Materials for Rechargeable Lithium-Ion Batteries
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energy storage (including batteries and capacitors↗
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Improved cycle stability and high-rate capability of LiNbO 3 -coated Li 3 VO 4 as anode material for lithium-ion battery
Lithium vanadate (Li 3 VO 4 ) has garnered considerable attention as an alternative negative electrode material for non-aqueous lithium-ion batteries due to its high capacity, energy efficiency, and stable discharge voltage. Nonetheless, the Li 3 VO 4 material displays a low rate capability, attributed mainly to its poor intrinsic electronic conductivity. Here, in this study, we report the synthesis of lithium niobate LiNbO 3 -coated Li 3 VO 4 (LVO@LNO) using a one-pot sol-gel method. The resulting LVO@LNO demonstrates a high reversible capacity of approximately 530 mAh/g, which is more than double that of free Li 3 VO 4 . To explore the effect of the LNO coating process on the morphological and structural properties, Raman, XRD, operando XRD, XPS, SEM and HTEM analyses were conducted. To explain the enhancement of electronic conductivity in our modified material after a LiNbO 3 coating, we conducted an Ex-Situ electrochemical impedance (EIS) and Density Functional Theory (DFT) computational study. Additionally, we designed a full cell utilizing a 1 wt% LNO-coated LVO anode and NMC-811 cathode. The cell yielded an output voltage of approximately 2.8 V with a high initial specific capacity of 350 mAh/g versus to the anode, at 1C with a capacity retention of 85 % after 100 cycles.
25 ENERGY STORAGE↗
Revisiting the Corrosion of the Aluminum Current Collector in Lithium-Ion Batteries
The corrosion of aluminum current collectors and the oxidation of solvents at a relatively high potential have been widely investigated with an aim to stabilize the electrochemical performance of lithium-ion batteries using such components. The corrosion behavior of aluminum current collectors was revisited using a home-build high-precision electrochemical measurement system, and the impact of electrolyte components and the surface protection layer on aluminum foil was systematically studied. The electrochemical results showed that the corrosion of aluminum foil was triggered by the electrochemical oxidation of solvent molecules, like ethylene carbonate, at a relative high potential. The organic radical cations generated from the electrochemical oxidation are energetically unstable, and readily undergo a deprotonation reaction that generates protons and promote the dissolution of Al3+ from the aluminum foil. This new reaction mechanism can also shed light on the dissolution of transitional metal at high potentials.
Environmental Molecular Sciences Laboratory↗
Effect of Calcination Temperature on the Electrochemical Properties of Nickel-rich LiNi0.76Mn0.14Co0.10O2 Cathodes for Lithium-ion Batteries
High energy density nickel (Ni)-rich layered LiNixMnyCozO2 (NMC, x = 0.6) materials are promising cathodes for lithium-ion batteries. However, several technical challenges, such as fast capacity fading, are hampering their large scale application. Herein, we demonstrate that a Ni-rich cathode LiNi0.76Mn0.14Co0.10O2 (NMC76) calcined at an optimal temperature of 750~775oC exhibits a high discharge capacity (~215 mAh g-1 when charged to 4.5 V) and an excellent high rate capability. Even at a 10C rate, it still exhibits a capacity of more than 160 mAh g-1 and retains ca. 79% of its initial capacity after 200 cycles. The high performance of NMC76 is directly related to its optimized primary particle size (that constitute the spherical secondary particles of >10 m) and cation mixing. Higher calcination temperature (= 800 oC) leads to rapid increase of primary particle size, poor cycling stability, and inferior rate capability of NMC76 due to its severe micro strain and crack formation upon repeated lithium ion de/intercalations. Therefore, NMC76 calcined at 750~775oC is a very good candidate for the next generation of Li ion batteries.
