bluuebunny/crossref_metadata_2025_split huggingface dataset:
Garnet-Based Electrolytes for All-Solid-State Li-S Batteries
Authors: Zhou Chengtian , Thangadurai Venkataraman 
Published: February 2020

Lithium sulfur (Li-S) batteries have emerged as one of the most promising post LIBs technologies with a remarkably high theoretical energy density and abundance of elemental sulfur. Nonetheless, there are several problems associated with Li-S batteries such as safety hazard due to lithium dendrite formation and fast capacity decay due to polysulfide dissolution effect.1 Employment of solid-state electrolytes is a promising strategy to address those issues.
Among different solid-state Li-ion electrolytes, Li-garnet attracts a lot of attention as it has a wide electrochemical window (> 6 V vs. Li/Li+), and high ionic conductivity (~ 1 mS cm-1) at room temperature. However, the application of garnet is hampered by its interfacial resistance against electrodes.2 In order to the reduce the interfacial area specific resistance (ASR) of Li/garnet interface, we devised a surfactant-processed interlayer for ceramic electrolytes (SPICE) method which can uniformly deposit a layer of ZnO onto the garnet surface. This process improves the wetting of Li and reduces the interfacial ASR to 10 Ω cm2 at room temperature.3 Stable Galvanostatic cycling of Li/garnet/Li at current densities up to 0.5 mA cm−2 was conducted, which presents a compelling method to solve the Li/solid electrolyte interface problem.
Another strategy we applied is incorporating garnet into polymer matrix to fabricate a flexible hybrid electrolyte. Polymer-based electrolytes possess low interfacial resistance due to its intimate contact with electrodes.4 The hybrid electrolyte merging the merits of garnet and polymer has been successfully employed in all-solid-state Li-S batteries operating at room temperature. Toward improving the energy density of the battery, we are working on tuning the cathode structure to effectively load more sulfur active materials. In this presentation, the SPICE method to tailor the interfacial resistance and the performance of all-solid-state Li-S batteries based on hybrid electrolyte will be discussed.

Manthiram, A.; Fu, Y.; Chung, S.; Zu, C.; Su, Y. Chem. Rev.
2014, 114, 11751-11787.

Han, X.; Gong, Y.; Fu, K.; He, X.; Hitz, G.; Dai, J.; Pearse, A.; Liu, B.; Wang, H.; Rubloff, G.; Mo, Y.; Thangadurai, V.; Wachsman, E.; Hu, L. Nat. Mater.
2016, 16, 572-579.

Zhou, C.; Samson, A.; Hofstetter, K.; Thangadurai, V. Sustainable Energy & Fuels
2018, 2, 2165-2170.

Zhou, C.; Bag, S.; Thangadurai, V. ACS Energy Lett.
2018, 3, 2181-2198.
Mwcnts-COOH/Cotton Flexible Supercapacitor Electrode Prepared By Improvement One-Time Dipping and Carbonization Method
Authors: Hao Tianqi , Wang Wei , Yu Dan 
Published: February 2020

In the field of soft electronic devices, flexible supercapacitor has received dramatical attention due to their appealing properties like lightweight, flexible, and environment friendly. To get the ideal flexibility of the supercapacitor, it is a key point to get a solid flexible substrate, which not only preserve the original physical properties of fabric but also offers self-supported scaffold for active materials. Among the different flexible substrate, cotton fabric is a good choice owing to the properties like low price, easily available and hydrophilicity, in which the hydroxyl groups make it favorable for adsorbing water and reacting with active materials.
Carbon nanotubes are widely used electrode materials with the merits of high specific surface area, good chemical stability, low resistance, thermal stability, high flexibility and excellent electrical properties. However, it is hard to obtain ideal properties only combining carbon nanotubes with cotton, because the low capacity of carbon nanomaterials. Herein, we proposed a new method to prepare flexible carbon materials with high capacitance.
First, we prepared flexible supercapacitor electrode based on carboxyl functionalized multiwalled carbon nanotubes (MWCNTs-COOH) and cotton fabric by a facile and highly efficient one-time dipping method under the condition of high pressure and temperature. After this process, MWCNTs-COOH coated on cotton fiber uniformly and winding together because of the presence of electrostatic interaction, van der Waals’ force and hydrogen bond between the oxygen-containing functional groups on MWCNTs-COOH and cotton fibers.
Second, the sample was dipped in solution of poly(ethylene oxide) (PEO) for improving the carbon content and strengthen the composite structure after carbonization. At last, the above sample was dealt with pre-oxidation and carbonization to get the final composite. Pre-oxidation was used to induce oxygen-containing groups and obtain stable skeleton. Carbonization is beneficial to increase the carbon content and get stable structure with bitter melon surface-shape, which can supply large specific area and mesoporous to store and transport electrons, leading to a high capacitance.
Therefore, the composite possessed excellent electrochemical performance with a high capacitance of 94.3 F g-1 at a current rate of 0.81 A g-1, and a good capacitance retention with over 96% after 3000 cycles. The prepared flexible supercapacitor electrode also showed good flexibility (93% capacitance retention after bending 60 times). Considering these good electrochemical performances, they are expected to be useful for practical applications in the field of supercapacitor.

