bluuebunny/crossref_metadata_2025_split huggingface dataset:
Sheet Type All-Solid-State Batteries with Sulfide Electrolyte
Authors: KIM KyungSu , Kang Seulki , Cho Woosuk , Park Kern-Ho , Jeong Goojin , Yu Ji-Sang 
Published: December 2020

Lithium ion batteries have received great attention due to emerging electric vehicle market to suppress global climate change issues. Batteries with higher energy density is required to improve driving distance of electric vehicle. As energy density increase, safety become more important point to prevent unexpected accident. Safety issues of current lithium ion battery system mainly comes from the oxide cathode and flammable organic electrolyte. All solid state batteries with non-flammable inorganic solid electrolytes come into the limelight due to its potential for securing higher energy density and safe characteristics over current lithium ion battery system.
In this study, composite electrode sheet and cell fabrication technology was examined by slurry mixing coating technique. Cathode electrode sheets were obtained by coating slurries consisting of LiNi0.8Co0.1Mn0.1O2 as the active material, an argyrodite structure Li6PS5Cl solid electrolyte, conductive carbon, butadiene-based binder with solvent on carbon coated aluminum foil as the current collector. Homogeneous mixing and coating conditions were examined by controlling composition, kinds of binder in order to achieve optimal conduction pathway of lithium ion and electron. All solid state batteries were fabricated and evaluated both half-cell and full-cell type. Electrochemical tests were investigated and the detailed results will be discussed in this presentation.
Introducing Electromagnetic Battery Sensors, with Unprecedented Performance
Authors: Roumi Mahshid , Roumi Farshid 
Published: December 2020

The chemistry of batteries have been improving constantly for the past century; however, the battery monitoring and thus management has not seen any real improvements since decades ago.
Internal shorts cost manufacturing companies millions of dollars each year. This is because it takes days and weeks to screen for cells with potential internal shorts. If undetected, the faulty cells in the field can cause millions of dollars in damages. Therefore, significantly increasing the speed of detection may double the profit of the manufacturing company. Internal shorts is also one of the major challenges of fast charging batteries. Fast charging can lead to hard- micro shorts that can result in battery failure and thermal runaway.
We have developed a completely new class of battery monitoring and screening sensors, PES™, first demonstrated by our team at Caltech in 2014. PES™ is an electromagnetic-based battery sensing platform, based on an extension of electrochemical impedance spectroscopy (EIS) to EM induction from an electrochemical system.
Conventional battery testing is primarily based on voltage, impedance, and/or temperature monitoring, which generally register issues only after significant internal changes to the condition of the battery have occurred. PES™ detects minor changes in the electric field itself, and can identify small internal shorts and structural variations in the battery well before they register in voltage/temperature-based reading fluctuations.
We have successfully demonstrated that it can detect gradually developing internal shorts, as large as 3300 ohms, which are extremely hard to detect by conventional voltage sensors. To significantly reduce the risk of failure and fire, the sensor should be an important part of any large Li-ion battery or any future Li-metal batteries. This class of sensors based on electromagnetism as opposed to the conventional voltage, current or temperature monitoring opens the door to many new applications, resulting in much higher utilization of batteries.

Figure 1
Double Approach Towards 3D Electrodeposited RuOx Porous Structure for High Energy/High Power Micro-Supercapacitors
Authors: Lotfi Benali Karroubi , Patnaik Sai , Guay Daniel , Pech David 
Published: December 2020

Hydrous RuOx has been one of the well-studied materials for application in supercapacitors owing to its excellent properties (high conductivity similar to metals, redox activity capable of fast faradaic reactions and structural water enabling swift proton transfer and decreased diffusion distance). The main issue regarding supercapacitors is that, they suffer from low energy density compared to batteries. One way to overcome this problem is to increase surface area of the active material and hence the energy stored through 3D structuration of current collector. Multiple techniques have been used in this regard like 3D printing, pholitography methods...etc.However, these techniques are pretty complex, time consuming and have constraining conditions. Hence, it’s necessary to develop economic and simple routes for 3D structuration of electrodes for micro-supercapacitors. One simple, time efficient and easy to set up method that can be used under ambient conditions is the electrochemical structuration using dynamic hydrogen bubble template (DHBT). With this strategy, 3D scaffolds which can hold small quantities of intrinsic pseudocapacitve materials like RuOx can be fabricated. The challenge in this latter case is magnified, needing controlled decoration of active materials for efficient utilization and full benefit of the 3D framework. Hence, the pursuit of superior micro-supercapacitors not only needs controlled deposition, but also requires stable 3D scaffolds to maximize capacitance per footprint area1. We have previously shown electrodeposition of active RuO2 on porous gold electrodes for micro-supercapacitors achieving a capacitance of 3 F/cm².
One other approach would be to deposit the active material directly by the DHBT method. As RuOx is a good conductor this would not hinder its efficiency (this would not be the case for MnO2 for example). The difficulty here is that, not all metals can be deposited by the DHBT technique as other factors play a crucial role such as the exchanged current density towards H2 evolution and mechanical stability3

