bluuebunny/crossref_metadata_2025_split huggingface dataset:
Model-Based SEI Layer Growth in EV and Phev Batteries for Standard Drive Cycles
Authors: Lawder Matthew T , Subramanian Venkat R. , Northrop Paul W. C. 
Published: February 2020

Capacity fade in electric vehicle batteries is caused through a number of mechanisms. Solid Electrolyte Interface (SEI) layer growth caused by side reactions at the battery anode is one of these mechanisms that results in loss of battery power and energy capacity. Reducing the growth of this layer can help increase battery life and overall utility of electric vehicles, especially near the end of their service life.
We use a model based approach to study how the SEI layer grows during different types of charging, specifically looking at how the regenerative braking portion of driving will contribute to SEI layer growth. Eight different drive cycles were used to analyze how different driving patterns contribute to SEI layer growth.
The battery model used for the study was a porous electrode pseudo two dimensional model.1 A mathematical reformulation of the model was used to increase computational efficiency and speed without greatly reducing model accuracy.2 Three different SEI layer growth equations from literature were studied for EV charging.3-5 SEI growth was studied for both charging and regenerative braking, during which the battery is being charged for short periods of time during driving cycles that are predominantly discharge.
Results show rates of SEI growth for driving duration (by time) and length (by distance traveled) and analyze similarities in the driving cycle characteristics that may lead similar SEI layer growth rates. Additionally, results look at the effects of different depth of discharge during cycling on the battery and how DOD affects the overall SEI layer growth.6

As EV batteries continue to go through cycles, the effects of SEI growth caused from different types of driving will become more pronounced. The results shown will help reveal how that SEI growth can be reduced through driving patterns.

References

1. M. Doyle, T. F. Fuller, and J. Newman, Journal of the Electrochemical Society,
140, (1993)
2. P. W. C. Northrop, B. Suthar, V. Ramadesigan, S. Santhanagopalan, R. D. Braatz, and V. R. Subramanian, Journal of the Electrochemical Society,
161, E3149(2014)
3. P. Ramadass, B. Haran, P. M. Gomadam, R. White, and B. N. Popov, Journal of the Electrochemical Society,
151, A196(2004)
4. M. Safari, M. Morcrette, A. Teyssot, and C. Delacourt, Journal of the Electrochemical Society,
156, A145(2009)
5. M. B. Pinson and M. Z. Bazant, Journal of the Electrochemical Society,
160, A243(2013)
6. M. T. Lawder, P. W. C. Northrop, and V. R. Subramanian, Journal of the Electrochemical Society,
161, A2099(2014)
Effect of Metal Nanoparticles on the Polysulfide Conversion Reactions in Rechargeable Li-Sulfur Batteries
Authors: al Salem Hesham , venkateswara Rao Chitturi , Ganguli Babu , Arava Leela mohana reddy 
Published: February 2020

Rechargeable lithium-sulfur (Li-S) batteries have emerged as the most promising electrochemical energy storage systems due to their high energy density, wide range of temperature operation, cost effectiveness, and eco-friendly in nature. Nevertheless, the drawbacks associated with the Li-S batteries such as insulating nature of sulfur species, corrosive nature of predeposited polysulfides at electrodes during discharge-charge processes, and formation of thick SEI layer still need to be circumvented. One of the promising ways to alleviate these problems is to use highly porous, conductive, and active species which can improve the kinetics of polysulfide conversion reactions and diffusion processes. In this context, we have investigated electronically conductive species incorporated graphene, specifically Metal/graphene hybrids (metal = Pt, Ni, and Co) as cathode in Li-S batteries and performed systematic studies to understand the electrochemical behavior of polysulfides during discharge-charge processes.
Metal/graphene hybrids were prepared through wet chemical routes and employed them as electrodes for the conversion of polysulfides in Li-S batteries. Structural and morphological techniques depicted phase purity of the materials and well-dispersed metallic nanocrystallites with an average size of 5 nm on the graphene sheets. Electrochemical studies were carried out by assembling Li/sulfur cells inside glove box using a porous metal/graphene as electrodes cathode, 0.6M Li2S8-1M LiTFSI in TEGDME as electrolyte, and metallic lithium as anode. Galvanostatic discharge-charge tests indicated a two-fold increment in the Li-S battery performance with metal/graphene compared to pure graphene. A high discharge capacity of 750 mAh/g at C-rates of C/10 has been observed with Pt/graphene. The studies on metal/graphene based Li-S battery revealed pivotal role of metallic nanoparticles in enhancing the polysulfide conversion processes.
# - Corresponding Author - leela.arava@wayne.edu
Reactions Between Deliathidated Cathodes and Electrolytes
Authors: Chen Zonghai , Amine Khalil 
Published: February 2020