Figure 1
Carbon Nanotubes Derived from Plastic Waste- a New Wave of Materials for Circular Economy
Authors: Lisak Grzegorz , Giannis Apostolos , Ahamed Ashiq , Moo James Guo Sheng , Veksha Andrei , Ge Liya , Weechachanchai Piyarat 
Published: February 2020

Large amounts of plastic waste are generated worldwide. Owing to the lack of profitable solutions, the recycling rates for waste plastics are low. A new approach is required to convert mixed plastics into valuable products with potential monetary benefits to encourage waste collection and recovery, thus increasing circular economy concepts in waste management.
This study focuses on the development of carbon based materials, such as carbon nanotubes (CNTs) from plastic waste (Fig. 1) containing high (H-PET) and low PET (L-PET) content and their subsequent application as materials for electrodes and the use in various analytical and process engineering systems.
The plastic-derived CNTs were evaluated as electrocatalysts for hydrogen evolution (HER) and oxygen reduction reaction (ORR). The results from HER and ORR study were found comparable or better to the ones using commercial CNTs. The plastic waste derived CNTs were also evaluated as electrodes in various analytical applications, e.g. support and solid contact for ion-selective electrodes in potentiometry and detection of analytes with increased sensitivity in voltammetry. The results were compared to commercially available electrodes and materials derived from pure feedstock. Life cycle assessment (LCA) was conducted in order to identify the environmental impact and benefits of using waste over pure feedstock derived carbon materials in analytical applications. The results indicate that waste derived material perform equally well in analytical applications as the ones derived from pure feedstock. Furthermore, LCA indicates that the use of waste derived materials result in much lower environmental impacts compared to the pure feedstock derived carbon materials.
This study strongly encourages the use of waste derived carbon materials in order to increase the circular economy concepts and decrease environmental impacts connected to material development and the use of materials in various applications.
Fig. 1. Plastic waste derived CNTs.

Figure 1
A Novel Si/C Composite as a High Capacity Anode Material for Lithium-ion Batteries
Authors: Jeehee Lee , Joonsup Kim , Sangjin Kim , Cho Jaephil , Namhyeong Kim 
Published: February 2020

Silicon based electrode materials for Li-ion battery have attracted great attention due to the high theoretical capacity of 4212 mAh/g (3.75 moles of Li per mole of Si) compared to graphite (1 mol Li per 6 mol C) used in commercial LIBs. Unfortunately, practical applications of silicon as an anode material exhibit the huge volume change (>300%) during the alloying / dealloying process with Li, which would result in the loss of electrical conductivity, dramatic pulverization of silicon, and consequently a rapid capacity fading in the cycling. To alleviate this problem, silicon nanosized or nanostructures materials have been suggested, which can increase the transport of electron and lithium ion and reduce mechanical stress during cycling, resulting in improved electrochemical performance. Among these nanostructures, the combination with carbon is becoming attractive and important material because it improves the electric conductivity and plays a role of a buffer of volume expansion.
In this research, a novel composite electrode material consisting of nanocrystalline silicon and porous graphite has been developed as an anode candidate for LIB. Nanocrystalline silicon was coated onto porous graphite via chemical vapor decomposition of SiH4 gas and subsequently pitch coating was carried out, which is known for a good method for preventing the natural oxidation of silicon layer and improving capacity.
We analyzed electrochemical properties of blended anode with graphite and nanocrystalline silicon­-porous graphite composite material. The capacity retention of the blending anode for nanocrystalline silicon­-porous graphite is 96% after 50 cycles with high coulombic efficiency of 90.1%, which is improved electrochemical performance compared with silicon non-porous graphite composite anode. Especially, the nanocrystalline silicon­-porous graphite composite material has lower expansion of electrode, comparing with silicon non-porous graphite composite material. The expansion of the nanocrystalline silicon­-porous graphite composite electrode is 42% after 1 cycle, while the expansion of the silicon non-porous graphite composite is 62% after 1 cycle. These improvements are attributed to the porous carbon shell, which reduces the cell expansion, prevents rupture of electrical path, stabilize the cycle performance.
(Plenary) Challenge for Innovation of Li-S Battery System
Authors: Sakaebe Hikari 
Published: February 2020

