bluuebunny/crossref_metadata_2025_split huggingface dataset:
New Separator Materials for Lithium-Ion and Lithium Primary Batteries Operating in Extreme Environments
Authors: Brandon Erik J. , Billings Keith J. , Ratnakumar Bugga V. , Jones Simon C. , Pasalic Jasmina , Seong Jessica , Warner William N. , Hu Carl , Morin Brian 
Published: February 2020

Lithium-ion battery technology is now pervasive in all areas and at all scales of energy storage, including consumer electronics, automotive applications and grid level storage. Traditionally limited to operation under terrestrial conditions, these limits of lithium-ion technology are being expanded to encompass operation under more extreme conditions, including aerospace applications. These scenarios require the consideration of new cell components, including electrolytes, cell designs and separators. This talk will focus on the development of new separator materials, targeted for operation in high radiation environments, often encountered in space missions. Conventional polyethyelene/polypropylene based separators have been evaluated for their electrical, chemical and mechanical performance. High doses of radiation have been shown to compromise the mechanical performance of these conventional separators. New aramid based separators are under development to address these limitations, and results from this development and testing will be reported. It is anticipated these separator materials may find application in lithium-ion battery cells used in other types of extreme environments.
The work described here was carried out at the Jet Propulsion Laboratory, California Institute of Technology, under contract with the National Aeronautics and Space Administration (NASA) and supported by the Europa Lander Pre-Project.
(Invited) Towards Fast Charging of High Energy Density Li-Ion Batteries
Authors: Du Zhijia , Liu Tianyi , Wu Xianyang , Lin Feng , Zhao Kejie , Wood David L. , Belharouak Ilias 
Published: February 2020

The development of Li-ion battery has attracted extensive efforts in the last three decades for its high energy density and long cycle life. The rapid growth of electric vehicle market has a demand for fast charging of Li-ion battery in order to increase the market penetration. The energy density of Li-ion battery has been increased to 225-250 Wh/Kg nowadays thanks to R&D of cell engineering development (mainly increasing electrode thickness). This high energy density ensures longer driving mileage, but also limits the fast charging capability compared to high power Li-ion cells with thinner electrodes.
The relationship between battery energy density, power density and areal capacity in thick electrodes has been studied by Du et al1. and Gallagher et al2. The results suggested that the rate capability is limited by both the Li-ions mass transport in liquid electrolytes and interfacial overpotential in graphite anodes 2,3. The findings also implied that a significant portion of the available energy in thick electrodes cannot be accessed because of the depletion of Li-ions in the electrolyte phase 1. Therefore, development of electrolyte that has the capability of fast mass transport in the cell is of great importance for fast charging of high energy density Li-ion cells.
The team at ORNL is developing electrolyte that can enable a fast charging of 15 minute for high energy density Li-ion cells. By developing suitable solvent, salt and additives, the Li ion transport properties can be increased by >20%. We will talk about the result in details during the meeting.

Z. Du, D. L. Wood, C. Daniel, S. Kalnaus, and J. Li, J. Appl. Electrochem., 47, 405–415 (2017).

K. G. Gallagher et al., J. Electrochem. Soc., 163, A138–A149 (2016).

S. Ahmed et al., J. Power Sources, 367, 250–262 (2017).
Rechargeable Aluminum Organic Batteries
Authors: Kim Dong Jun , Yoo Dong-Joo , Otley Michael T , Prokofjevs Aleksandrs , Pezzato Cristian , Owczarek Magdalena , Lee Seung Jong , Choi Jang Wook , Stoddart J.Fraser 
Published: February 2020

Since aluminum is the third most abundant element in Earth’s crust, developing rechargeable aluminum-ion offers1 a golden opportunity for delivering a high energy-to-price ratio. Nevertheless, finding appropriate host electrodes for inserting aluminum (complex) ion remains a fundamental challenge. Here, we demonstrate2 a new strategy for designing active materials for rechargeable aluminum batteries. This strategy entails the use of redox-active triangular phenanthrenequinone-based macrocycles which form layered superstructures resulting in the reversible insertion and extraction of cationic aluminum complex. This architecture exhibits an outstanding electrochemical performance with a reversible capacity of 110 mAh g–1 along with a superior cyclability of up to 5000 cycles. Furthermore, we prepared a hybrid electrode by blending the macrocycle with graphite flakes, featuring homogeneous stacking of both macrocycle and graphite flake. These findings lay the groundwork for future design and operation of aluminium-ion batteries and represent a promising starting point for developing affordable large-scale energy storage applications.
References

M. -C. Lin, et al.
Nature
2015, 520
, 324–328.

D. J. Kim, D.-J. Yoo, M. T. Otley, A. Prokofjevs, C. Pezzato, M. Owczarek, S. J. Lee, J. W. Choi, and J. F. Stoddart, Nat. Energy, 2019, 4, 51–59.

