bluuebunny/crossref_metadata_2025_split huggingface dataset:
The Effect of Solid Electrolyte Interphase on the Mechanism of Operation of Lithium-Sulfur Batteries
Authors: Markevich Elena , Salitra Gregory , Rosenman Ariel , Talyosef Yosef , Chesneau Frederick Francois , Aurbach Doron 
Published: February 2020

Composite sulfur–carbon electrodes were prepared by encapsulating sulfur into the micropores of highly disordered microporous carbon AC1 with micrometer-sized particles and and carbonized polyacrylonitrile (PAN) cloth. We demonstrated that in bis(fluorosulfonyl)imide (FSI) based ionic liquid and in organic carbonates based electrolyte solutions the performance of the obtained electrodes is governed by the formation of solid electrolyte interphase (SEI) during the initial discharge. In both types of the electrolyte solutions the formation of SEI starts at potentials lower than 1.5V vs. Li/Li+ (Fig.1). We attribute the process of the formation of SEI to the reaction of lithium polysulfides with FSI anions or organic carbonates, respectively. Subsequent galvanostatic cycling is characterized by one plateau voltage profile specific to quasi-solid-state reaction of Li ions with sulfur encapsulated in the micropores in solvent deficient conditions. The stability of the SEI thus formed, is critically important for the effective desolvation of Li ions participating in quasi-solid-state reactions.
We proved that realization of the quasi-solid-state mechanism is controlled not only by the porous structure of the carbon host but also by the nature of the electrolyte solution composition and the discharge cut off voltage value. We showed that the FEC-based electrolyte solution demonstrates improved capacity retention during charge–discharge cycling of S/C composite electrodes compared to the EC-based electrolyte. The obtained results are very promising for the development of SLS batteries with FEC-based electrolyte solution which is in progress.
The cycling behavior of these cathodes is highly dependent on sulfur loading. Despite cracking of the particles observed due to a large volume expansion of sulfur during the lithiation, the best performance and initial coulombic efficiency at room temperature in FSI-based IL electrolyte solutions were demonstrated by S–AC1 composite electrodes with a sulfur loading of 60 wt%. This sulfur loading prevents the access of electrolyte solution molecules to the micropores, and the quasi-solid-state reaction of Li ions with encapsulated sulfur occurs in a solvent free environment. This insight into the mechanism of operating of S–C composite electrodes provides a new approach to the development of new electrolyte solutions and additives for Li–S cells.

Figure 1
Electrolyte Decomposition in Li-S Cells
Authors: Hagen Markus , Joos Martin , Abert Michael , Fanz Patrik , Tübke Jens 
Published: February 2020

Li-S cells are attractive due to their high potential gravimetric energy density, but they achieve only low cycle numbers. A major reason for this is a continuous electrolyte decomposition during cycling. As low electrolyte/sulfur ratios are required for high gravimetric energy density, this electrolyte decomposition reduces the obtainable cycle number to below 50.
It is therefore extremely important to evaluate, reduce or ideally prevent this electrolyte decomposition by utilizing new electrolyte (additives), separators and protection layers.
Applying in-situ mass spectroscopy, the electrolyte decomposition has been characterized for Li-S cells with lithium metal anode, silicon anode and carbon anode with various electrolyte compositions, electrodes and cycling parameters. Electrolyte cracking leads to gaseous substances, some of which are created continuously while others show a maximum depending on the state of charge. Standard ether-based Li-S electrolytes (e.g. DME:DIOX) are unstable with Li metal anodes and will always limit the obtainable cycle number unless further protection devices are applied.
The attached figure demonstrates specific gaseous substances created in a Li-S cell during cycling between 1.8-2.6 V at 0.6 mA/cm².