In the current work, we report two different strategies for the 3D deposition of RuOx. The first is the successful fabrication of highly porous 3D platinum current collector using DHBT followed by a conformal coating of hydrous RuOx to achieve a specific capacitance as high as 10 F/cm². The second is the direct electrodeposition of the active material, RuOx, in a 3D porous structure. These two approaches are characterized and discussed within the framework of fabricating superior micro-supercapacitors with excellent capacitance and low internal resistance.

References

N. A. Kyeremateng, T. Brousse, and D. Pech, Nat. Nanotechnol., 12, 7–15 (2017)

A. Ferris, S. Garbarino, D. Guay, and D. Pech, Adv. Mater., 27, 6625–6629 (2015)

Plowman, B. J., Jones, L. A., & Bhargava, S. K. Chem. Commun., 51(21), 4331–4346.

Figure 1
Molecular Crowding Electrolytes for High-Voltage Aqueous Batteries
Authors: Xie Jing , Liang Zhuojian , Lu Yi-Chun 
Published: December 2020

Replacing flammable nonaqueous electrolytes with non-flammable aqueous electrolytes is critical to achieve safe, low-cost and eco-friendly Li-ion batteries. However, the voltage window of an aqueous Li-ion battery is limited by the thermodynamic stability window of water (1.23 V), which limits the energy density of the aqueous Li-ion batteries. Recently developed LiTFSI-based “water-in-salt” electrolytes with highly-concentrated salts (>21 m) have expanded the electrochemical stability window of water to over 3.0 V by decreasing the amount of free water molecules and creating artificial solid-electrode interfaces, however, raise concerns of cost and toxicity.
Molecular crowding is a common phenomenon in living cells where water activity is substantially reduced as a consequence of the changes in the water hydrogen-bonding structuring in the presence of molecular crowding agents. Herein, we introduce a molecular crowding electrolyte using water-miscible polymer poly(ethylene glycol) (PEG) as the crowding agent to decrease water activity, thereby allowing a high operational cell voltage (3.2 V) with a low salt concentration (2 m). Aqueous Li4Ti5O12/LiMn2O4 full cells with stable specific energies between 75-110 Wh kg-1 were demonstrated over 300 cycles. Extensive electrolyte characterizations including nuclear magnetic resonance spectroscopy (NMR), Fourier-transform infrared spectroscopy (FTIR), online electrochemical mass spectroscopy (OEMS) and density functional theory (DFT)-molecular dynamic (MD) simulation were used to confirm the HER suppression effect of the molecular crowding aqueous electrolyte.
The molecular crowding electrolyte enables numerous negative electrode materials that can not be used in traditional aqueous battery systems. This work provides a new platform for designing aqueous electrolytes with high stability for low-cost and sustainable energy storage.
References:
[1] Xie, J., Liang, Z. & Lu, Y. C. Molecular crowding electrolytes for high-voltage aqueous batteries. Nat. Mater. (2020). https://doi.org/10.1038/s41563-020-0667-y

Acknowledgement
This work is fully supported by a grant from the Research Grant Council of Hong Kong Special Administrative Region, China (Project No. CUHK14307318).
Enhanced Electrode/Electrolyte Interphases in Fluorinated Orthoformate Electrolytes for Stable High-Voltage Lithium Metal Batteries
Authors: Cao Xia , Xu Wu , Zhang Ji-Guang 
Published: December 2020

