical performances. Despite their well-ordered structure, the materials calcined at higher temperatures were characterized by a stronger sintering effect, adverse particle growth, and higher Ni2+/Li+ cation mixing, thus deteriorating their electrochemical properties. The importance of a careful selection of the heat treatment (calcination) temperature for each individual cathode material was emphasized.

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Zhao, Wengao, Lianfeng Zou, Haiping Jia, Jianming Zheng, Donghao Wang, Junhua Song, Chaoyu Hong, et al. "Optimized Al Doping Improves Both Interphase Stability and Bulk Structural Integrity of Ni-Rich NMC Cathode Materials." ACS Applied Energy Materials 3, no. 4 (March 5, 2020): 3369–77. http://dx.doi.org/10.1021/acsaem.9b02372.

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32

Whittingham, Stan, BEN PEI, Isik Buyuker, Krystal Lee, Fengxia Xin, and Hui Zhou. "(Invited, Digital Presentation) Pushing the Limits of High Nickel NMC Cathodes." ECS Meeting Abstracts MA2022-01, no. 2 (July 7, 2022): 334. http://dx.doi.org/10.1149/ma2022-012334mtgabs.

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Анотація:

Lithium-ion batteries now dominate electrochemical energy storage for vehicle propulsion and grid storage in addition to portable electronics. In 2022, they celebrate their 50th anniversary, and yet still achieve only 25% of their theoretical energy density. The dominant anode and cathode today are graphitic carbon and the layered NMC oxides, LI[NiMnCoAl]O2. Both need improving. Most of the carbon in the anode must go, and the NMCs need pushing to their limit and at the same time eliminating cobalt. I will today discuss the challenges faced as we push the limits of the NMCs to their limits, > 80% lithium cycling, and Ni>0.8 and Co <<0.1. The higher the Ni content the lower the charging voltage needed for a given cycling capacity, but the greater its surface and bulk reactivity. The issues discussed will include 1stcycle loss [1], high rate capability [2], cathode stability [3], and surface/bulk reactivity and the impact of surface/bulk modification [4,5] and the micron-size single crystals vs meatballs on these [6]. This work is being supported by DOE-EERE-BMR-Battery500 consortium. [1]. Hui Zhou, Fengxia Xin, Ben Pei, M. Stanley Whittingham, “What Limits the Capacity of Layered Oxide Cathodes in Lithium Batteries?”, ACS Energy Lett. 2019, 4: 1902−1906. [2]. Chunmei Ban, Zheng Li, Zhuangchun Wu, Melanie J. Kirkham, Le Chen, Yoon Seok Jung, E. Andrew Payzant, Yanfa Yan, M. Stanley Whittingham, and Anne C. Dillon “Extremely Durable High-Rate Capability of a LiNi0.4Mn0.4Co0.2O2 Cathode Enabled by Single–Wall Carbon Nanotubes”, Advanced Energy Materials, 2011, 1: 58-62. [3]. Hyung-Joo Noh, Sungjune Youn, Chong Seung Yoon, Yang-Kook Sun “Comparison of the structural and electrochemical properties of layered Li[NixCoyMnz]O2 (x = ¼ 1/3, 0.5, 0.6, 0.7, 0.8 and 0.85) cathode material for lithium-ion batteries”, J. Power Sources, 2013, 233: 121-130. [4]. Fengxia Xin, Hui Zhou, Yanxu Zong, Mateusz Zuba, Yan Chen, Natasha A. Chernova, Jianming Bai, Ben Pei, Anshika Goel, Jatinkumar Rana, Feng Wang, Ke An, Louis F. J. Piper, Guangwen Zhou, and M. Stanley Whittingham, “What is the Role of Nb in Nickel-Rich Layered Oxide Cathodes for Lithium-Ion Batteries?”, ACS Energy Letters, 2021, 6: 1377-1382. [5]. Ben Pei, Hui Zhou, Anshika Goel, Mateusz Zuba, Hao Liu, Fengxia Xin, and M. Stanley Whittingham, “Al Substitution for Mn during Co-Precipitation Boosts the Electrochemical Performance of LiNi0.8Mn0.1Co0.1O2”, J. Electrochemical Society, 2021, 68: 050532. [6]. Yujing Bi, Jinhui Tao, Yuqin Wu, Linze Li, Yaobin Xu, Enyuan Hu, Bingbin Wu, Jiangtao Hu, Chongmin Wang, JiGuang Zhang, Yue Qi and Jie Xiao, “Reversible planar gliding and microcracking in a single-crystalline Ni-rich cathode”, Science, 2020, 370: 1313-1317.