The safety concern of lithium-ion batteries has been one of major technological barriers that hinder the deployment of lithium-ion batteries for automobile applications. As an alternative to conventional thermal analysis techniques like differential scanning calorimetry and accelerating rate calorimetry, an in situ high energy X-ray diffraction technique was established to investigate the decomposition mechanism of delithiated cathode materials at thermal abuse conditions. Figure 1 show a typical in situ high energy X-ray diffration data during the thermal abuse of delithated Li1.2Ni0.15Mn0.55Co0.1O2. In this talk, the mass/charge transfer throught the material interface will be disccused to illustrated the degration mechanism of delithiated cathode materials.

Figure 1
Beyond State of the Art: A Family of Novel and Highly Performing Electrolytes for Rechargeable Magnesium Batteries Based on Boron-Hydrogen Compounds
Authors: Mohtadi Rana , Tutusaus Oscar , Arthur Timothy S. , Zhang Ruigang , Carter Tyler , Mizuno Fuminori 
Published: February 2020

Owing to a high volumetric capacity (3833 mAh cm-3 vs. 2046 mAh mAh cm-3 for Li), absence of dendrites formation and lower cost of Mg metal (about 10 times cheaper than Li), rechargeable magnesium batteries have been receiving an increased attention. One major challenge facing these batteries is related to the electrolytes as they are restricted to a handful of corrosive halogen based magnesium reagents and complexes. Electrolytes based on conventional inorganic and ionic Mg salts, such as MgClO4, were found unsuitable due to their instability in the reducing environment of the Mg anode resulting in complete Mg passivation [1]. Overcoming the hurdles with current electrolytes calls for discovering new non-halo based systems that are compatible with Mg metal (Fig.1.a). Recently, motivated by the thermal stability and a presumed robustness of the BH4
- anion against electrochemical reduction, we proposed magnesium borohydride as an electrolyte beyond state of the art for rechargeable magnesium batteries [2]. Owing to a high reductive stability, we discovered that magnesium borohydride could withstand the reducing environment of Mg metal making it the first and so far only example of an inorganic, relatively ionic and halide free salt that could function as an electrolyte in Mg batteries. This breakthrough offered a path towards designing non-corrosive electrolytes and has been used as a basis to create a whole new family of highly performing systems, Fig.1.a [3]. For example, to increase the anodic stability of the B-H bond while preserving the attractive features of BH4
- anion, icosahedral boron clusters were proposed. Unlike the case in typical halo Mg reagents, which require the addition of a Lewis acid as AlCl3 to increase its anodic stability, we developed the Mg salt Mg(1,7-C2B10H11)Cl [3,4] that while displaying greater than 98% Mg deposition/stripping efficiency, demonstrates high anodic stability (3.2 V) and solubility (> 1M in tetrahydrofuran solvent) (Fig.1b).
Herein, we will explain our bottom up design strategies, discuss fundamental properties obtained from systematic spectroscopic and electrochemical studies and share up-to-date results related to these new promising systems.