nickel-rich cathodes, calcination temperature, cyc↗
Focused Ion Beam Fabrication of LiPON-based Solid-state Lithium-ion Nanobatteries for In Situ Testing
Solid-state electrolytes are a promising replacement for current organic liquid electrolytes, enabling higher energy densities and improved safety of lithium-ion (Li-ion) batteries. However, a number of setbacks prevent their integration into commercial devices. The main limiting factor is due to nanoscale phenomena occurring at the electrode/electrolyte interfaces, ultimately leading to degradation of battery operation. These key problems are highly challenging to observe and characterize as these batteries contain multiple buried interfaces. One approach for direct observation of interfacial phenomena in thin film batteries is through the fabrication of electrochemically active nanobatteries by a focused ion beam (FIB). As such, a reliable technique to fabricate nanobatteries was developed and demonstrated in recent work. Herein, a detailed protocol with a step-by-step process is presented to enable the reproduction of this nanobattery fabrication process. In particular, this technique was applied to a thin film battery consisting of LiCoO 2 /LiPON/a-Si, and has further been previously demonstrated by in situ cycling within a transmission electron microscope.
25 ENERGY STORAGE↗
Understanding thermal and mechanical effects on lithium plating in lithium-ion batteries
Lithium plating is one of the main concerns for cell durability, as cyclable lithium and cell capacity are decreased during the process. Thermal and mechanical loads can influence cell behavior, including lithium plating driving forces, as suggested by the Arrhenius equation and the Bruggeman relation, respectively. Hence, a 1D and a 3D model are employed to study the thermal and mechanical effects on lithium plating in a lithium-ion battery with a high areal capacity (4 mAh/cm 2 ). The 1D model assumes uniform mechanical and temperature profile, while the 3D model is capable of capturing the nonuniformity of stress and temperature in the cell. Further, the effects of mechanical deformation and different temperatures on the process of lithium plating are investigated in this study. With the help of the 1D charging simulations, it is observed that lower temperatures increase the risk of lithium plating and the presence of mechanical deformations can accelerate its initiation. Furthermore, 3D charging simulations indicated that folds and boundaries of jellyrolls are more susceptible to lithium plating due to the higher stress concentration and lower temperature, respectively.
25 ENERGY STORAGE↗
Semiconducting Zn x Mo 3 S 13 -GO Chalcocarbogel: A High-Capacity and Stable Sulfur-Equivalent Conversion-Based Electrode for Lithium-Ion Batteries
Lithium–sulfur batteries with a sulfur electrode offer a theoretical capacity of ∼1672 mAh g –1 , but rapid capacity loss mainly constrains their practical application. This work introduces a semiconducting and amorphous Zn x Mo 3 S 13 -GO (x = 0.5) chalcocarbogel sulfur-equivalent electrode with superior capacity and stability for lithium-ion batteries (LIBs). The Zn x Mo 3 S 13 -GO is synthesized in solution under ambient conditions, and its local structure contains S–S, M-Q (M = Mo, Zn; Q = S, O), C–S, and Mo–Mo bonding motifs with Mo coordination environment closely related to Mo 3 S 13 anions, as determined by X-ray photoelectron spectroscopy, synchrotron X-ray scattering, X-ray absorption spectroscopy, and ab initio molecular dynamics simulations. The Li/Zn x Mo 3 S 13 -GO cell offers an initial discharge capacity of 1019 mAh g –1 at a rate of C/3. After the activation cycles, the Li/Zn x Mo 3 S 13 -GO cell demonstrates good cycling stability, retaining a discharge capacity of 519.4 mAh g –1 after 250 cycles with ∼99.98% Coulombic efficiency and excellent rate capabilities. Moreover, it provides an initial discharge capacity of ∼574 mAh g –1 and maintains a retention capacity of 279 mAh g –1 at 1C after 625 cycles. The Lewis acidic Zn 2+ ion enhances the Lewis basic polysulfide anchoring ability and reduces the dissolution of polysulfides produced during the redox process through Zn–S covalent interaction, while the semiconducting and amorphous structure of the chalcocarbogel increases the electrical and ionic conductivity. Furthermore, this work highlights chalcocarbogels’ potential for developing high-capacity and stable electrodes for LIBs.
25 ENERGY STORAGE↗
A Tunable 3D Nanostructured Conductive Gel Framework Electrode for High-Performance Lithium Ion Batteries
This study develops a tunable 3D nanostructured conductive gel framework as both binder and conductive framework for lithium ion batteries. A 3D nanostructured gel framework with continuous electron pathways can provide hierarchical pores for ion transport and form uniform coatings on each active particle against aggregation. The hybrid gel electrodes based on a polypyrrole gel framework and Fe3O4 nanoparticles as a model system in this study demonstrate the best rate performance, the highest achieved mass ratio of active materials, and the highest achieved specific capacities when considering total mass, compared to current literature. This 3D nanostructured gelbased framework represents a powerful platform for various electrochemically active materials to enable the next-generation high-energy batteries.