Figure 1
Thermodynamic Perspective on Co-Intercalation Behavior of Li/Mg Dual Cations in Intercalation Cathode Materials
Authors: Li Hongyi , Hatakeyama Takuya , Okamoto Norihiko L. , Kumagai Yu , Oba Fumiyasu , Ichitsubo Tetsu 
Published: February 2020

Post Li-ion batteries using multivalent ions, such as Mg2+, Ca2+, Zn2+, have attracted much attention in recent years, but developing appropriate intercalation cathode materials for these multivalent cations remains a difficult task due to the sluggish solid-phase diffusion behavior, which is usually caused by the strong coulomb interaction between multivalent cations with the ionic cathode hosts. As an attempt to solve this problem, we proposed a new battery technology, which is referred to as Li-Mg dual-cation batteries.[1-2] The Li-Mg dual-cation batteries possess a so-called “rocking-chair”-type structure, where Li ion and Mg ion are involved in each half-cell reaction simultaneously.
When exploring the characteristics of these batteries, we found an interesting phenomenon that Mg intercalation usually shows higher discharge potential in Li-Mg dual-cation electrolyte than in Mg single-cation electrolyte. The increase of discharge potential (i.e. decrease of the overpotential for Mg intercalation) strongly suggests that the co-existing Li ion is helpful to promote the Mg intercalation with cathode hosts. To elucidate what causes this phenomenon, we performed the first-principles calculations[3-4] with the Nudged Elastic Band (NEB) method[5] to estimate the activation energy of Mg cation migration in cathode hosts that are discharged in Li or Mg single-cation and Li-Mg dual-cation electrolytes and finally revealed a facilitating mechanism for the solid-phase diffusion of Mg cation.[6]
In this presentation, we give a comprehensive explanation on the co-intercalation behavior of Li ion and Mg ion in Li-Mg dual-cation batteries, especially from a thermodynamic perspective. This work advances the fundamental understanding of ionic conduction phenomena of multivalent cations, which is indispensable for developing future energy storage devices.
[1] T. Ichitsubo, S. Okamoto, T. Kawaguchi, Y, Kumagai, F. Oba, S. Yagi, N. Goto, T, Doi, E. Matsubara, J. Mater. Chem. A
3, 10188(2015).
[2] H. Li, T. Ichitsubo, S. Yagi, E. Matsubara, J. Mater. Chem. A
5, 3534(2017).
[3] P. E. Blöchl, Phys. Rev. B
50, 17953(1994).
[4] J. P. Perdew, K. Burke, M. Ernzerhof, Phys. Rev. Lett.
77, 3865(1996).
[5] G. Henkelman, B. P. Uberuaga, H. Jónsson, J. Chem. Phys.
113, 9901(2000).
[6] H. Li, N. L. Okamoto, T. Hatakeyama, Y, Kumagai, F. Oba, T. Ichitsubo, Adv. Energy Mater.
8, 1801475(2018).
Li-Substituted Layered-Spinel Cathode Material for Sodium-Ion Batteries
Authors: Deng Changjian , Skinner Paige , Liu Yuzi , Hunt Riley , Lau Miu Lun , Sun Meiling , Ma Chunrong , Tong Wei , Xu Jing , Xiong Hui (Claire) 
Published: February 2020

