Impact of Cathode Material Particle Size on the Capacity of Bulk-Type All-Solid-State Batteries

Strauss, Florian; Bartsch, Timo; Biasi, Lea de; Kim, A‐Young; Janek, Jürgen; Hartmann, Pascal; Brezesinski, Torsten

doi:10.1021/acsenergylett.8b00275

Cited by 248 publications

(279 citation statements)

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“…[28,33,34] For this reason, sulfidebased SSBs will require coated cathode materials in order to avoid reactions between the SE and the CAM, thereby preventing the oxidation of the SE. Additionally, state-of-the-art CAMs undergo significant volume changes during lithium (de) intercalation (Figure 2c), [35,36] which often leads to detrimental contact loss within the composite cathode ( Figure 2d). [27] It will therefore be of interest to explore whether coatings can mechanically confine CAMs in order to reduce such volume changes, which may mitigate crack formation as well, or perhaps enhance adhesion within the cathode composite in order to prevent contact losses.…”

Section: Cam Coatings For Ssbs: General Considerationsmentioning

confidence: 99%

On the Functionality of Coatings for Cathode Active Materials in Thiophosphate‐Based All‐Solid‐State Batteries

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Koerver

Zeier

et al. 2019

Advanced Energy Materials

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achievable by SSBs. Meanwhile, polymer-, oxide-, and sulfide-based ionic conductors are being heavily investigated as the solid electrolyte (SE) separator. [9][10][11][12][13][14][15] Nevertheless, recent estimates [16,17] show that only batteries possessing sulfide-based SEs will be leading contenders for room-temperature applications.The sulfides, which are better denoted as thiophosphates, provide the highest lithium-ion conductivity, a relatively low E modulus, and can be processed at low temperatures. [2,3,18] Currently, only thiophosphates allow for the preparation of thick cathode composites with sufficient rate capability. [19,20] Unfortunately, thiophosphates also have a rather narrow electrochemical stability window, i.e., the onset of oxidative decomposition begins even before 3 V versus Li + /Li due to S(0)/S(−2) redox reactions, while reductive decomposition is theoretically expected at potentials of about 1.7 V versus Li + /Li due to P(+5)/P(−3) redox reactions. [21,22] Importantly, the perfect SE does not actually exist. The perfect SE would combine the ionic transport properties of thiophosphates, the mechanical properties of polymers, and the oxidation stability of oxides. Therefore, in order to exploit the superionic transport properties of thiophosphates, the implementation of protective coatings to overcome the intrinsic electrochemical instabilities is most certainly a necessity. The thermodynamic prerequisites for coatings (Figure 1) have already been treated in a number of theoretical papers, [18,21,[23][24][25] which provide the initial design guidelines.Beyond the thermodynamic considerations, it is well known that within SSBs, thiophosphate SEs are oxidized and decomposed in direct contact with cathode active materials (CAMs), in particular at high potentials during charging. [2,[26][27][28] Several years ago, Takada summarized the early work on SSBs and described the need for coatings against the formation of space charge layers at the interface between high-voltage cathodes and thiophosphate SEs. [29] Haruyama et al. concluded from density functional theory calculations that space charge layers between LiCoO 2 (LCO) and thiophosphate-based SEs are responsible for high impedances and that the addition of a buffer layer reduces such effects. [30] However, experimental evidence for such claims has not yet been reported. While these considerations are certainly valuable, from a current perspective, effects arising from the space charge layer are likely overstated and the role of oxidative degradation of the SE is understated. [31] Though the The last decade has seen considerable advancements in the development of solid electrolytes for solid-state battery applications, with particular attention being paid to sulfide superionic conductors. Importantly, the intrinsic electrochemical instability of these high-performance separators highlights the notion that further progress in the field of solid-state batteries is contingent on the optimization of component material interfaces in order to se...

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Section: Cam Coatings For Ssbs: General Considerationsmentioning

confidence: 99%

On the Functionality of Coatings for Cathode Active Materials in Thiophosphate‐Based All‐Solid‐State Batteries

Culver

Koerver

Zeier

et al. 2019

Advanced Energy Materials

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“…[129] Operando XRD is well suited to analyze crystallographic changes under dynamic conditions, for example during electrochemical cycling, and several studies have reported on the lattice parameter changes of NCM CAMs with cycling, [17,18,53,61,63,104,[129][130][131][132][133][134] but only few of them revealed sufficient time and angular resolutions. Crystallographic volume changes and multiphase transformations are assumed to be responsible for the capacity fading and to be one of the main factors governing the material fatigue.…”

Section: Crystallographic Changes In Ncmmentioning

confidence: 99%

Chemical, Structural, and Electronic Aspects of Formation and Degradation Behavior on Different Length Scales of Ni‐Rich NCM and Li‐Rich HE‐NCM Cathode Materials in Li‐Ion Batteries