Figure 1
Material Interactions Between Cathode Active Material and Conductive Components in Solid-State Lithium Batteries
Authors: Uhlenbruck Sven , Bünting Aiko , Dellen Christian , Finsterbusch Martin , Tsai Chih Long , Vaßen Robert 
Published: February 2020

Today’s conventional lithium ion batteries comprise organic liquid electrolytes, which allow high performance of the batteries, however, also cause problems due to their limited stability. A promising approach to solve these issues is to replace the liquid electrolyte by a ceramic lithium ion conductor thus creating a so-called solid-state battery. Ceramics in general offer a superior chemical and thermal stability compared to any organic material.
A challenge in solid-state batteries is the processing of a fully inorganic battery cell because of thermally or field activated high-energy treatments that are necessary to create an inherent contact between the functional layers. This work focuses on the interaction and diffusion phenomena of the cathode material LiFePO4 and typical current collector materials like aluminum, titanium, and carbon as a conductive additive. It turned out that the current collector species exhibited high diffusion into and chemical reaction with the cathode material during processing and significantly changed the electrochemical performance of the cathode material. Planar and compact thin-film batteries manufactured by physical vapor deposition (PVD) were used to study this behavior in more detail by scanning electron microscopy, X-ray diffraction, cyclic voltammetry and secondary ion mass spectrometry (SIMS). Especially SIMS benefits from the thin-film approach on planar geometry with smooth surfaces and interfaces, along with pure LiFePO4 cathodes, to identify for example interdiffusion phenomena or chemical reactions.
The capacity of the pure LiFePO4 cathode layers was significantly lower than the theoretical capacity of 170 mAh/g. LiFePO4 is well known to be a material with extremely low electronic conductivity, and the lower capacity has been also attributed to this issue. Carbon is usually added to this active material to circumvent this drawback, as done with all cathode materials applied in conventional lithium ion batteries. After PVD processing of the cathode material with additional carbon, where carbon was already added to the sputter target, the cathodes had a capacity in the range of the theoretical one. This is not only accounted for a higher electronic conductivity – surprisingly, the microstructure completely changed from an apparently dense layers of LiFePO4 without carbon to a highly porous morphology consisting fibers with dimensions of the order of 100 nanometers with clear spacings of about 100 nanometer between them. As an outlook, these layers could also be used in lithium batteries with liquid electrolyte, featured by apparently continuous LiFePO4 wires instead of LiFePO4 powder stuck together with polymeric binders.
Systematic Investigation of an All-Solid-State Li-Ion Battery
Authors: Zhang Wenbo , Weber Dominik , Zeier Wolfgang G. , Janek Jürgen 
Published: February 2020

Towards the improvement of the state-of-art lithium-ion battery with liquid electrolyte, all-solid-state battery (ASSB) has become one of the most promising systems in the near future, due to the enhancement in the aspect of safety and volumetric energy efficiency. Even though thin film ASSBs have shown excellent performance, it is not suitable for large-scale applications due to its limited size. Therefore, development of bulk ASSB has gained great attentions in recent years. Different inorganic solid electrolytes (SE) have been intensively synthesized and investigated. The electric conductivity was thought to be the limiting factor. But it is no longer a big issue with the constant improvement of conductivity up to 1.2 * 10-2 S/cm.[1] On the other hand, the cell performance is limited to the high interfacial resistance generated between active material and solid electrolyte. A highly resistive layer at the interface between LiCoO2 and sulfide SE was reported.[2] This was considered to be the formation of space-charge layer or the mutual diffusion of elements between oxide cathode material and sulfide SE. [2,3] One of the solutions is the interposition of a buffer layer, which suppressed the increase of interfacial resistance and enabled the high-rate cycle of the ASSB.[4]

However, a detailed study of the ASSB system was not yet reported. In this poster, an ASSB composed of oxide cathode and sulfur based SE will be introduced. The schematic diagram of the cell is shown in Figure 1. The design and the structure of the cell, characterizations of cell components with XRD, SEM and electrochemical impedance will be shown. The relationship between the design of composite cathode and the long cycle stability and rate performance of assembled cells will also be revealed. The influence of interfacial resistance between oxides and sulfide based SE on the cell performance will be discussed. The reasons for the capacity fading observed during cycling will be analyzed and possible solutions will be proposed.
[1] N. Kamaya, K. Homma, Y. Yamakawa, M. Hirayama, R. Kanno, M. Yonemura, T. Kamiyama, Y. Kato, S. Hama, K. Kawamoto, A. Mitsui, Nat. Mater.
2011, 10, 682.
[2] N. Ohta, K. Takada, L. Zhang, R. Ma, M. Osada, T. Sasaki, Adv. Mater.
2006, 18, 2226.
[3] A. Sakuda, A. Hayashi, M. Tatsumisago, Chem. Mater.
2010, 22, 949.
[4] N. Ohta, K. Takada, I. Sakaguchi, L. Zhang, R. Ma, K. Fukuda, M. Osada, T. Sasaki, Electrochem. commun.
2007, 9, 1486.