References

[1] a. H. D. Yoo, I. Shterenberg, Y. Gofer, G. Gershinsky, N. Pour, D. Aurbach, Energy Environ. Sci. 2013, 6, 2265-2279; b. R. Mohtadi, F. Mizuno, Beilstein J. Nanotechnol. 2014, 5, 1291 –1311.
[2] R. Mohtadi, M. Matsui, T. S. Arthur, S.-J. Hwang, Angew. Chem. Int. Ed. 2012, 51, 9780 –9783.
[3] O.Tutusaus, R. Mohtadi, ChemElectrochem, DOI 10.1002/celc.201402207,2014.
[4] T. J. Carter, R. Mohtadi, T. S. Arthur, F. Mizuno, R. Zhang, S. Shirai, J. W. Kampf, Angew. Chem. Int. Ed. 2014, 53, 3173 –3177; Angew. Chem. 2014, 126, 3237– 3241.

Figure 1
Novel Highly Conductive Polymer Electrolytes for Li-Ion Batteries Applications
Authors: Leclere Melody , Mendil-Jakani Hakima , Rannou Patrice , Lyonnard Sandrine , Livi Sebastien , Gebel Gerard , Duchet-Rumeau Jannick , Picard Lionel 
Published: February 2020

One of the most important research topics in the field of Li-ion batteries is the substitution of the conventional liquid electrolytes by solid polymer electrolytes for increasing both safety and performances. But another approach concerning the conduction mechanisms of the Li+ has to be envisaged to increase the intrinsic performance of the polymer. Recently, a new approach has been developed by Armand & al [1,2]: they immobilize the anion on a block copolymer using STFSI[i] monomer for one block. But the conduction mechanism is still ensured by POE blocks.
In this work we developed a novel class of anionic epoxy polymer electrolytes, with noteable properties (thermotropic liquid crystalline), involving a new mode of Li+ mobility. The thermodynamic encryption given by the nature of different segment of the polymer lead to a self-organization of the polymer (columnar, lamellar, gyroid …). We propose that the anionic sites are thus organized for efficient Li-conduction by a hoping mechanism as presented in the figure below. The synthesis and electrochemical properties of this new crystalline polyelectrolyte were investigated. The preliminary results showed a RT conductivity over 0.1 mS.cm-1.

[i] 4-styrenesulfonyl)(trifluoromethanesulfonyl)imide
[1] Meziane, R; Bonnet, J.P; Courty, M; Djellab, K; Armand, M. Electrochimica Acta
, 2011, 57, 14
[2] Bouchet, R; Maria, S; Meziane, R. ; Aboulaich, A ; Lienafa, L ; Bonnet, J.P ; Phan, T. N. T. ; Bertin, D ; Gigmes, D. ; Devaux, D; Denoyel, R ; Armand, M. Nature Materials, 2013,12,452

Figure 1
Progress Towards Magnesium-Ion Batteries
Authors: Marschilok Amy C , Takeuchi Kenneth J , Takeuchi Esther S 
Published: February 2020

The efficient management of energy sources is critical to addressing future global energy demands. For example, the growing electrical energy storage needs of mobile and stationary devices demonstrate the need for rechargeable batteries with a variety of application-based performance capabilities, including sufficient energy density, appropriate voltage and current capabilities. One of the most successful and broadly implemented rechargeable battery technologies developed to date is lithium ion. However, questions regarding the future of using lithium ion technology for large scale applications center on the sustainability and high cost of lithium, especially due to the projected increase in demand for lithium based electrodes used in hybrid and plug in electric vehicles and stationary (grid) storage.
Of the possible alternatives to lithium ion, rechargeable magnesium-ion batteries are an intriguing candidate, and research into the technology has accelerated in recent years. Magnesium ion technology is promising due to divalent nature of Mg ions, presenting a potential advantage in terms of high volumetric capacity, the high natural earth abundance of magnesium, and higher atmospheric and thermal stability for magnesium metal relative to lithium metal.
One critical issue impeding progress in this area has been development of a suitable electrolyte-anode interphase which will enable reversible release of Mg2+ ions and reversible charge of Mg based anodes. A second fundamental challenge is the strong polarization of the small divalent Mg2+, requiring mitigation of the inherently slow ion diffusion associated with magnesium-ion cathodes. Progress toward viable Mg-ion battery systems will be described in this presentation, including recent achievements in the development of anodes, cathodes, and electrolytes.
Tailoring the Desired Surface Chemistry in Silicon-Based Lithium-Ion Batteries with Electrolyte Additives
Authors: Shi Feifei , Zhao Hui , Komvopoulos Kyriakos , Somorjai Gabor , Ross Philip N 
Published: February 2020