25 ENERGY STORAGE↗
Scalable Dry Printing Manufacturing to Enable Long-Life and High Energy Lithium-Ion Batteries
Slurry casting method dominates the electrode manufacture of lithium-ion batteries. The entire procedure is similar to the newspaper printing that includes premixing of cast materials into solvents homogeneously, and continuously transferring and drying the slurry mixture onto the current collector. As a market approaching US $80 billion by 2024, the optimization of manufacture process is crucial and attractive. However, the organic solvent remains irreplaceable in the wet method for making slurries, even though it is capital-intensive and toxic. In this paper, an advanced powder printing technique is demonstrated that is completely solvent-free and dry. Through removing the solvent and related procedures, this method is anticipated to statistically save 20% of the cost at a remarkably shortened production cycle (from hours to minutes). The dry printed electrodes outperform commercial slurry cast ones in 650 cycles (80% capacity retention in 500 cycles), and thick electrodes are successfully fabricated to increase the energy density. Furthermore, microscopy techniques are utilized to characterize the difference of electrode microstructure between dry and wet methods, and distinguish dry printing's advantages on controlling the microstructure. Finally, this study proves a practical fabrication method for lithium-ion electrodes with lowered cost and favorable performance, and allows more advanced electrode designs potentially.
25 ENERGY STORAGE↗
Halide Substitution Effects on Lithium-Ion Diffusion in Protonated Antiperovskites
Solid-state electrolytes (SSEs) for all-solid-state lithium-ion batteries are generating intense interest because these batteries can improve the safety and performance compared with devices fabricated with conventional, flammable liquid electrolytes. In these SSEs, it has been suggested that Li + ion diffusion in the grain boundaries is hindered and is a critical determinant of the overall ionic conductivity (σ). However, Li + ion diffusivities in the grain (D G ) and the grain boundary (D GB ) are difficult to determine experimentally, with few techniques capable of distinguishing the individual contributions. Here, we distinguished the D G and D GB for the protonated lithium antiperovskites (pLiAPs) SSEs: Li 2 OHCl, Li 2 OHBr, Li 2 OHF 0.1 Cl 0.9 , Li 2 OHF 0.1 Br 0.9 , and Li 2 OHCl 0.3 7Br 0.63 . The measurements were obtained directly from 7 Li pulsed-field gradient nuclear magnetic resonance (PFG-NMR) at 353 K. The 7 Li PFG-NMR echo profiles were composed of two primary components with additional secondary oscillatory components – the so-called NMR diffraction phenomenon. The length scale separating the two main components corresponds to a diffusion length of ~1.7 µm, which is thought to be the average grain size (by diameter). The short-range (≤ 1.7 µm) diffusion component associated with D G (≈10 -11 m 2 /s) varied minimally with halide substitution, while the long-range (≥ 1.7 µm) component D GB (≈10 -12 to 10 -15 m 2 /s) was highly sensitive to the substitution of halides and closely correlated with s. In addition, from the comparison of the ratio D GB /D G to D t (the Li + ion diffusion coefficient estimated from the rotational correlation time, t c ), it was determined that the contribution of D G to σ is negligible; 0.01 ~ 0.04 in the pLiAPs studied here. Finally, these insights provide fundamental understanding of the halide substitution effects on Li + ion grain versus grain boundary diffusion, and suggest that careful engineering of the grain boundaries at the microscopic level is necessary to achieve high-performance pLiAP SSEs.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Effects of cryogenic freezing upon lithium-ion battery safety and component integrity
Not Available
Sunderlin, Nathaniel↗
Mesoscale-architecture-based crack evolution dictating cycling stability of advanced lithium ion batteries
The cracking phenomenon of Ni-rich NMC (LiNixMnyCo1-x-yO2, x = 0.6) secondary particles is frequently discovered and believed to be one of critical reasons deteriorating the long-term cycling stability of NMC cathode in lithium ion batteries (LIBs). However, the initiation and evolution of those cracks is still controversial due to the limited quantification especially by in situ monitoring, leading to the challenge of identifying an efficient approach to inhibit the formation of the fractures during repeated cycling. Herein, the irreversible, anisotropic cycling lattice and mesoscale expansion/shrinkage of nano-grain during the first cycle, as revealed by in situ X-ray diffraction (XRD) and in situ atomic force microscopy (AFM), have been quantified and confirmed to be the dominant driving forces of microcracks initiation at the grain boundaries. These microcracks preferentially nucleates at the core region with random oriented nano-grains in early stage. The further growth and aggregation of microcracks into macrocrack eventually results in microfracture propagation radially outward to the periphery region with more uniform nano-grain orientation. This mesoscale nano-grain architecture controlled cracking process highlight the importance of predictive synthesis of cathode materials with controllable multiscale crystalline architecture for high-performance LIBs.