Policy recommendations of the electrification of the vehicles have been issued all over the world in these years. Energy density is one of the important keywords for realizing such policies. Several novel systems have been investigated, and Li-S system is quite promising among them. Leading research organizations and start-up companies have manufactured the trial prototype Li-S cell with energy density of 300-400 Wh/kg. And Li-S batteries application is not limited to vehicles.
We have tried to innovate the conventional Li-S battery using metal polysulfides like a-TiS4
1,2, Li8FeS5
3, 4, VS4
5, and so on in RISING2 (Research and Development Initiative for Scientific Innovation of New Generation Batteries 2) project. Sulfur is connected to metal atom and dissolution of Li polysulfides into the electrolyte was greatly suppressed. Quite recently 8 Ah cell was constructed and energy density of more than 310 Wh/kg was confirmed. Project target is to confirm 500 Wh/kg by prototype cell for innovative batteries in the end of FY2020. In the presentation, RISING2 activity, state of the art of the Li-S and our recent progress will be introduced.
Acknowledgement
This work was financially supported by RISING2 project by NEDO and METI.
References
1. A. Sakuda, T. Takeuchi, H. Sakaebe, et al., Electrochem. Commun., 31 (2013) 71
2. A. Sakuda, H. Sakaebe, T. Takeuchi, et al., J. Am. Chem. Soc., 139 (2017) 8796.
3. T. Takeuchi, H. Sakaebe, et al., J. Electrochem. Soc., 162 (2015) A1745.
4. T. Takeuchi, H, Sakaebe, et al., Solid State Ionics, 320 (2018), 378.
5. K. Koganei, T. Takeuchi, H. Sakaebe, et al., Solid State Ionics, 323 (2018) 32.
(Invited) Perspectives and Challenges of Next Generation Automotive Li-Ion Materials and Cells
Authors: Paschos Odysseas 
Published: February 2020

The development of e-mobility is at a tipping point with increasingly optimistic forecasts for the future market share of electric vehicles. Nonetheless, for electric vehicles to achieve mass-market penetration, a further improvement in the ratio between driving range and costs is mandatory. Different strategies are considered to increase electric range, including the optimization of battery pack, cell, and electrode. However the largest impact on energy density could be realized through the introduction of novel cathode and anode materials. There are a number of electrode materials currently in the research or development stage. Nevertheless, only a few of them have chances to meet automotive requirements, particularly in terms of lifetime and safety. Considerable improvements in these respects are still required, before a possible industrialization of the new generations of batteries for automotive application can be envisaged. In parallel, more revolutionary concepts based on post-lithium full-solid-state systems are evolving and could offer an even larger improvement potential.
This presentation will outline the potential and limits of present material concepts from a car manufacturer point of view. In particular, it will address open issues to be solved in the future development of electric energy storage technologies for automotive applications.
(Invited) Progress on Hybrid Gel Polymer Electrolyte and Solid Electrolyte for Lithium Ion Batteries
Authors: Bascour Dominique , Braida Marc-David , Gloesener Daniel , Abusleme Julio A. , Rouault Helene , Besnard Gaelle , Mourzagh Djamel , Salomon Jérémie 
Published: February 2020