Sodium-ion battery (SIB) has been considered as an attractive technology for the next-generation, large-scale energy storage systems (EES) in support of reliable, robust and cost-effective electrical power grids.1-4 The O3-type layered Na(NixFeyMnz)O2 (0 < x, y, z< 1) cathode materials are of great interest in sodium-ion batteries due to the abundance and cost of raw materials and their high specific capacities. However, the cycling stability and rate capability at high voltages (>4.0V) of these materials remains an issue. Herein, we successfully synthesized a Li-substituted layered-tunneled (O3-spinel) intergrowth cathode (LS-NFM) to address these issues. The remarkable structural compatibility and connectivity of the two phases were confirmed by X-ray diffraction (XRD), selected area electron diffraction (SAED) and high resolution transmission electron microscopy (HRTEM). LS-NFM electrode reached a discharge capacity 107 mAh g-1 with a capacity retention of 95% after 50 cycles at a current rate of 100 mA g-1 in a voltage window of 2.0 - 4.2 V. Moreover, the LS-NFM cathode exhibited an enhanced rate capability in comparison to the un-doped layered cathode (NFM). The enhanced rate capability of LS-NFM can be explained by the significantly increased effective Na+ diffusivity measured by galvanostatic intermittent titration technique (GITT) compared to the un-doped control NFM cathode, which can be ascribed to the improved charge transport kinetics through shortened diffusion path by direct connection between the 3D channels in the spinel phase and 2D channels in the layered phase. The results from ex situ hard/soft X-ray adsorption spectroscopy (XAS) suggest that the capacity of LS-NFM cathode is mainly associated with the Ni2+/Ni4+ redox couple, and slightly from the Fe3+/Fe4+ redox couple. The voltage profile of the LS-NFM cathode exhibited a reversible plateau above 4.0 V, indicating great stability at high voltages and structural stabilization by the spinel phase. In addition to the substitution of various transition metals, or the modification of the stoichiometry of each transition metal, this study provides a new strategy to improve electrochemical performance of layered cathode materials for sodium ion batteries.
References:
(1) Yabuuchi, N.; Kubota, K.; Dahbi, M.; Komaba, S. Chemical Reviews
2014, 114, 11636.
(2) Pan, H. L.; Hu, Y. S.; Chen, L. Q. Energ Environ Sci
2013, 6, 2338.
(3) Kundu, D.; Talaie, E.; Duffort, V.; Nazar, L. F. Angew Chem Int Edit
2015, 54, 3431.
(4) Slater, M. D.; Kim, D.; Lee, E.; Johnson, C. S. Advanced Functional Materials
2013, 23, 947.

Figure 1
Enhancing the Performance of Vanadium Redox Flow Batteries Using Carbon Cloth Electrode Decorated with C/WOx Nanocomposites
Authors: El Diwany Farah , El Sawy Ehab N , Allam Nageh 
Published: February 2020

Given the growing world population and the industrial revolution, there is an immense global energy demand, which has heavily been established by fossil fuels for several decades. However, the depletion rate of fossil fuel reserves and their environmental hazards have led the global energy systems to shift to using renewable energy sources. Even though the roles of solar and wind energy are expected to increase over the coming years, their intermittent behavior requires their integration with electrical energy storage systems for frequency balancing and efficient utilization. Whereas conventional energy storage techniques (e.g., pumped hydro, compressed air, flywheel, and thermal energy) have large footprints, require big investments and lack flexibility, electrochemical energy storage methods, have higher energy density and better flexibility depending on their design. Compared to other electrochemical systems (e.g., Li-ion batteries and supercapacitors), vanadium redox flow batteries are thought to be an optimal solution to create smart grids when combined with renewable energy sources, owing to their scalability, site versatility, long lifetime and ease of operation.
Nevertheless, there are some issues concerning their efficiency and further market penetration, including (i) low solubility of vanadium ions in acidic electrolyte leading to low energy density; (ii) crossover of vanadium ions through membrane leading to self-discharge and low capacity; and (iii) slow kinetics of vanadium ions reactions at the electrodes. Even though the widely used carbon-based electrodes have high stability in acidic solutions and high conductivity, modifications are needed to improve the kinetics of the electrocatalytic reaction, which is the aspect being concerned in this study. Thermal treatment of carbon cloth showed faster electrode kinetics at 0.1 M and 1 M vanadium ion concentration in pure H2SO4 and H2SO4/HCl. Incorporation of carbon and tungsten oxide nanostructures also demonstrated excellent electrocatalytic activity, resulting in high energy efficiency. A proposed description of the poorly understood mechanism of this electrochemical reaction will be presented, along with these findings, allowing for a big step forward towards a more efficient vanadium redox flow battery.
Novel Electrolytes to Enable Energy Dense Batteries
Authors: Mohtadi Rana , Tutusaus Oscar 
Published: February 2020