Rechargeable lithium (Li) metal batteries (LMBs) have been revived in recent years because of the ever-increasing demand for high-energy-density batteries. 1,2 However, significant challenges, such as low Columbic efficiency (CE), pulverization and large volume expansion related to the Li metal anode still limit the large-scale application of these batteries. 3 Here, we report an approach to improve the Li CE and minimize the Li pulverization and volume expansion by using fluorinated orthoformate in electrolytes. 4 Tris(2,2,2-trifluoroethyl) orthoformate (TFEO) functions as an efficient diluent in electrolytes based on lithium bis(fluorosulfonyl)imide (LiFSI) and 1,2-dimethoxyethane (DME) and formulates highly concentrated LiFSI-DME clusters that are dispersed among the TFEO diluent. Such localized high-concentration electrolytes demonstrate superior electrochemical properties when used in LMBs with a high voltage LiNi0.8Mn0.1Co0.1O2 (NMC811) cathode. The mechanisms behind the long cycle life of Li||NMC811 cells under practical conditions are mainly the formation of highly effective solid electrolyte interphase and cathode electrolyte interphase, which are monolithic and prevent continuous electrode/electrolyte side reactions. This work provides guidance for further development of electrolytes for high-energy-density LMBs. The details will be discussed during the presentation.
References
1 J.-G. Zhang, W. Xu, W. A. Henderson, Lithium Metal Anodes and Rechargeable Lithium Metal Batteries. XV, 194 (Springer International Publishing, 2017).
2 J. Liu, et al. Pathways for practical high-energy long-cycling lithium metal batteries. Nature Energy
4, 180-186 (2019).
3 C. Niu, et al. High-energy lithium metal pouch cells with limited anode swelling and long stable cycles. Nature Energy
4, 551-559 (2019).
4 X. Cao, et al. Monolithic solid–electrolyte interphases formed in fluorinated orthoformate-based electrolytes minimize Li depletion and pulverization. Nature Energy
4, 796-805 (2019).
Effects of Aniline Tetramer-Co-Acrylic Monomer Grafted to Polysaccharide Backbone As a Conductive and Adhesive Binder for High Capacity Si/C Composite Anodes
Authors: OH Eun-Suok , Gendensuren Bolormaa , Taewon Kim 
Published: December 2020

Conducting polymers such as polyaniline and polypyrrole have been sometimes described as a potential candidate binder for high silicon anode materials due to its low price, high conductivity, and simple synthesis. The manufacturing process of conducing polymerbased electrodes requires environmental-unfriendly organic solvents such as n-methylpyrrolidone. Due to the drawback, natural polysaccharides blended with the conductive polymers have been often investigated as water-soluble, electronically conductive, and adhesive binder to improve the electrochemical performance of the high-capacity Si anodes. However, the polymer blends are still needed to modify their properties through functionalization with some additional groups, for example, grafting with adhesive monomers and crosslinking for high adhesion strength.
In this study, we first prepared aniline tetramer-co-acrylic monomer (AT-Am) by two step polymerization using 4-aminodiphenylamine in acidic solution at ~ 0°C, and then AT was reacted with acryloyl chloride monomer at room temperature for 3 hours to produce AT-Am monomer. Finally, AT-Am and pure acrylamide (AAm) monomers with various weight ratios are grafted and polymerized to the backbone of sodium alginate (Alg). Here AT and AAm have roles of electronic conduction and strong adhesion, respectively. This water-treatable alginate-graft-poly(acrylamide-aniline tetramer) (Alg-g-PAAT) was used as a conductive and adhesive binder for Si/C composite anodes to improve electronic conduction and adhesion ability when compared to natural Alg and Alg-g-PAAm. As a result, the Si/C anode containing Alg-g-PAAT yielded 800 mAh g-1 after 200 cycles with maintaining high columbic efficiency when compared to Alg-g-PAAm and physical blend between Alg-g-PAAm and AT.
Suppressing Lithium Dendrite Growth with Nanoparticle-Dispersed Colloidal Electrolytes
Authors: Lee Hongkyung , Kwak Won-Jin , Lee Jinhong , Kim Hee-Tak , Lim Hyung-Seok , Cao Xia , Ren Xiaodi , Rodriguez Perez Ismael , Zhang Ji-Guang 
Published: December 2020