The design of safe, high-energy batteries exhibiting prolonged lifetime greatly depends on understanding the surface reactions occurring on the electrode surfaces and the role of the solid electrolyte interphase (SEI) film. Most of the naturally forming SEI films demonstrate undesirable characteristics, such as instability and continuous surface reaction that decrease the capacity of Si-based Li-ion batteries (LIBs). An effective and economic way to modify the surface chemistry in LIBs rather than the Si architecture is by electrolyte additives. The objective of the present study is the examination of the concentration dependence of vinylene carbonate (VC) and fluoroethylene carbonate (FEC) additives on the long-term electrochemical performance of LIBs, as well as the dependence of the SEI formation mechanism on the concentration of the VC and FEC additives.
A significant improvement in the cycling performance of Si electrodes can be achieved under operation conditions of optimum VC and FEC concentration. To better understand the additive concentration effect, the reduction mechanisms of VC and FEC were investigated for both Si nanoparticle and Si(100) single crystal working electrodes. Ex-situ ATR-FTIR spectra of Si electrodes for 5% VC additive show a broad peak at a higher wavenumber (1831 cm–1) compared to the EC residual electrolyte (1799 and 1769 cm–1) (Fig. 1). Based on synthesized poly-VC standard spectra, the VC additive reduction compound is assigned to poly-VC or its oligomer, which is consistent with previous reports. However, for Si electrode and FEC additive, the original C=O stretch (1829 and 1802 cm–1) disappears or shifts to a lower wavenumber. The exact reduction product of FEC degradation has not been confirmed yet due to the lack of significant features other than the residual electrolyte. However, it is clear that FEC follows a different reduction path than VC. The reduction path of VC is polymerization with the reduction product remaining a “ring” structure (the C=O peak shifts to a higher wavenumber), whereas the reduction path of FEC is similar to that of ethylene carbonate (EC), leading to a reduction product of open “ring” structure, similar to that produced from EC reduction. More experiments are underway to confirm the different reduction paths of VC and FEC stated above.

Acknowledgement

This work was supported by the Assistant Secretary for Energy Efficiency and Renewable Energy, Office of Freedom CAR and Vehicle Technologies of the U.S. Department of Energy under contract No. DE-AC02-OSCH11231.

Figure 1
Solvating Additives and Their Role in Increasing the Capacity of Nonaqueous Li-O2 Batteries
Authors: Viswanathan Venkatasubramanian 
Published: February 2020

The passivation of Li-O2 battery cathode by the electronically insulating Li2O2 limits the maximum attainable capacity in these batteries.[1] We show that electrolyte additives, such as tiny amounts of water, which activate solution-mediated growth of Li2O2, make it possible to circumvent this fundamental limitation and enable high capacity Li-O2 batteries. Design rules for choosing these solvent additives are presented.[2]

V. Viswanathan, K. Thygesen, J.S. Hummelshøj, J. K. Nørskov, G. Girishkumar, B.D. McCloskey, A. Luntz, J. Chem. Phys., 135, 214704 (2011).