The ever-increasing demands for safe, energy dense and low cost energy storage systems have been driving interests in beyond Li-ion batteries such as those based on Li metal, magnesium metal and all solid state battery systems[1,2]. These high energy density batteries suffer from several challenges, several of which are related to the instability or incompatibility of the electrolytes[1,3,4]. Our group has been pioneering the development of electrolytes that enabled overcoming several key challenges in magnesium batteries and created a new family of highly performing and practical electrolytes [3,4]. One challenge with electrolytes for batteries in general is the high flammability and volatility, that can be overcome with the use ionic liquid solvents. However, available ionic liquids suffer from several key draw backs associated with insufficient anodic stability and incompatibility with reactive metallic anode.
Herein, we outline the classes of electrolyte materials we developed and how we overcome current challenges with ionic liquids for Mg and Li metal batteries.[5]

References

[1] Choi J. W. Aurbach D. Nature Reviews Materials 1, 2016, 16013 1-16.
[2] Manthiram A., Yu X., Wang S. Nature Reviews Materials 2, 2017 16103.
[3] Mohtadi R., Orimo S., Nature Reviews Materials, 2016, 2,16091. 1311.
[4] Mohtadi R., Mizuno F. Beilstein J. Nanotechnol. 2014, 5, 1291–
[5] Kar, M., Tutusaus O., Doug R. MacFarlane, Mohtadi R., Energy Environ. Sci., 2018, Advance Article
Amorphous Silicon Nitride - an Anode Material for the Next Generation Li-Ion Batteries
Authors: Ulvestad Asbjørn , Koposov Alexey Y , Skare Marte O , Preston Thomas J , Prytz Oystein , Mæhlen Jan Petter , Andersen Hanne Flåten 
Published: February 2020

Despite a decade of extensive research, silicon, as material for anodes of lithium ion batteries, still has not become a practical solution. Suffering from enormous expansion/contraction during lithiation/delithiation cycles, silicon undergoes rapid self-destruction resulting in battery failure. To counteract the degradation several options has been explored over the years. Those include downsizing of the material to nanoparticles, doping and coating with organic or inorganic shells.
An alternative approach was proposed to mitigate the structural destruction of silicon, which is preparation of the alloyed materials. In the present work we demonstrate the use of nanostructured amorphous substoichiometric silicon nitride as such alternative anode material. We demonstrate that upon lithiation, silicon nitride forms lithiated subunits of silicon and ternary phase of lithium silicon nitride, which serves as a matrix material. Such phase separation leads to remarkable stability: the nanostructured thin films of SiNx allowed fabrication of electrodes exhibiting capacities above 1500 mAh/g for 2000 cycles. To achieve sufficient capacities for the practical applications, we demonstrate the application of this principle to particle-based composite electrodes, using SiNx nanoparticles fabricated through a CVD process. Such amorphous substoichiometric nanoparticles demonstrated reversible capacities above 1000 mAh/g and excellent cycling stability over several hundred cycles. We also demonstrate the effects of chemical composition on initial and long-term cycling stability of nanostructured silicon nitride.
Probing Solid-Solid Interfacial Reactions in All-Solid-State Batteries
Authors: Tang Hanmei , Deng Zhi , Banerjee Abhik , Wu Erik , Nguyen Han , Meng Shirley , Ong Shyue Ping 
Published: February 2020

We have developed a hierarchy of DFT-based approaches to understand and design electrode/buffer/SE interfaces in all-solid-state batteries. Even with relatively efficient thermodynamics approximations, we reveal that S-O exchange reactions between oxides (O2-) and thiophosphates (PS4
3-) resulting in the formation of phosphates (PO4
3-) are responsible for large reaction driving force between the common NaMO2 (M = Co, Ni, Fe, Mn) cathodes and Na3PS4 SE. Such reactions, with their associated large volume changes, can be mitigated by careful selection of the cathode/SE combination, or the use of buffer layers with good stability between both materials. We have also identified several promising binary oxides with similar or better chemical compatibility with most electrodes and SEs than the commonly-used Al2O3.
Despite the success of thermodynamics-based approximations, we further demonstrate that explicit modelling of the electrode/SE interface via ab initio molecular dynamics (AIMD) simulations sometimes yield different and more realistic predictions of interfacial reaction products. For example, AIMD predicts that formation of SO4
2– are kinetically favored over the formation of PO4
3– at the NaCoO2/Na3PS4 interface model, in contrast to the predictions of the thermodynamic models. These observations have been validated experimentally. We have also extended such studies to the LiNi0.85Co0.1Al0.05O2/Li6PS5Cl interface, with and without buffer layers, and the predicted interfacial reactions are in good agreement with experimental characterizations.
In Operando XAFS of Vanadium Oxide Nanomaterials Produced through Rapid Microwave Synthesis
Authors: Booth Samuel Guy , Corr Serena 
Published: February 2020