Lithium (Li) metal has been considered as a very promising anode material for next-generation batteries because of its low electronegativity (-3.04 V), low gravimetric density (0.53 g cc-1) and ultrahigh specific capacity (3860 mAh g-1). The recent simulations forecast that the rechargeable Li metal batteries (LMBs) coupled with the conventional transient metal oxide cathodes and the Li metal anode can deliver a high gravimetric energy density of up to 500 Wh kg-1. However, significant challenges, including low Coulombic eﬃciency (CE), short cycle life, and safety concerns have plagued the practical applications of Li metal as the anode in recharge batteries.
However, its poor cycling stability due to Li dendrite formation and excessive Li pulverization is the major hurdle for its practical applications. In this work, we present a silica (SiO2) nanoparticle-dispersed colloidal electrolyte (NDCE) and its design principle for suppressing Li dendrite formation. SiO2 nanoclusters over the percolated threshold of Li+ ion transport play roles of enhancing the Li+ transference number and increasing the Li+ diffusivity in the vicinity of the Li plating substrate. NDCE enables less-dendritic Li plating by manipulating the nucleation-growth mode and extending Sand's time. Moreover, SiO2 can interplay with the electrolyte at the Li-metal surface, and thus, it can modify the solid-electrolyte interphase (SEI) structure by enriching fluorinated compounds. The initial control of the Li plating morphology and SEI structure by NDCE leads to a more uniform and denser Li deposition upon subsequent cycling, resulting in three-fold enhancement of the cycle life. The efficacy of the NDCEs has been further demonstrated by the practical battery design featuring a commercial-level NMC cathode (4.2 mAh cm-2) and very thin Li metal (40 μm) anode.
Nanospace-Assisted Anti-Oxidative Li Storage on Carbon Nanotubes
Authors: Yoo JongTae , Lee Sang-Young 
Published: December 2020

Lithium (Li) metal has attracted significant interest as a next-generation battery anodes due to its high theoretical speciﬁc capacity and low redox potential. However, inhomogeneous plating/stripping behavior of Li metal accelerates Li-consuming parasitic reaction and sometimes provokes an internal short circuit problem. In particular, its environmental vulnerability (e.g., notorious reactivity upon exposure to air and water) due to the electrochemical instability poses a formidable challenge to commercial applications, thus it should be resolved as an indispensable prerequisite in addition to resolving the concerns on cell performance and safety.
Here, we report a new class of anti-oxidative Li reservoir based on nanospaces of carbon nanotube (CNT) bundles. The CNT bundles are formed by assembling themselves via van der Waals interactions, producing one-dimensional nanospaces (i.e., external grooves and interstitial channels). The Li preferentially stored in the interstitial channels is chemically stable against to air and water. Notably, the Li electrochemically extracted from Li-confined CNTs onto a copper (Cu) foil prohibits reliable electrochemical performance (e.g., stable charge/discharge behavior) comparable to those of pristine Li foils. We envision that this nanospace reservoir strategy will open a new avenue for development of environmentally tolerant, high-capacity Li storage.
Suitability of Ethyl Cellulose As a Binder in Positive Electrode of Aqueous Li-Ion Battery
Authors: Sepp Silver , Peljo Pekka 
Published: December 2020

Novel materials for energy storage devices need to be affordable, durable, safe and environmentally friendly. PVDF, which is the most popular polymer used as a binder in battery cathode electrodes, requires the use of and toxic solvents for processing, such as N-methyl-pyrrolidone (NMP).1 Ethyl cellulose is a biodegradable and water-insoluble polymer. Ethyl cellulose based slurry can be prepared using ethanol as solvent, which makes the process cheaper and more sustainable. Replacing PVDF with more environmentally friendly binder like ethyl cellulose in positive electrode of aqueous Li-ion battery would be beneficial in many ways. It would shorten the assembly procedure due to high speed of solvent evaporation, there are no strict requirements for humidity control and the recycling procedure is easier as there are no fluorinated compounds.2 Therefore, this replacement would enable to produce safer and cheaper energy storage devices.
In this work electrodes with different composition have been described using galvanostatic charging-discharging and cyclic voltammetry. LiMn2O4 (LMO) has been used as active material for cathode, carbon black Super P as conductive additive and PDVF or ethyl cellulose as a binder. The electrodes were prepared using different mass ratios of conductive additive and binder to evaluate the performance of this sustainable polymer. Using ethyl cellulose as a binder, discharge capacity 100 mAhg−
1 was achieved at 0.2C rate for LMO cathode which is comparable to the results obtained with PVDF as a binder. 500 cycles at the rate of 1C showed somewhat better capacity retention for electrodes prepared using PVDF. However, the results show that ethyl cellulose is a promising option to replace PVDF as cathode binder in aqueous systems. Further optimization is needed to prepare these novel and sustainable cathodes for aqueous Li-ion battery.
The research was supported by the Estonian Research Council grant PUTJD956 and Magnus Ehrnrooth Foundation.
References:

I. Doberdò, N. Löffler, N. Laszczynski, D. Cericola, N. Penazzi, S. Bodoardo, G. T. Kim, and S. Passerini, J. Power Sources, 248, 1000–1006 (2014).