Next generation batteries will have to provide high performances with reduced costs and safety advantage compared to the current lithium-ion products based on liquid electrolyte technology. For doing so, an appealing solution is to reformulate the electrolyte in a nonflammable form, such as a quasi solid state. Solvay, as a raw materials provider to battery manufacturers, develops components for next generation electrolyte materials.
The first part of the talk will focus on our Solgain™ solution. This technology, based on a hybrid organic/inorganic network combined with trapped liquid electrolyte, exhibits high ionic conductivity, high flexibility and good mechanical strength in addition to good electrochemical performances. Safety concern will be discussed and progress achieved so far on advanced Li-Ion batteries will be presented.
The second part of the talk will be focused toward solutions for Solid State Batteries. All-solid-state batteries using inorganic solid electrolytes and composite electrolytes are considered as promising energy storage systems because of their safety and long life. We will discuss the pathway and product development that Solvay has established to propose full solid state battery materials for future market needs.
(Invited) Anionic and Cationic Substitution to Control the Properties of Vanadium Fluorophosphates for Li and Na-Ion Batteries
Authors: Croguennec Laurence , Boivin Edouard , Nguyen Hoang Bao Long , Broux Thibault , Chotard Jean-Noël , Olchowka Jacob , Fauth François , Iadecola Antonella , Carlier Dany , Masquelier Christian 
Published: February 2020

Optimized carbon-coated Na3V2(PO4)2F3 showed exceptional rate and electrochemical cycling capabilities, more than 4000 times at 1 C rate, as demonstrated by performance of hard carbon//Na3V2(PO4)2F3 18650 prototypes of 75 Wh kg−1.1 These attractive results, among others, attract a renewed interest in the field of Na-ion and Li-ion batteries for vanadium fluoride phosphates. The control of their electrochemical performance requires the careful tuning of the oxygen and thus vanadyle-type defects’ concentration in these materials. Indeed, the competition between the ionic V3+−F bond and the covalent V4+=O bond has a major effect on the structure of the pristine materials, and thus on the phase diagram and redox mechanisms involved upon their cycling in batteries.
It will be illustrated for series of LiVPO4F1-yOy
2,3 and Na3V2-xMx(PO4)2F3-yOy
1, 4-6 phases combining mainly Synchrotron X-ray diffraction and spectroscopy studies. Original, probably firstly unexpected, crystal chemistry and redox activity will be discussed.
Acknowledgements:
The authors thank the European Union’s Horizon 2020 Research and Innovation Program under grant agreement No 646433-NAIADES, the French National Research Agency (STORE-EX Labex Project ANR-10-LABX-76-01, HIPOLITE Progelec Project ANR-12-PRGE-0005-02 and SODIUM Descartes Project ANR-13-RESC-0001-02), and the French RS2E and European ALISTORE-ERI networks for funding.
References

T. Broux, F. Fauth, N. Hall, Y. Chatillon, M. Bianchini, T. Bamine, J.-B. Leriche, E. Suard, D. Carlier, Y. Reynier, L. Simonin, C. Masquelier, and L. Croguennec - Small Methods
2018, 1800215-1800226

E. Boivin, R. David, J.-N. Chotard, T. Bamine, A. Iadecola, L. Bourgeois, E. Suard, F. Fauth, D. Carlier, C. Masquelier, and L. Croguennec - Chemistry of Materials
2018, 30 (16), 5682-5693

E. Boivin et al., submitted

T. Broux, T. Bamine, F. Fauth, L. Simonelli, W. Olszewski, C. Marini, M. Ménétrier, D. Carlier, C. Masquelier, and L. Croguennec - Chemistry of Materials
2016, 28(21), 7683-7692

T. Broux, T. Bamine, L. Simonelli, L. Stievano, F. Fauth, M. Ménétrier, D. Carlier, C. Masquelier, and L. Croguennec - Journal of Physical Chemistry C
2017, 121(8), 4103-4111

H. B. L. Nguyen et al., submitted
(Invited) Can a “Battery” Only be Used as a “Battery” or Can We Do More?
Authors: Liu Junnan , Wang Sunny , Goonetilleke Damian , Andersen Henrik L , Al Bahri Othman K , Sharma Neeraj 
Published: February 2020