Figure 1
High Energy Density Aqueous Electrochemical Capacitors with a KI-KOH Electrolyte
Authors: Wang Xingfeng , Chandrabose Raghu Subash , Chun Sangeun , Zhang Tianqi , Evanko Brian , Jian Zelang , Boettcher Shannon Wachter , Stucky Galen , Ji Xiulei 
Published: February 2020

We report a new electrochemical capacitor with an aqueous KI-KOH electrolyte that exhibits a higher specific energy and power than the state-of-the-art nonaqueous electrochemical capacitors. In addition to electrical double layer capacitance, redox reactions in this device contribute to charge storage at both positive and negative electrodes via a catholyte of IOx
-/I- couple and a redox couple of H2O/Had on the negative electrode, respectively. Here, we, for the first time, report utilizing IOx
-/I- redox couple for the positive electrode, which pins the positive electrode potential to be 0.4-0.5 V vs. Ag/AgCl. With the positive electrode potential pinned, we can polarize the cell to 1.6 V without breaking down the aqueous electrolyte so that the negative electrode potential could reach -1.1 V vs. Ag/AgCl in the basic electrolyte, greatly enhancing energy storage. Both mass spectrometry and Raman spectrometry confirm the formation of IO3
- ions (+5) from I- (-1) after charging. Based on the total mass of electrodes and electrolyte in a practically relevant cell configuration, the device exhibits a maximum specific energy of 7.1 Wh/kg, operates between -20 to 50 °C, provides a maximum specific power of 6222 W/kg, and has a stable cycling life with 93% retention of the peak specific energy after 14,000 cycles.
Carbon Electrodes for Potassium-Ion Batteries
Authors: Jian Zelang , Luo Wei , Xing Zhenyu , Bommier Clement , Li Zhifei , Ji Xiulei 
Published: February 2020

Large-scale stationary energy storage demands technologies based on Earth abundant elements. The scarcity and rising cost of lithium resources necessitate alternative storage devices to Li-ion batteries. To date, Na-ion batteries receive most attention; however, the challenge associated to the carbon anodes may potentially affect its commercialization. Here, we demonstrate that all major bulk carbons, including graphite, soft carbon, and hard carbon, can reversibly store K-ions in non-aqueous electrolytes at room temperature. All carbon electrodes can exhibit a high reversible capacity near 270 mAh/g. In particular, ex situ XRD studies on graphite electrodes confirm that KC36, KC24, and KC8 sequentially form upon potassiation, whereas depotassiation recovers graphite through phase transformations in an opposite sequence. Graphite shows moderate rate capability and relatively fast capacity fading. In contrast, we discover that both soft carbon and hard carbon exhibit much enhanced rate capability and cyclability compared to graphite. Cycling of hard carbon is the most stable. Interestingly, we determined that the hard carbon exhibits an unambiguously better rate capability in K-ion batteries than in Na-ion batteries. These works may open up a new paradigm toward rechargeable K-ion batteries.
Electrification of Urban Public Transportation Networks
Authors: Patey Timothy John 
Published: February 2020

Sustainable mobility includes powering urban public transportation systems with renewable energy. This CO2-neutral vision means replacing diesel bus fleets with all-electric ones. The use of wayside and on-board battery energy storage systems are presented as a way to replace diesel with electric buses, while releasing no particulate matter in the urban surroundings. Through the use of high-power battery design, opportunity charging, and understanding traffic impact, electric bus transportation networks are able to support the life of today’s growing cities.
In this work, the overview and parameterization of an electro-thermal-aging model of a high power Li-ion battery to represent battery use cases in an urban electric bus is presented. The advantages and shortcomings of battery models are discussed as an engineering tool in dimensioning prototypes.
On Uncertainty Quantification of Thermal Aspects of Lithium-Ion Battery
Authors: Esfahanian Vahid , Dehghandorost Hojat , Chaychizadeh Farzin , Ansari Amir Babak 
Published: February 2020