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33

Teichert, P., H. Jahnke, and E. Figgemeier. "Degradation Mechanism of Monocrystalline Ni-Rich Li[Ni x Mn y Co z ]O 2 (NMC) Active Material in Lithium Ion Batteries." Journal of The Electrochemical Society 168, no. 9 (September 1, 2021): 090532. http://dx.doi.org/10.1149/1945-7111/ac239f.

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Stegemann, Frank, and Oliver Janka. "Crystal structure and magnetic properties of the ternary rare earth metal-rich transition metallides RE14T3Al3 (RE = Y, Gd–Tm, Lu; T = Co, Ni)." Zeitschrift für Naturforschung B 74, no. 1 (January 28, 2019): 125–35. http://dx.doi.org/10.1515/znb-2018-0196.

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Анотація:

AbstractThe rare earth metal-rich RE14T3Al3 series (RE=Y, Gd–Tm, Lu; T=Co, Ni) have been prepared by arc-melting the rare earth metals with appropriate amounts of TAl precursors. All compounds crystallize in the tetragonal crystal system with space group P42/nmc in the Gd14Co3In2.7-type structure. Two structures (Y14Co2.78(1)Al3.22(1): a=952.99(4), c=2292.98(10) pm, wR2=0.0423, 2225 F2 values, 63 variables; Y14Ni3.07(2)Al2.93(2): a=955.06(5), c=2298.77(10) pm, wR2=0.0416, 2225 F2 values, 63 variables) have been refined from single-crystal data, indicating T/Al mixing on one crystallographic site. The lattice parameters of all members have been refined from powder X-ray diffraction experiments. The Y and Lu containing compounds for T=Co and Ni exhibit Pauli paramagnetic behavior, indicating that the Co and Ni atoms exhibit no localized magnetic moment in line with a filled 3d band. The other compounds show paramagnetism, in line with the rare earth atoms in the trivalent oxidation state. Detailed magnetic investigations, however, were impossible due to the presence of e.g. RE3T trace impurities.

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35

Kanthachan, Jaruwan, Sukum Eitssayeam, Sitthi Duangphet, Uraiwan Intatha, Wilaiwan Leenakul, and Tawee Tunkasiri. "The Study of Synthesis Parameters of Synthesis Ni-Rich of LiNi_0.75Mn_0.15Co_0.10O₂ Powder by Co-Precipitation Method." Applied Mechanics and Materials 891 (May 2019): 206–13. http://dx.doi.org/10.4028/www.scientific.net/amm.891.206.

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Lithium Nickel Manganese Cobalt Oxide (LiNi0.75Mn0.15Co0.10O2: NMC) is become interested materials for lithium battery applications due to high specific energy and low cost. The pure phase and well-ordered layered structure has been synthesized by co-precipitation method. In this study, the Nickel-rich LiNi0.75Mn0.15Co0.10O2 positive electrode powder was prepared using co-precipitation method. The influence of synthesis parameters such as calcination temperature, time and amount of water for rinse a NaOH and NH4OH were studied. Then, phase formation and structure were studied by X-ray Powder Diffraction (XRD). The morphological changes is also confirmed by scanning electron microscope (SEM). A checking weight loss by thermo gravimetric Analysis (TGA). Finally, the optimum parameter to prepare highest pure NMC powder are rinse suddenly until pH 7 and calcination only single1 step.

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36

Orlova, Elena D., Aleksandra A. Savina, Sergey A. Abakumov, Anatolii V. Morozov, and Artem M. Abakumov. "Comprehensive Study of Li+/Ni2+ Disorder in Ni-Rich NMCs Cathodes for Li-Ion Batteries." Symmetry 13, no. 9 (September 3, 2021): 1628. http://dx.doi.org/10.3390/sym13091628.