Electrodes in batteries undergo a variety of changes during function. These include, but are not limited to intercalation, alloying and conversion reactions, evolution of the oxidation state of elements, crystal structures and the particle size (and distribution). Ideally minimal or controlled structural, morphological and macroscopic changes are desired for long term rechargeable battery function, and indeed many electrodes undergo transitions that are both highly reversible and irreversible. Furthermore, a variety of tools exist to probe these changes both in an in situ/operando and ex situ manner, e.g. Raman and NMR spectroscopy, X-ray, electron and neutron diffraction, to name a few techniques.
This presentation will detail two inter-related but unconventional aspects of research recently performed by our group.
We have been working towards using batteries or electrochemical cells as part of a synthetic strategy, whereby the changes induced by electrochemical reactions are purposefully used to generate new phases. These new phases are likely feature new properties and possibly new functionalities thus new applications. The energy storage aspects of the battery are replaced with the synthetic flexibility provided by applying controlled amounts of charge, for controlled amounts of time and being able to visualise changes using various in situ methods.
We have coined the term electrochemically activated solid state synthesis, whereby an electrode reacted in an electrochemical cell is subsequently extracted and heated resulting in the generation of a range of new or metastable phases, most of which have not been previously reported. This has been demonstrated for materials within the Ta1-x­NbxVO5 and Sc2W3-xMoxO12 families of electrodes used in Li, Na and K-based cells. A multitude of phase transitions are found with thermal treatments approximately at the onset of the decomposition of the binder used in the electrode. The talk will highlight the electrode preparation parameter space that can result in the generation of new phases, the identification of the phases and preliminary development of the mechanistic model associated with the synthetic strategy.
The second part of this talk will detail our recent investigation into solar batteries, where an electrode is able to both generate photocurrent and store charge carriers with exposure to light. We detail a new in situ electrochemical cell used to verify structural evolution (charge storage) during photo-irradiation of a MoO3 electrode providing direct experimental evidence for this process.
The culmination of these ideas allows batteries to be more than batteries, or possibly more appropriately it allows electrodes to have multiple functions in electrochemical cells.
(Keynote) Polyanionic Compounds for K-Ion Batteries
Authors: Hosaka Tomooki , Shimamura Tomoaki , Kubota Kei , Komaba Shinichi 
Published: February 2020

We reported the high working voltage of K-ion battery (KIB) comparable to Li-ion and higher than Na-ion thanks to the standard potential of potassium is lower than those of lithium and sodium in non-aqueous electrolyte [1,2]. In 2015, our group reported graphite negative electrode delivering 250 mAh g-1 or higher with excellent reversibility [1]. Furthermore, a Prussian blue analogue (PBA) of K2Mn[Fe(CN)6] demonstrated highly reversible potassium insertion/extraction and 4 V operation, realizing a 4 V-class K2Mn[Fe(CN)6]/graphite full cell [3]. The previous studies revealed that a three-dimensional open framework structure of PBAs is suitable for insertion/extraction of large K+ ion. Addition to the PBAs, polyanionic compounds are potential positive electrode materials for KIBs due to their open framework structure and inductive effect. In this talk, our recent studies on potassium insertion into various polyanionic compounds, such as heterosite FePO4, KFePO4, KMnPO4, K2FeP2O7, K2MnP2O7, KVPO4F, KVOPO4, monoclinic KFeSO4F, and orthorhombic KFeSO4F (o-KFeSO4F) [4,5], will be presented to give a perspective of potassium insertion material design.
Because K+ ion is too large to occupy the octahedral site in heterosite FePO4 prepared from olivine-type LiFePO4, the crystallinity of heterosite FePO4 significantly decreases after potassium insertion. On the other hand, KVPO4F, KVOPO4, and o-KFeSO4F possess the KTiOPO4-type structure providing large channels to diffuse K+ ion and show the reversible potassium insertion/extraction properties and excellent rate performance. These results indicate that the crystal structure plays a key factor for reversible potassium insertion and rate performance. Moreover, the average discharge voltage of KVPO4F and KVOPO4 is as high as 4 V in a K half-cell. That of o-KFeSO4F is 3.6 V, which is notably high redox potential of Fe2+/Fe3+ due to the strong inductive effect of SO4
2- and F- on the Fe2+/3+ couple. The cycling stability of these high-voltage electrode materials is highly improved by using highly concentrated potassium salt solutions [6]. From these results, we will present our future insight into electrochemical potassium insertion chemistry for high voltage battery applications.

References

[1] S. Komaba et al., Electrochem. Commun., 60, 172 (2015).
[2] K. Kubota, T. Hosaka, S. Komaba et al., Chem. Rec., 18, 459 (2018).
[3] X. Bie, K. Kubota, S. Komaba et al., J.
Mater. Chem. A, 5, 4325 (2017).
[4] K. Chihara, S. Komaba et al., Chem. Commun.,
53, 5208–5211 (2017).
[5] T. Hosaka, T. Shimamura, S. Komaba et al., Chem. Rec., in-press

[6] T. Hosaka, Kei Kubota, S. Komaba et al., Chem. Commun., 54, 8387 (2018).