Thermal management of lithium-ion battery pack in hybrid electric vehicles (HEVs) and electric vehicles (EVs) have become a research focus in recent years because performance, safety and life time of battery have significant dependency on temperature distribution throughout the cell. As the first step in designing a reliable thermal strategy, heat generation of battery must be computed accurately. But the most effective physical properties involved in heat source may not be exactly known, possibly because of intrinsic variability which cannot be measured directly in practice.
In any simulation process, some uncertainties appear whose understanding and quantification is critical to assess the differences between the numerical predictions and actual system behavior. For this purpose, these uncertainties must be quantified and propagated through energy equation and heat flux to roll up the uncertainties of interest in order to determine range of temperature distribution, and consequently improve the safety and increase the life-cycle of lithium-ion battery.
Commonly, the uncertain model parameters are represented by random variables/processes which are known as probabilistic techniques. In the present study, stochastic spectral methods based on polynomial chaos (PC) expansions is employed due to their advantages over traditional uncertainty quantification (UQ) techniques, i.e., perturbation-based and Monte Carlo sampling (MCS) methods. In PC-based method, the coefficients of the solution expansion are computed intrusively or non-intrusively. Non-intrusive methods depend on individual realizations to determine the stochastic model response to random inputs and consume less time in comparison with intrusive methods. Since governing equations of lithium-ion battery are very complex, non-intrusive method is chosen in the present study.
Numerical simulation results are verified by discharge process at different C-rates which show good agreement with previous studies. Moreover, PC-based model is implemented to study the effects of parametric model uncertainties on the heat generation of cell and temperature distribution. The obtained numerical results can be used to design more efficient thermal management strategy. Moreover, the numerical results show that the proposed UQ method can accurately compute the variability in the output quantity of interest such as the heat generation and temperature distribution within a wide range of heat convection coefficients for lithium-ion battery.
Measurement of Thermal Behaviour from a Cell Under Operating Loads and Temperatures
Authors: Charles Terrance Priestley 
Published: February 2020

This study looks to predict the thermal behaviour of a battery, from cell level upwards, under a variety of operating loads and temperatures in order to improve battery efficiency. Battery charge and discharge behaviour depend on the electrochemical reactions at cell level and these are temperature dependent. A difference between the temperatures in individual cells can alter the performance of an EV, as well as affect the life of a battery pack[TC1] . It is the purpose of this research to understanding how thermal energy is generated at a cell level and how this energy migrates through the cell and into the battery. This understanding will be used to develop predictive assessment of the thermal behaviour of the battery under loading conditions typically experienced within an EV application. This will enable development of targeted interventions that can control the generation and management of thermal energy within the battery leading to a more efficient operation and less battery degradation over the long term.
[TC1]Examples - % degradation
Life expectancy change?
Multifunctional Silicon Anode for Lithium-ion Batteries
Authors: Bélanger Daniel , Assresahegn Birhanu Desalegn 
Published: February 2020

A silicon anode is prepared for application in lithium-ion batteries that can serve different functions such as decreasing the amount of the binder and thus allowing a larger quantity of the active material, better overall integration of the electrode components upon cycling and better stability of the solid-electrolyte interface that could enable to completely get rid of the expensive electrolyte additives. The synthesis of the materials involves the functionalization of a hydrogenated silicon nanopowder by covalent attachment of polyacrylic acid that partially substitutes the silicon-oxygen bond via a silicon-carbon bond. The presence and grafting of polyacrylic acid is confirmed by transmission and scanning microscopy and energy dispersive X-ray spectroscopy, thermogravimetric analysis, Fourier transform infrared and X-ray diffraction spectroscopy. The electrochemical performance of the silicon anode is evaluated by galvanostatic cycling, cyclic voltammetry and four point-probe electronic conductivity measurements. The composite silicon anode showed a significantly improved performance, relative to the hydrogenated Si electrode in terms of gravimetric capacitance (1200 mAh g-1 for more than 100 cycles at 0.5 C rate) with a 100 % capacity retention in a capacity limited discharge/charge cycling. When an unmodified and modified-based electrodes are allowed to fully discharge/charge, a lower initial capacity loss and a better overall physical integrity of the structure is achieved for the latter. Moreover, the composite electrode performs better at high rate discharge/charge cycles. Unlike reports making use of an electrolyte additive for silicon anode, mainly to afford stability of the solid-electrolyte interface and better cyclability, the polyacrylic acid (PAA) modified silicon composite electrode can be cycled without such additive and demonstrate a better electrochemical performance than the unmodified silicon.