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Анотація:

The layered oxides LiNixMnyCozO2 (NMCs, x + y + z = 1) with high nickel content (x ≥ 0.6, Ni-rich NMCs) are promising high-energy density-positive electrode materials for Li-ion batteries. Their electrochemical properties depend on Li+/Ni2+ cation disordering originating from the proximity of the Li+ and Ni2+ ionic radii. We synthesized a series of the LiNi0.8Mn0.1Co0.1O2 NMC811 adopting two different disordering schemes: Ni for Li substitution at the Li site in the samples finally annealed in air, and close to Ni↔Li antisite disorder in the oxygen-annealed samples. The defect formation scenario was revealed with Rietveld refinement from powder X-ray diffraction data, and then the reliability of semi-quantitative parameters, such as I003/I104 integral intensity ratio and c/(2√6a) ratio of pseudocubic subcell parameters, was verified against the refined defect concentrations. The I003/I104 ratio can serve as a quantitative measure of g(NiLi) only after explicit correction of intensities for preferred orientation. Being normalized by the total scattering power of the unit cell, the I003/I104 ratio depends linearly on g(NiLi) for each disordering scheme. The c/(2√6a) ratio appears to be not reliable and cannot be used for a quantitative estimate of g(NiLi). In turn, the volume of the R3¯m unit cell correlates linearly with g(NiLi), at least for defect concentrations not exceeding 5%. The microscopy techniques such as high-resolution high-angle annular dark-field scanning transmission electron microscopy (HAADF-STEM) and electron diffraction tomography (EDT) allow us to study the materials locally, still, there is no proper quantitative approach for comprehensive analysis of defects. In the present work, the TEM-assisted quantitative Li+/Ni2+ disordering analysis with EDT and HAADF-STEM in six Ni-rich NMC samples with various defects content is demonstrated. Noteworthy, while PXRD and EDT methods demonstrate overall defect amounts, HAADF-STEM allows us to quantitatively distinguish regions with various disordering extents. Therefore, the combination of mentioned PXRD and TEM methods gives the full picture of Li+/Ni2+ mixing defects in Ni-rich NMCs.

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Gupta, Himani, Shishir K. Singh, Nitin Srivastava, Dipika Meghnani, Rupesh K. Tiwari, Raghvendra Mishra, Anupam Patel, Anurag Tiwari, Achchhe L. Saroj, and Rajendra Kumar Singh. "Improved High Voltage Performance of Li-ion Conducting Coated Ni-rich NMC Cathode Materials for Rechargeable Li Battery." ACS Applied Energy Materials 4, no. 12 (November 28, 2021): 13878–89. http://dx.doi.org/10.1021/acsaem.1c02681.

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38

Poches, Christopher, Amir Abdul Razzaq, Haiden Studer, Xuguang Li, Krzysztof Pupek, and Weibing Xing. "High Voltage Electrolytes to Stabilize Ni-Rich Lithium Battery Performance." ECS Meeting Abstracts MA2022-02, no. 3 (October 9, 2022): 188. http://dx.doi.org/10.1149/ma2022-023188mtgabs.

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Анотація:

State-of-the-art (SOA) lithium-ion (Li-ion) batteries are approaching their specific energy density limit (~250 Wh kg−1).1 Layered structured, nickel-rich (Ni-rich or high Ni content) lithium transition metal oxides, e.g., LiNi0.8Mn0.1Co0.1O2 (NMC811), have attracted great interests2 owning to their practically deliverable high specific capacity >200 mAh/g. Coupled with high average discharge voltages (~4V vs. Li/Li+), Ni-rich cathode-based lithium batteries possess a great potential to achieve much higher specific energies, e.g., >350 Wh/kg at cell level targeted for electric drive vehicles,3 than SOA Li-ion batteries. In addition, Ni-rich oxides are economically viable as low-cost battery cathode materials due to their low cobalt content. However, Ni-rich cathode-based Li-ion batteries exhibit a quick capacity degradation upon cycling particularly at high charge cutoff voltages (e.g., 4.5V vs. Li/Li+) and at elevated temperatures. Possible degradation mechanisms of Ni-rich based Li cells include structural changes of the material (large c-axis shrinkage at high potentials)4 and parasitic reactions that arise from the interactions between the electrolytes and highly reactive delithiated cathode surface (due to high oxidation state Ni4+ ions).5,6 Therefore, R&D efforts are needed to tackle technical challenges facing the Ni-rick based Li batteries before they become commercially viable. We will present our efforts of developing high voltage electrolytes to afford stable electrochemical performance of Ni-rich cathode-based Li cells. Figure 1 shows the electrochemical performance of NMC-811 cathode, paired Li metal anode, in conventional Li-ion battery electrolyte (Baseline electrolyte) and the high voltage electrolyte developed in this study, evaluated at C/4 rate during the formation and 1 C rate during cycling, between 2.5V and 4.5V, at room temperature. The cell with the high voltage electrolyte maintained ~80% capacity retention after 400 cycles. In contract, the cell with the baseline electrolyte experieced a large capacity fade with only ~25% capacity retention after 400 cycles. The superior cycle stability of the high votage electrolyte, Ni-rich based cell is attributed to the inharently high-voltage stable, multi-functional. Electrolyte chemical structures and their correlation with the electrochemical stability will be discussed. References Chen, W.; Lei, T.; Qian, T.; Lv, W.; He, W.; Wu, C.; Liu, X.; Liu, J.; Chen, B.; Yan, C.; Xiong, J., Advanced Energy Materials 2018, 8 (12). Jiang, M.; Danilov, D. L.; Eichel, R.-A.; Notten, P. H. L., Advanced Energy Materials 2021, 11 (48), 2103005. Gomez‐Martin, A.; Reissig, F.; Frankenstein, L.; Heidbüchel, M.; Winter, M.; Placke, T.; Schmuch, R., Advanced Energy Materials 2022, 12 (8). Cho, D.-H.; Jo, C.-H.; Cho, W.; Kim, Y.-J.; Yashiro, H.; Sun, Y.-K.; Myung, S.-T., Journal of The Electrochemical Society 2014, 161 (6), A920-A926. Chen, C. H.; Liu, J.; Amine, K., Journal of Power Sources 2001, 96 (2), 321-328. Li, J.; Downie, L. E.; Ma, L.; Qiu, W.; Dahn, J. R., Journal of The Electrochemical Society 2015, 162 (7), A1401-A1408. Acknowledgement This material is based upon work supported by the Naval Air Warfare Center Weapons Division, China Lake, CA under Contract No N6893622C0017. Any opinions, findings and conclusions or recommendations expressed in this material are those of the author(s) and do not necessarily reflect the views of the Naval Air Warfare Center Weapons Division, China Lake, CA. Figure 1

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39

Hendrickx, Mylène, Andreas Paulus, Maria A. Kirsanova, Marlies K. Van Bael, Artem M. Abakumov, An Hardy, and Joke Hadermann. "The Influence of Synthesis Method on the Local Structure and Electrochemical Properties of Li-Rich/Mn-Rich NMC Cathode Materials for Li-Ion Batteries." Nanomaterials 12, no. 13 (June 30, 2022): 2269. http://dx.doi.org/10.3390/nano12132269.

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Electrochemical energy storage plays a vital role in combating global climate change. Nowadays lithium-ion battery technology remains the most prominent technology for rechargeable batteries. A key performance-limiting factor of lithium-ion batteries is the active material of the positive electrode (cathode). Lithium- and manganese-rich nickel manganese cobalt oxide (LMR-NMC) cathode materials for Li-ion batteries are extensively investigated due to their high specific discharge capacities (>280 mAh/g). However, these materials are prone to severe capacity and voltage fade, which deteriorates the electrochemical performance. Capacity and voltage fade are strongly correlated with the particle morphology and nano- and microstructure of LMR-NMCs. By selecting an adequate synthesis strategy, the particle morphology and structure can be controlled, as such steering the electrochemical properties. In this manuscript we comparatively assessed the morphology and nanostructure of LMR-NMC (Li1.2Ni0.13Mn0.54Co0.13O2) prepared via an environmentally friendly aqueous solution-gel and co-precipitation route, respectively. The solution-gel (SG) synthesized material shows a Ni-enriched spinel-type surface layer at the {200} facets, which, based on our post-mortem high-angle annual dark-field scanning transmission electron microscopy and selected-area electron diffraction analysis, could partly explain the retarded voltage fade compared to the co-precipitation (CP) synthesized material. In addition, deviations in voltage fade and capacity fade (the latter being larger for the SG material) could also be correlated with the different particle morphology obtained for both materials.

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40

Alqahtani, Yahya M., and Quinton L. Williams. "Reduction of Capacity Fading in High-Voltage NMC Batteries with the Addition of Reduced Graphene Oxide." Materials 15, no. 6 (March 15, 2022): 2146. http://dx.doi.org/10.3390/ma15062146.