N. B. Aetukuri, B. D. McCloskey, Jeannette M. García, L. E. Krupp, V. Viswanathan and A. C. Luntz, Nature Chemistry., DOI: 10.1038/nchem.2132 (2014).

Figure 1: Proposed mechanism for the growth of Li2O2 toroids in the presence of water.The deposition of Li2O2 in a Li-O2 cell is shown, schematically, to proceed via a surface electrochemical growth process. The presence of a additive (water in our experiments) that solvates LiO2
* to Li+ and O2
- triggering a solution mechanism. Design rules for additive engineering are presented in the contour plot.

Figure 1
An Experimental Investigation - How Much Influence Has the Electrolyte Composition on the Ageing Behaviour of Separators in Lithium-Ion Cells?
Authors: Kraemer Yvonne , Meiler Markus , Hintennach Andreas 
Published: February 2020

The most widely used liquid non-aqueous electrolytes for lithium-ion cells used in HEV (hybrid electric vehicle), PHEV (plug-in-hybrid electric vehicle) and EV (electric vehicle) applications consist of LiPF6 dissolved in carbonates (e.g. EC, DMC and DEC). These electrolytes undergo a variety of hydrolysis and thermal aging mechanisms [1]. Ongoing decomposition reactions lead to further impurities inside the lithium-ion cell which are not well-known. The separator is a second critical component in lithium-ion cells, which can be classified into three groups according to structure and composition: microporous polymer membranes, non-woven fabric mats and inorganic composite membranes [2].
In this contribution, the decomposition reaction mechanisms are evaluated under a number of different thermal conditions for various commercial electrolytes from automotive lithium-ion cells. Furthermore, their influences on the ageing behaviour of different separator types are investigated. Details of the experimental procedure, analytical methods (NMR, GC-MS, SEM/EDX) and first results will be presented. Finally, we will give an overview of our mechanistic interpretation.

References:

[1] P. Handel, G. Fauler, K. Kapper, M. Schmuck, C. Stangl, R. Fischer, F. Uhlig, S. Koller, J. of Power Sources
2014,
doi: 10.1016/j.jpowersour.2014.05.080
[2] S. Zhang,J. of Power Sources
2007, 164, 351 – 364

Acknowledgement:

This research is funded by the German Federal Ministry of Education and Research (BMBF) under the grant number 03X4631E within the cluster “excellence and technological implementation of Battery research (ExcellentBattery).
Effects of Doping on Lithium Rich NMC Cathode Prepared Via Spray Pyrolysis
Authors: Lengyel Miklos , Shen Kuan-Yu , Axelbaum Richard L. 
Published: February 2020

LixMO2(M= Mn, Ni, Co) materials with layered structures have received attention as high-capacity, low cost and safe cathode materials for lithium-ion batteries (1, 2). Various synthesis methods have been developed for the production of these materials, including co-precipitation, solid-state synthesis and ball milling. Recently a spray pyrolysis synthesis method has been developed by this group for producing cathode materials with porous morphologies and high tap density (3). Spray pyrolysis has certain advantages compared to other methods: the short residence time in the reactor allows large throughput; the process is scalable, no further post-synthesis purification steps are required and the product is inherently purified throughout the synthesis. Most importantly, each particle is synthesized with precise stoichiometry because each droplet behaves as a mini-reactor. This allows for accurate control of composition.
The layered lithium-nickel-manganese-cobalt oxides, such as Li1.2Mn0.54Ni0.13Co0.13O2 or 0.5 NMC are known to demonstrate a voltage fade over cycling. This effect has been attributed to a layered-spinel transformation (4). This study will focus on doping Li1.2Mn0.54Ni0.13Co0.13O2using trace level dopants and exploring their effects on voltage fade and cycling stability.
Figure 1 shows a typical SEM result of lithium rich material prepared via spray pyrolysis, demonstrating the uniform and spherical morphology. Figure 2 compares the effect of synthesis method for dopant free material synthesized via co-precipitation and spray pyrolysis, indicating distinct advantages both in terms of capacity and voltage fade for the material synthesized via spray pyrolysis, due to the superior uniformity of the synthesis method (5-7). Figure 3 shows the cycle test results for 0.5 NMC with Al doping. Al doping clearly improves the cycle stability of the sample.