Reference:

[1] S. Yang, Q. Pan, J. Liu, Electrochem.
Commun.
2010, 12, 479.
[2] B. D. Assresahegn, T. Brousse, D. Bélanger, Carbon
2015, 92, 362–381.
[3] B. D. Assresahegn, D. Bélanger, Adv.
Funct. Mater.
2015, 25, 6775.
[4] M. P. Stewart, J. M. Buriak, Comments Inorg. Chem.
2010, 23, 179.
[5] C. Martin, M. Alias, F. Christien, O. Crosnier, D. Bélanger, T. Brousse, Adv. Mater.
2009, 21, 4735.
[6] C. Martin, O. Crosnier, R. Retoux, D. Bélanger, D. M. Schleich, T. Brousse, Adv. Funct. Mater.
2011, 21, 3524.

Figure 1
High Lithium Storage Properties of MnFe2O4 Mesoporous Microspheres As an Anode Material for Li-Ion Batteries
Authors: Sunkara Satyendar 
Published: February 2020

Lithium-ion batteries (LIBs) have attracted tremendous attention because of their sustai-nability, high energy density, long cycle life and environmental benignity. Apart from these, LIBs have great potential applications in electric vehicles, potable electronics, solar and wind-based electricity generation systems and renewable energy storage. LIBs became prominent power sources as the non-renewable fossil-fuels result in massive air pollution and depleting very fast. Considering the scarcity, environmental benignity and cost, it is important to develop low cost, high abundance and eco-friendly electrode materials for LIBs which can deliver high energy and power densities with long cycle lives. Manganese ferrite, MnFe2O4 is one of the binary metal oxides and belongs to iron spinel which has been studied widely for its application in drug delivery supercapacitors and in magnetic devices. However, to the best of our knowledge, there have been only a few studies on the application of MnFe2O4 as anode materials for LIBs although it possesses a high theoretical capacity of 930 mA g-1, which is much higher than that of commercial graphite anode. But MnFe2O4 suffers from poor cycling stability because of the large volume changes during lithiation/delithiation. Here, mesoporous microspheres of MnFe2O4 have been successfully synthesized by a facile method followed by a post heat treatment. The mesoporous MnFe2O4 electrodes exhibit high reversible capacity of 733 mA h g-1 after 50 cycles at the current density of 100 mA g-1 indicating the excellent cycling stability. The cell delivered discharge capacities of 1371, 1008, 876, 625, 523, 380 mA h g−1 at current densities of 100, 200, 400, 800, 1000, 1500 mA g−1, respectively. Even at a high current density of 1000 mA g−1, the electrode could deliver a discharge capacity of 523 mA h g−1, which is much higher than the theoretical capacity of graphite. Interestingly, even after stepwise increment in the current densities while measuring the rate capability, the electrode retains a capacity of 812 mA h g−1 when the current rate reverts back to 100 mA g−1. We believe that such good performance results from the mesoporous nature of MnFe2O4 microspheres, which can substantially absorb large volume changes due during Li+ insertion/extraction.

Figure 1
Parsing the Battery Lithium Supply Chain: A Quantitative as well as a Qualitative View of Lithium Mining, Refining, and its Use in Fabricating Storage Battery Components
Authors: Lifton Jack P 
Published: February 2020

The identification of mineable deposits of lithium in brines; hard rock; or clay is just the beginning of a process to complete a supply chain for storage battery components that is strictly controlled by two comprehensive factors: 1, The economics of the best available technologies; and 2, The geopolitics of the regions and nations in which the deposits are located. The broad spread of the use of EVs, HEVs, and PHEVs may well depend on the fact that the best manufacturing technologies for them are located in East Asia while the largest deposits of the necessary lithium and other elements are located in South America; Africa; and Australia.
Lithium itself is a relatively cheap commodity today. What will be the effect of a global demand exceeding supply in the near term and in the long term. Can mining and refining keep up with government subsidized demand?