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Lithium-ion batteries for electric vehicles (EV) require high energy capacity, reduced weight, extended lifetime and low cost. EV manufacturers are focused on Ni-rich layered oxides because of their promising attributes, which include the ability to operate at a relatively high voltage. However, these cathodes, usually made with nickel–manganese–cobalt (NMC811), typically experience accelerated capacity fading when operating at a high voltage. In this research, reduced graphene oxide (rGO) is added to a NMC811 cathode material to improve the performance in cyclability studies. Batteries made with rGO/NMC811 cathodes showed a 17% improvement in capacity retention after 100 cycles of testing over a high-voltage operating window of 2.5–4.5 V.

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Phattharasupakun, Nutthaphon, Juthaporn Wutthiprom, Salatan Duangdangchote, Sangchai Sarawutanukul, Chanikarn Tomon, Farkfun Duriyasart, Suchakree Tubtimkuna, Chalita Aphirakaramwong, and Montree Sawangphruk. "Core-shell Ni-rich NMC-Nanocarbon cathode from scalable solvent-free mechanofusion for high-performance 18650 Li-ion batteries." Energy Storage Materials 36 (April 2021): 485–95. http://dx.doi.org/10.1016/j.ensm.2021.01.032.

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Gomez‐Martin, Aurora, Friederike Reissig, Lars Frankenstein, Marcel Heidbüchel, Martin Winter, Tobias Placke, and Richard Schmuch. "Magnesium Substitution in Ni‐Rich NMC Layered Cathodes for High‐Energy Lithium Ion Batteries (Adv. Energy Mater. 8/2022)." Advanced Energy Materials 12, no. 8 (February 2022): 2270029. http://dx.doi.org/10.1002/aenm.202270029.

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Dose, Wesley M., Jennifer P. Allen, Christopher A. O'Keefe, Israel Temprano, Erik Björklund, Robert S. Weatherup, Clare P. Grey, and Michael F. L. De Volder. "Anodic Stability of Electrolyte Solvents and Additives at the Ni-Rich NMC Cathode-Electrolyte Interface in Li-Ion Batteries." ECS Meeting Abstracts MA2021-01, no. 2 (May 30, 2021): 87. http://dx.doi.org/10.1149/ma2021-01287mtgabs.

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Tatara, Ryoichi, Yang Yu, Pinar Karayaylali, Averey K. Chan, Yirui Zhang, Roland Jung, Filippo Maglia, Livia Giordano, and Yang Shao-Horn. "Enhanced Cycling Performance of Ni-Rich Positive Electrodes (NMC) in Li-Ion Batteries by Reducing Electrolyte Free-Solvent Activity." ACS Applied Materials & Interfaces 11, no. 38 (August 21, 2019): 34973–88. http://dx.doi.org/10.1021/acsami.9b11942.

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Qi, Gongshin, Jiazhi Hu, Michael P. Balogh, Lei Wang, Shubha Nageswaran, Nicholas Pieczonka, and Wei Li. "Impact of Ni Content on the Structure and Electrochemical Performance of the Co-Free, Li/Mn-Rich Layered Cathode Materials." ECS Meeting Abstracts MA2022-01, no. 2 (July 7, 2022): 377. http://dx.doi.org/10.1149/ma2022-012377mtgabs.

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Since early 1990s lithium-ion batteries (LIBs) have become the most important secondary/rechargeable battery technology for portable electronic devices; and more recently for battery powered vehicles. Extensive research has been conducted on high-capacity electrode materials for LIBs due to the emerging demands for high energy density batteries for electric vehicles. Compared with the conventional cationic redox-based cathode materials, such as NMC, LMO and LFP, Li-excess, Manganese rich layered cathode (LLC) materials containing cationic and anionic redox process, show great potential as the next generation cathode materials because of their higher theoretical specific capacity and lower raw material cost. Our work has shown that Ni content of the Co-free, LLC materials, Li1.2NixMn0.8-xO2 (x = 0.12, 0.24, 0.30 and 0.36) prepared by a citric acid method, has a significant impact on the material structure, electrochemical performance, and thermal stabilities. Generally, the primary particle size increased as the Ni content increased with a primary particle size distribution in the range of 200–600 nm for the samples investigated. Monoclinic phase (C2/m) and spinel (Fd3m) phase depending on the content of Ni have been identified by XRD. With increasing Ni content, the fraction of the spinel phase decreased and eventually the pure layered structure was obtained on the samples at x = 0.30 and 0.36. Our work demonstrates that the charging and discharging capacities are determined by the Ni or Mn content. The highest charging and discharging capacities were achieved when x = 0.24. As Ni content increased, the first cycle coulombic efficiency decreased, and the thermal stability deteriorated. But, an increase in Ni content results in an increase in average discharge voltage, higher electrochemical stability of the layered structure, fast Li ions diffusivity. Li1.2Ni0.12Mn0.68O2 sample exhibited the best capacity retention and thermal stability among the tested samples. However, its specific energy density was limited due to the lowest average discharge voltage. The Li1.2Ni0.36Mn0.44O2 sample which contained the highest Ni content exhibited the worst thermal stability, but relatively higher specific energy density due to the highest average discharge voltage.