et al. 2019

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costs are required. Current state-of-theart LIBs using, e.g., well-established LiNi 1/3 Co 1/3 Mn 1/3 O 2 (NCM111) cathode material are yet not able to fulfill all these demands. In order to increase the energy density of LIBs, battery produ cers and researchers pursue various strategies. Substitution of expensive Co by Ni to achieve LiNi 1−x−y Co x Mn y O 2 compounds with x < 0.3 in order to increase the structural stability at high state-of-charge (SOC) is one possible approach. Another promising material class is represented by Li-rich high-energy NCM (HE-NCM) materials (cLi 2 MnO 3 ⋅[1 − c]LiTMO 2 [TM = Ni, Co, Mn, etc.]). All of these subgroups of layered oxides have in common a crystal structure that is prone to irreversible changes and fatigue during continuous Li (de-)intercalation. The relevant changes in electronic and crystal structure strongly depend on the particular cathode composition and micro/nanostructure. The development of a target-oriented roadmap to improved LIBs that meet the above requirements must address the underlying mechanisms on different cell levels, i.e., from the atomic level to the electrode level. A comprehensive summary of the properties and developments in the field of Ni-rich NCM [1][2][3][4][5][6][7][8][9] and Li-rich HE-NCM [10][11][12][13][14][15][16] has been presented recently In order to satisfy the energy demands of the electromobility market, both Ni-rich and Li-rich layered oxides of NCM type are receiving much attention as high-energy-density cathode materials for application in Li-ion batteries. However, due to different stability issues, their longevity is limited. During formation and continuous cycling, especially the electronic and crystal structure suffers from various changes, eventually leading to fatigue and mechanical degradation. In recent years, comprehensive battery research has been conducted at Karlsruhe Institute of Technology, mainly aiming at better understanding the primary degradation processes occurring in these layered transition metal oxides. The characteristic process of formation and mechanisms of fatigue are fundamentally characterized and the effect of chemical composition on cell chemistry, electrochemistry, and cycling stability is addressed on different length scales by use of state-of-the-art analytical techniques, ranging from "standard" characterization tools to combinations of advanced in situ and operando methods. Here, the results are presented and discussed within a broader scientific context. by several authors. Here, we focus on the detailed characterization of these materials on different length scales, including the processes during formation and fatigue.After a brief introduction of the different materials addressed here, their characteristic process of formation and mechanisms of fatigue are discussed with respect to cell chemistry, electrochemistry, and cycling stability. Based on the fundamental results of our experimental studies on the material level, the effect of formation and fatigue on different cell levels is evalu...

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“…The size and morphological controls of the cathode particles enhanced the physical contact with the SEs, thereby contributing to the formation of a facile lithium ion pathway that consequently improved the energy density of ASSLBs. Strauss et al recently evaluated the electrochemical performance of LiNi 0.6 Co 0.2 Mn 0.2 O 2 cathode with different particle sizes ( Figure a,b) . They revealed that the initial reversible capacity strongly depended on the particle size of the cathode material.…”

Section: Recent Progress In Electrode Materialsmentioning

confidence: 99%

“…g) Solid state NMR exchange spectroscopy measurements (1D and 2D) data of the mixture III, there are large change in off‐diagonal cross‐leak intensity after the little time, high mobility of the lithium ion. a–e) Reproduced with permission . Copyright 2018, American Chemical Society.…”

Section: Recent Progress In Electrode Materialsmentioning

confidence: 99%

“…The current sulfide‐ASSLB is compared with the conventional liquid LIB aimed at electric vehicle (EV) applications in Table 1 . Note that the reported electrode gravimetric energy density of the full‐cell of ASSLBs lags those of the conventional LIBs, being below 61% . The battery research consists of 1) material engineering to improve the material's electrochemical performances, 2) electrode design to maximize the electrode properties such as energy density, rate capability, and cycle ability, and 3) battery (package) system design.…”

Section: Introductionmentioning

confidence: 99%

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Advances and Prospects of Sulfide All‐Solid‐State Lithium Batteries via One‐to‐One Comparison with Conventional Liquid Lithium Ion Batteries

et al. 2019

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Owing to the safety issue of lithium ion batteries (LIBs) under the harsh operating conditions of electric vehicles and mobile devices, all‐solid‐state lithium batteries (ASSLBs) that utilize inorganic solid electrolytes are regarded as a secure next‐generation battery system. Significant efforts are devoted to developing each component of ASSLBs, such as the solid electrolyte and the active materials, which have led to considerable improvements in their electrochemical properties. Among the various solid electrolytes such as sulfide, polymer, and oxide, the sulfide solid electrolyte is considered as the most promising candidate for commercialization because of its high lithium ion conductivity and mechanical properties. However, the disparity in energy and power density between the current sulfide ASSLBs and conventional LIBs is still wide, owing to a lack of understanding of the battery electrode system. Representative developments of ASSLBs in terms of the sulfide solid electrolyte, active materials, and electrode engineering are presented with emphasis on the current status of their electrochemical performances, compared to those of LIBs. As a rational method to realizing high energy sulfide ASSLBs, the requirements for the sulfide solid electrolytes and active materials are provided along through simple experimental demonstrations. Potential future research directions in the development of commercially viable sulfide ASSLBs are suggested.

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Impact of Cathode Material Particle Size on the Capacity of Bulk-Type All-Solid-State Batteries

Cited by 248 publications

References 26 publications

On the Functionality of Coatings for Cathode Active Materials in Thiophosphate‐Based All‐Solid‐State Batteries

On the Functionality of Coatings for Cathode Active Materials in Thiophosphate‐Based All‐Solid‐State Batteries

Chemical, Structural, and Electronic Aspects of Formation and Degradation Behavior on Different Length Scales of Ni‐Rich NCM and Li‐Rich HE‐NCM Cathode Materials in Li‐Ion Batteries

Advances and Prospects of Sulfide All‐Solid‐State Lithium Batteries via One‐to‐One Comparison with Conventional Liquid Lithium Ion Batteries

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