Acknowledgements:

The authors are grateful to the NSF and X-tend Energy LLC for support. RLA and Washington University may receive income based on a license of related technology by the University to X-tend Energy LLC.

References:

1. C. S. Johnson, J. S. Kim, C. Lefief, N. Li, J. T. Vaughey and M. M. Thackeray, Electrochem. Commun., 6, 1085 (2004).
2. C. S. Johnson, N. C. Li, C. Lefief, J. T. Vaughey and M. M. Thackeray, Chem. Mater., 20, 6095 (2008).
3. M. Lengyel, D. Elhassid, G. Atlas, W. T. Moller and R. L. Axelbaum, J. Power Sources, 266, 175 (2014).
4. D. Mohanty, J. Li, D. P. Abraham, A. Huq, E. A. Payzant, D. L. W. III and C. Daniel, Chem. Mater. (2014).
5. D. Mohanty, S. Kalnaus, R. A. Meisner, K. J. Rhodes, J. Li, E. A. Payzant, D. L. W. III and C. Daniel, J. Power Sources, 229, 239 (2013).
6. M. Lengyel, X. Zhang, G. Atlas, H. L. Bretscher, I. Belharouak and R. L. Axelbaum, J. Electrochem. Soc., 161, A1338 (2014).
7. J. Zheng, M. Gu, A. Genc, J. Xiao, P. Xu, X. Chen, Z. Zhu, W. Zhao, L. Pullan, C. Wang and J.-G. Zhang, Nano Lett., 14, 2628 (2014).

Figure 1
In-Situ TEM Study of Intercalation- and Conversion-Driven Lithiation in Single Î±-MnO2 Nanowire
Authors: Yuan Yifei , Nie Anmin , Santhanagopalan Sunand , He Kun , Meng Dennis Desheng , Klie Robert F , Shahbzian-Yassar Reza 
Published: February 2020

Nano-sized transitional metal oxides (TMOs, M=Fe, Co, Cu, Mn, etc.) have been increasingly recognized as promising candidate anode for lithium ion battery (LIB) with high specific capacity (700–1200 mAh/g). The high capacity is achieved via a so-called reversible “conversion reaction” with Li+, as shown in Equation (1):
MxOy + 2yLi+ + 2ye- = xM + yLi2O (1)

where TMO, after reaction with Li+, is reduced to metal (M), and Li2O also forms via combination of Li+ and O2-. In spite of their high capacity, most TMOs suffer from poor rate performance, poor cycle performance and low coulombic efficiency in 1st cycle, preventing its commercialization. The origins and mechanisms underlying these problems are still unclear.
In this study, single crystalline α-MnO2 nanowire is used as a TMO representative to study the electrochemical lithiation mechanism by constructing an all-solid open-cell inside Transmission Electron Microscope (TEM) with MnO2 as the target electrode and Li metal as Li+ source. Morphological evolution, structural change and phase transition are simultaneously characterized inside TEM. A novel two-step expansion behavior of α-MnO2 nanowire is first visually observed during lithiation. These two expansion stages are sharply different in terms of expansion-needed time, propagation speed of each expansion front and volume change during each expansion. High resolution TEM and Selected Area Electron Diffraction analysis confirm that the first expansion stage is lead by 2×2 tunnel-driven lithiation and formation of LixMnO2 solid solution, while the second expansion stage is caused by thorough conversion of LixMnO2 to Mn and Li2O accompanied by fracture formation and electrode pulverization. These findings provide possible origins for electrochemical drawbacks of TMOs as LIB electrode and also cast light on potential electrode improvement by proper structural and compositional modification.