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Park, Jeong Hoon, Sang Hoon Sung, Sunhyung Kim, and Kyung Hyun Ahn. "Significant Agglomeration of Conductive Materials and the Dispersion State Change of the Ni-Rich NMC-Based Cathode Slurry during Storage." Industrial & Engineering Chemistry Research 61, no. 5 (January 25, 2022): 2100–2109. http://dx.doi.org/10.1021/acs.iecr.1c04205.

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Xue, Xiaoyin, Hao Zhang, Shuai Yuan, Liyi Shi, Yin Zhao, Zhuyi Wang, Haijun Chen, and Jiefang Zhu. "PEDOT:PSS @Molecular Sieve as Dual‐Functional Additive to Enhance Electrochemical Performance and Stability of Ni‐Rich NMC Lithium‐Ion Batteries." Energy Technology 8, no. 10 (August 31, 2020): 2000339. http://dx.doi.org/10.1002/ente.202000339.

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Desta, Gidey Bahre Bahre, and Yao Jane Hsu (b)*. "Using Synchrotron Techniques, Investigation of Electrochemical Interfaces in Ni-Rich NMC and Sulfide Electrolytes in All-Solid-State Lithium Metal Batteries." ECS Meeting Abstracts MA2022-02, no. 7 (October 9, 2022): 2610. http://dx.doi.org/10.1149/ma2022-0272610mtgabs.

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a Nano-electrochemistry Laboratory, Graduate Institute of Applied Science and Technology, National Taiwan University of Science and Technology, Taipei 106, Taiwan, R.O.C b National Synchrotron Radiation Research Center (NSRRC), Hsinchu, 30076, Taiwan, R.O.C In all-solid-state lithium metal batteries enable long cyclability of high voltage oxides cathode persistent problem for the large scale application as their underprivileged interfacial steadiness in contrast to sulfide solid-state electrolyte. In this context, the interfaces of the solid electrolyte and Ni-rich NMC811 active material are looked upon as interfacial chemical responses induced by delithiation. In this study, we monitor the impedance progress at the unstable electrode|electrolyte interface due to the electrochemical interfacial response and help us understand the complex nature of reactivity and degradation kinetics with the solid-solid interface redox decomposition, which makes decoupling each effect difficult. we investigated the interfacial phenomenon between LPSC and high voltage cathode NMC811. The effects of spontaneous retort by the side of the interface were separated, and the intrinsic electrochemical decomposition of LPSC was quantified. Moreover, we show that the notch of interfacial degradation surges and the presence of oxidation mechanisms. At the higher delithiation stage, the cathode might twitch structural defenselessness and oxygen utter and resulting in further stark degradation. This complex kinetic degradation behavior was investigated at the solid-solid interface in a delithiation NMC811 and SSE based on the local oxidation state of NMC811, and LPSC SE interfacial chemical response. In this work, we used various characterization techniques to investigate the interfacial phenomenon between LPSC|NMC811 combining EIS and advanced synchrotron techniques such as sXAS, XPS, XRF-XANES mapping, and In-situ Raman spectroscopy. Keywords: delithiation, Ni-rich cathode, Sulfide-solid-state electrolyte, interfacial reaction, Synchrotron XPS, XRF.

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Wulfmeier, Hendrik, Alexander Omelcenko, Daniel Albrecht, Detlef Klimm, Wassima El Mofid, Marc Strafela, Sven Ulrich, Andreas Bund, and Holger Fritze. "Thermal Stability of Materials for Thin-Film Electrochemical Cells Investigated by Thin-Film Calorimetry." MRS Advances 1, no. 15 (2016): 1043–49. http://dx.doi.org/10.1557/adv.2016.72.