L. Ibing, T. Gallasch, P. Schneider, P. Niehoff, A. Hintennach, M. Winter, and F. M. Schappacher, J. Power Sources, 423, 183–191 (2019).
Suppressing Electrochemical Instabilities of Li Metal Using Ionomer-Based Interfaces
Authors: Huang Zhuojun 
Published: December 2020

A fundamental challenge shared across many energy storage devices, is the complexity of electrochemistry at the electrode-electrolyte interfaces that impacts the faradaic efficiency, operational rate capability and lifetime. Specifically, in energy-dense lithium metal batteries, the charging process results in morphological heterogeneity of the metal anode, leading to battery failure by short-circuit or capacity fade. Perhaps, a facile way of addressing these challenges is designing a polymer thin-film at the electrode-electrolyte interface. We envision that an ideal interface should be based on several design principles including: presence of Li+ ion conduction pathway; chemically inert, mechanically robust, adaptive to volume changes and solution-processable for large scale thin-film casting.
Here, we use free-radical polymerization technique to synthesize novel stimuli-responsive polymers which exhibit the aforementioned characteristics. Unlike, previous works where the electrode coating acts as a pure physical barrier, the designer polymers in this work possess multifunctional characteristics to suppress different electrochemical instabilities. Because of the viscoelastic and electroactive nature of the polymers, they respond to any morphological changes of the electrodes during electrodeposition, giving rise to an electrochemical shielding mechanism that modulates lithium ion migration pathway and prevents surface roughening.
This work takes advantage of contemporary characterizations techniques like NMR, voltammetry and rheology to mechanistically understand the role of polymer dynamics and ion content on the electrodeposition morphology. We show that systematic optimization of these parameters can significantly boost the coulombic efficiency of the battery. Remarkably, we found that these polymer coatings can enhance the lifetime of conventional high-voltage lithium metal battery by at least two-times.
Solute and Solvent Structural Effects in Concentrated-Electrolyte Transport
Authors: Wang Andrew , Fawdon Jack , Hou Tianhong , Pasta Mauro , Monroe Charles W. 
Published: December 2020

Super-concentration of electrolytic solutions has been hypothesized as a route to improve battery performance [1]. To predict electrolyte behavior accurately in superconcentrated systems, one must account for their fundamentally different molecular structures. Interactions between species such as ion pairs in concentrated electrolytes may impact the transport laws governing diffusion, migration, and convection, and solute-volume effects may be large because the solution volume fraction occupied by salt is extremely high.
Transport phenomena relating to solute and solvent structure, such as Faradaic convection and the excluded-volume effect, can become dominant in the superconcentrated regime [2]. In very concentrated electrolytes convection can be important because when the salt occupies a large volume fraction of the solution, salt flux across the boundary of a solution drives a bulk solution velocity through overall mass continuity. Experiments demonstrate that at high concentration, viscosity no longer determines ion mobility, i.e., the Stokes–Einstein relation fails. The dynamics of ion-pair formation and salt association/dissociation kinetics both can impact the availability of charge-carrying species in an electrolyte. Experimentally, Faradaic convection can be quantified by combining densitometry with electrochemical measurements. Ion speciation and extent of dissociation can be quantified with spectroscopic techniques.
Newman’s application of Onsager–Stefan–Maxwell theory to electrochemical transport considers solute/solute interactions neglected in Nernst–Planck dilute solution theory [3]. We will add to this perspective by discussing how solute-volume effects and ion-association equilibria additionally influence apparent flux-explicit transport properties such as conductivity, diffusivity and transference number [4].
[1] Yamada, Y., Wang, J., Ko, S., Watanabe, E. & Yamada, A. Advances and issues in developing salt-concentrated battery electrolytes. Nat. Energy
4, 269–280 (2019).
[2] Liu, J. & Monroe, C. W. Solute-volume effects in electrolyte transport. Electrochim. Acta
135, 447–460 (2014).
[3] Monroe, C. W. & Delacourt, C. Continuum transport laws for locally non-neutral concentrated electrolytes. Electrochim. Acta
114, 649–657 (2013).
[4] Hou, T. & Monroe, C. W. Composition-dependent thermodynamic and mass-transport characterization of lithium hexafluorophosphate in propylene carbonate. Electrochim. Acta (2019).

Figure 1