The increase in demand for portable electronics combined with a need for grid storage to match the expansion of renewable energy sources has led to a requirement for new, higher capacity electrode materials. For such a development, vanadium is a promising material due to the number of readily accessible oxidation states. The ability to access multiple oxidation states results in much higher theoretical capacities when compared to sites capable of only single electron transfer.1 A number of previously studied materials have shown that such an increase in capacity can come at the cost of battery cyclability. Where the intercalation and deintercalation processes result in the breakdown of the framework structure, causing the rapid capacity fade.
In our lab we have been developing microwave-based reactions to produce a number of different vanadium oxide structures from V2O5. Such structures can be formed using non-harmful solvents with rapid reaction times (on the order of 2-4 hours). Whereas, to produce the same materials, traditional hydrothermal methods often require higher reaction temperatures and need to be run for upwards of a day, making them more energy intensive.
Such structures are of great interest as outlined above, however, to develop them further it is key to understand how the structures may alter during cycling to start to understand the degradation mechanisms. Alongside bulk techniques such as XRD and IR, highly incisive structural information can be garnered through X-ray absorption fine structural (XAFS) analysis; an element specific, local probe. When measurements are conducted during battery cycling, this can give precise information about what is happening to the local structure and how reversible the changes in structure are on charge and discharge.2 Such information provides a clear demonstration of the suitability of the materials for future battery cathodes. Additionally, a broader idea of the likely stresses induced in the structure will aid the design of model architectures for future battery materials.

1 J. Prado-Gonjal, B. Molero-Sánchez, D. Ávila-Brande, E. Morán, J. C. Pérez-Flores, A. Kuhn and F. Garcia-Alvarado, J. Power Sources, 2013, 232, 173-180.

2 Y. N. Zhou, J. Ma, E. Hu, X. Yu, L. Gu, K. Nam, L. Chen, Z. Wang and X. Q. Yang, Nature Commun, 2014, 5, 1-8.
A Series of Polyhydric Esters As Novel Candidates for Battery Solvents in Lithium Metal Cells: Electrochemical Investigations and Influences of Moisture and Alcohol Residues in Contact with Lithium Metal
Authors: Grünebaum Mariano , Buchheit Annika , Lürenbaum Constantin , Winter Martin , Wiemhöfer Hans-Dieter 
Published: February 2020

In recent years, the lithium metal anode has aroused great interest, not at least through the development of the lithium//sulfur and the lithium//air battery technologies, in all-solid-state batteries. However, the application of lithium metal anodes is limited by safety issues and several failure mechanisms, including, dendrite growth and direct chemical reactions with electrolyte components like battery solvents, which leads to fast capacity losses.
In this context, a new series of polyhydric propyl-based esters were investigated, namely n-propyl acetate, isopropyl acetate (monohydric esters), trimethylene diacetate, 1,2-propylene glycol diacetate (dihydric esters) and triacetin (trihydric ester) as attractive and environmental friendly candidates for electrolyte solvents in lithium metal battery applications.The above mentioned organic esters were examined in respect to their reactivity in contact with lithium metal, influenced by water or alcohol impurities. The resulting reaction products were analyzed and determined via 1H-NMR spectroscopy. Additional experiments were performed and the resulting products compared to anticipated reaction products which were prepared separately, to evidence possible reaction mechanisms like the occurrence of a CLAISEN-condensation.
Furthermore, the here mentioned propyl-based esters and the reaction products were analyzed by cyclic voltammetry against copper, platinum and aluminum as working electrode to evaluate the anodic and cathodic stability, as well as possible anodic dissolution reactions in the presence of LiTFSI as conducting salt.
In both cases, the reactivity in contact with lithium metal and the anodic dissolution of aluminum, a reactivity could be observed whereupon the trihydric esters were least reactive followed by the dihydric and monohydric esters.
In absence of water and alcohols all investigated esters show no detectable reaction with lithium metal.

ACKNOWLEDGMENT

The authors want to acknowledge the German Federal Ministry for Economic Affairs and Energy (BMWi) for funding within the project FesKaBat (03ET6092E). The authors also acknowledge the analytical group of Sascha Nowak (MEET Battery Research Center, University of Münster) for all performed TXRF measurements.