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ABSTRACTPhase transformation enthalpies are determined using the recently developed measurement technique Thin-Film Calorimetry (TFC), which is based on piezoelectric resonators vibrating in thickness shear mode. They are applicable up to at least 1000 °C. To the best of our knowledge, no comparable TFC systems for such high temperatures exist.The experimental part is divided into two subsections. The first is addressed to a thermodynamic investigation on piezoelectric langasite crystals (LGS, La3Ga5SiO14) which are the key component of the TFC system. The specific heat capacity is measured on LGS crystals of three different manufacturers. It ranges from about 0.45 J g-1 K-1 at 40 °C to about 0.60 J g-1 K-1 at 1000 °C. Thereby, deviations of up to 5 % between the different crystals are detected. Thermal diffusivity data for Y-cut LGS crystals are determined as well. Here, a constant decrease with temperature is detected ranging from 0.48 mm2 s-1 at room temperature to 0.38 mm2 s-1 at 700 °C.The second part presents thin-film calorimetric investigation on thin films of the family Li-Ni-Mn-Co-Al-Oxide (NMC/NMCA). These cathode materials are investigated and compared when annealed in ambient air or 0.5 % H2/Ar up to 860 °C. Three stoichiometries are chosen: Li(Ni1/3Mn1/3Co1/3)O2, Li(Ni0.6Mn0.2Co0.2)O2, and Li(Ni0.6Mn0.2Co0.15Al0.05)O2. The samples show three or four phase transformations. In air, the samples crystallize in the range of 250-350 °C. In 0.5 % H2/Ar, the transformations occur at higher temperatures. Especially in air, stoichiometric NMC crystallizes at lower temperatures compared to Ni-rich compositions. Additional doping with Al enhances the thermal stability which shifts all phase transformations to higher temperatures in both atmospheres.

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Barai, Pallab, Mark Wolfman, Xiaoping Wang, Jiajun Chen, Arturo Gutierrez, Juan Garcia, Jianguo Wen, Tim Fister, Hakim Iddir, and Venkat Srinivasan. "Morphology of Transition Metal Carbonate Cathode Precursors." ECS Meeting Abstracts MA2022-02, no. 6 (October 9, 2022): 630. http://dx.doi.org/10.1149/ma2022-026630mtgabs.

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Increasing the capacity of cathode materials used for lithium-ion batteries is desirable, as it ultimately enhances the energy density. Due to their lower cost and reversible cycling capacity of 250 – 300 mAh/g, Li- and Mn-rich LMR-NMC oxides are strong candidates as next generation cathodes used in lithium-ion batteries. Apart from the atomic structure, morphology of the cathode particles also influence their performance. LMR-NMC cathode particles are usually constructed through a two-step cathode fabrication process, which involves initial coprecipitation of the Mn-rich carbonate based cathode precursors, and later calcination of these precursors with a lithium salt at elevated temperatures. The secondary particles generally maintain their as precipitated precursor morphologies even after high temperature calcination. Even though the primary particles do change their size during calcination, the rate of oxidation and lithiation experienced by the transition metal precursors depend substantially on the primary particle morphology. Hence, it is critical to understand and control both the primary and secondary particle morphologies obtained after the coprecipitation process. In the present context, carbonate based NMC cathode precursors containing only Mn, only Ni and only Co, is precipitated, along with equal amount of the transition metals (Ni0.33Mn0.33Co0.33CO3), using conventional batch reactors. NH4HCO3 is used as the source of carbonate anions during the coprecipitation process, and the entire reaction is conducted at 50°C. The obtained particle morphologies for different transition metals are shown in Figure 1(a) as visualized using high resolution TEM techniques. Except MnCO3, all other transition metals demonstrate aggregated morphologies, which most probably form through surface growth mechanisms. Competition between growth rate and surface energies that leads to the formation of single crystalline particles for MnCO3, and particulate features for other transition metals, are demonstrated in Figure 1(b). Multiscale computational methodologies are developed to elucidate the impact of reaction kinetics and thermodynamics on determining the overall primary and secondary particle morphologies. Influence of transition metal content and ammonia concentration in determining the final particle size and size distribution will be discussed as part of this study. Figure 1

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