25 ENERGY STORAGE↗
Silicon-based anodes for lithium-ion batteries: Effectiveness of materials synthesis and electrode preparation
Lithium-ion batteries are widely used throughout the world for portable electronic devices and mobile phones and show great potential for more demanding applications like electric vehicles. Unfortunately, lithium-ion batteries still lack the required level of energy storage to completely meet the demands of such applications as electric vehicles. Among advanced materials being studied, silicon nanoparticles have demonstrated great potential as an anode material to replace the commonly used graphite. Silicon has been shown to have a high theoretical gravimetric capacity, approximately 4200 mA h/g, compared to only 372 mA h/g for graphite. Though silicon nanoparticles have remarkably high capacity, they suffer from rapid degradation with each cycle due to electrode volume expansion of approximately 400% during lithiation, placing a large strain on the material. With each cycle that strain creates cracks in the electrode particles and causes them to break down into smaller particles, which create void spaces between the particles and lead to poor contact as reflected in poor conductivity. In this review, we discuss exciting new research on silicon-based anodes conducted during the past couple of years. Besides stressing the importance of well-designed nanostructures of Si, we focus on optimization of the Si electrode and resulting performance enhancement by properly selecting binders and synergistically integrating them with various carbon materials during electrode design and fabrication. Importantly, although each improvement strategy has its own advantage, appropriate combination of them will yield much higher anode performance. We summarize the core issues in developing the silicon anode and effective strategies in yielding more promising results. (C) 2016 Elsevier Ltd. All rights reserved.
Casimir, Anix↗
Anomalous metal segregation in lithium-rich material provides design rules for stable cathode in lithium-ion battery
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99 GENERAL AND MISCELLANEOUS↗
A controlled nucleation and growth of Si nanowires by using a TiN diffusion barrier layer for lithium-ion batteries
Uniform size of Si nanowires (NWs) is highly desirable to enhance the performance of Si NW-based lithium-ion batteries.
36 MATERIALS SCIENCE↗
Helical Covalent Polymers with Unidirectional Ion Channels as Single Lithium-Ion Conducting Electrolytes
Single-ion conducting polymer electrolytes have attracted great attention as safe alternatives to liquid electrolytes in high energy density lithium-ion batteries. Herein, we report the first example of a crystalline anionic helical polymer as a single lithium-ion conducting solid polymer electrolyte (SPE). Single-crystal X-ray analysis shows that the polymer folds into densely packed double helices, with bundles of unidirectional negatively charged channels formed that can facilitate lithium-ion transportation. Such a helical covalent polymer ( HCP) exhibits excellent room temperature lithium-ion conductivity (1.2 x 10 -3 S cm -1 ) in the absence of external lithium salts, a high transference number (0.84), low activation energy (0.14 eV), and a wide electrochemical stability window (0.2-5 V). We found that nonflammable, nonvolatile ionic liquid can serve as a solvating medium and excellent conductivity enhancer (>1000 times increase). These ion-conducting properties are comparable to the best polyethylene oxide-based polymer electrolytes mixed with lithium salts. Finally, we show that the solvated HCP SPE enables the reversible cycling of an all-solid-state cell prepared with a high-voltage NMC 811 cathode. Our study opens up new possibilities for developing next-generation high-performance solid-state electrolytes.
25 ENERGY STORAGE↗