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2. Strategies towards enabling lithium metal in batteries: interphases and electrodes

Author

Horstmann, Birger, Shi, Jiayan, Amine, Rachid, Werres, Martin, He, Xin, Jia, Hao, Hausen, Florian, Cekic-Laskovic, Isidora, Wiemers-Meyer, Simon, Lopez, Jeffrey, Galvez-Aranda, Diego, Baakes, Florian, Bresser, Dominic, Su, Chi-Cheung, Xu, Yaobin, Xu, Wu, Jakes, Peter, Eichel, Rüdiger-A, Figgemeier, Egbert, Krewer, Ulrike, Seminario, Jorge M, Balbuena, Perla B, Wang, Chongmin, Passerini, Stefano, Shao-Horn, Yang, Winter, Martin, Amine, Khalil, Kostecki, Robert, and Latz, Arnulf

Subjects
Engineering, Materials Engineering, Chemical Sciences, Physical Chemistry, Affordable and Clean Energy, Energy
Abstract

Despite the continuous increase in capacity, lithium-ion intercalation batteries are approaching their performance limits. As a result, research is intensifying on next-generation battery technologies. The use of a lithium metal anode promises the highest theoretical energy density and enables use of lithium-free or novel high-energy cathodes. However, the lithium metal anode suffers from poor morphological stability and Coulombic efficiency during cycling, especially in liquid electrolytes. In contrast to solid electrolytes, liquid electrolytes have the advantage of high ionic conductivity and good wetting of the anode, despite the lithium metal volume change during cycling. Rapid capacity fade due to inhomogeneous deposition and dissolution of lithium is the main hindrance to the successful utilization of the lithium metal anode in combination with liquid electrolytes. In this perspective, we discuss how experimental and theoretical insights can provide possible pathways for reversible cycling of two-dimensional lithium metal. Therefore, we discuss improvements in the understanding of lithium metal nucleation, deposition, and stripping on the nanoscale. As the solid-electrolyte interphase (SEI) plays a key role in the lithium morphology, we discuss how the proper SEI design might allow stable cycling. We highlight recent advances in conventional and (localized) highly concentrated electrolytes in view of their respective SEIs. We also discuss artificial interphases and three-dimensional host frameworks, which show prospects of mitigating morphological instabilities and suppressing large shape change on the electrode level.

Published
2021

5. Fast interfacial electrocatalytic desolvation enabling low‐temperature and long‐cycle‐life aqueous Zn batteries

Author

Wang, Jian, primary, Hu, Hongfei, additional, Jia, Lujie, additional, Zhang, Jing, additional, Zhuang, Quan, additional, Li, Linge, additional, Zhang, Yongzheng, additional, Wang, Dong, additional, Guan, Qinghua, additional, Hu, Huimin, additional, Liu, Meinan, additional, Zhan, Liang, additional, Adenusi, Henry, additional, Passerini, Stefano, additional, and Lin, Hongzhen, additional

Published
2024
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12. Emerging Battery Technologies to Boost the Clean Energy Transition

Author

Passerini, Stefano, Barelli, Linda, Baumann, Manuel, Peters, Jens, and Weil, Marcel

Subjects
Energy Storage, Electrochemical energy storage, large-scale energy storage, energy storage for de-carbonization, emerging batteries, thema EDItEUR::T Technology, Engineering, Agriculture, Industrial processes::TG Mechanical engineering and materials::TGM Materials science, thema EDItEUR::P Mathematics and Science::PN Chemistry, thema EDItEUR::T Technology, Engineering, Agriculture, Industrial processes::TH Energy technology and engineering::THV Alternative and renewable energy sources and technology
Abstract

This open access book provides a totally new perspective on the rapidly developing sector of electrochemical energy storage, putting a spotlight on their sustainability under consideration of the latest developments and emerging future technologies. A number of selected, high-level authors from different disciplines discuss the potential contribution of batteries to a cleaner society, the need for new battery concepts, necessary new chemistries and their sustainability. These include not only analyses of the most relevant technological developments in the field, but also the latest state of knowledge in terms of their applicative functionalities in transport and stationary applications within the clean energy transition framework, their potential environmental impacts, resource demands and social impacts, and the corresponding methodological advances. All these aspects are analyzed on micro-level (i.e., for the specific technology), but also on macro-scale i.e., from a systemic perspective, providing a glimpse on how emerging battery systems might cover future energy storage demand. By taking a prospective and interdisciplinary viewpoint, this book will be of interest for a broad field of readers interested in electrochemistry, engineering with particular focus on electric grids and on-board systems and energy system analysis, but also those worried about the sustainability and societal challenges related with the energy transition(s).

Published
2024
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26. Density Functional Theory screening of gas-treatment strategies for stabilization of high energy-density lithium metal anodes

Author

Koch, Stephan L., Morgan, Benjamin J., Passerini, Stefano, and Teobaldi, Gilberto

Subjects
Condensed Matter - Materials Science
Abstract

To explore the potential of molecular gas treatment of freshly cut lithium foils in non-electrolyte based passivation of high energy-density Li anodes, density functional theory (DFT) has been used to study the decomposition of molecular gases on metallic lithium surfaces. By combining DFT geometry optimization and Molecular Dynamics, the effects of atmospheric (N2, O2, CO2) and hazardous (F2, SO2) gas decomposition on Li(bcc) (100), (110), and (111) surfaces on relative surface energies, work functions, and emerging electronic and elastic properties are investigated. The simulations suggest that exposure to different molecular gases can be used to induce and control reconstructions of the metal Li surface and substantial changes (up to over 1 eV) in the work function of the passivated system. Contrary to the other considered gases, which form metallic adlayers, SO2 treatment emerges as the most effective in creating an insulating passivation layer for dosages <= 1 mono-layer. The substantial Li->adsorbate charge transfer and adlayer relaxation produce marked elastic stiffening of the interface, with the smallest change shown by nitrogen-treated adlayers.

Published
2015

29. Layered Oxide Material as a Highly Stable Na‐ion Source and Sink for Investigation of Sodium‐ion Battery Materials.

Author

Wu, Fanglin, Li, Huihua, Diemant, Thomas, Mullaliu, Angelo, Zhang, Huang, and Passerini, Stefano

Subjects
LITHIUM titanate, NEGATIVE electrode, SODIUM ions, TRANSITION metal oxides, LITHIUM, STANDARD hydrogen electrode, IRON
Abstract

Investigating Na‐ion battery (SIB) materials is complicated by the absence of a well‐performing (reference) electrode material since sodium metal cannot be considered as a quasi‐reference electrode. Taking advantage of the activity of both Ni and Mn, herein, the P2‐type and Mn‐rich Na0.6Ni0.22Al0.11Mn0.66O2 (NAM) material, known to be an excellent positive electrode, is investigated as a negative electrode. To prove NAM stability as both positive and negative electrode, symmetric cells have been assembled without pre‐sodiation, which showed a reversible capacity of 73 mA h g−1 and a remarkable capacity retention of 82.6 % after 500 cycles. The outstanding cycling performance is ascribed to the high stability of the active material at both the highest and lowest Na‐ion storage plateaus and the rather limited electrolyte decomposition and solid‐electrolyte‐interphase (SEI) formation occurring. The long‐term stability of NAM at both electrodes enables its use as a "reference" electrode for the investigation of other positive and negative electrode materials for SIBs, resembling the role played by lithium titanate (LTO) and lithium iron phosphate (LFP) in LIBs. [ABSTRACT FROM AUTHOR]

Published
2024
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33. A combined theoretical and experimental study of the influence of different anion ratios on lithium ion dynamics in ionic liquids

Author

Lesch, Volker, Jeremias, Sebastian, Moretti, Arianna, Passerini, Stefano, Heuer, Andreas, and Borodin, Oleg

Subjects
Condensed Matter - Materials Science
Abstract

In this paper we have investigated via experimental and simulations techniques the transport properties, in terms of total ionic conductivity and ion diffusion coefficients, of ionic liquids and lithium salt mixtures composed of two anions, bis(fluorosulfonyl)imide (FSI) and bis(trifluoromethanesulfonyl)imide (TFSI), and two cations, N-ethyl-N-methylimidazolium (emim) and lithium. The comparison of the experimental results with the simulations shows an exceptional agreement over a wide temperature range. Of particular interest is the high agreement achieved at lower temperature, which is a result of the extended simulation length of, at least, a factor of 5 compared with previous work. The results show as the addition of TFSI favor the formation of lithium dimers (Li+ - TFSI- - Li+). A closer analysis of such dimers shows that involved lithium ions move nearly as fast as single lithium ions although they have a different coordination and much slower TFSI exchange rates., Comment: 21 pages, 9 figures; JPC submitted

Published
2014

38. Hysteresis effects in the potential-dependent double layer capacitance of room temperature ionic liquids at a polycrystalline platinum interface

Author

Drueschler, Marcel, Huber, Benedikt, Passerini, Stefano, and Roling, Bernhard

Subjects
Condensed Matter - Materials Science, Condensed Matter - Disordered Systems and Neural Networks
Abstract

This paper has been withdrawn by the author since it had been submitted to Journal of Physical Chemistry C., Comment: This paper has been withdrawn

Published
2009

41. Investigation of the Stability of the Poly(ethylene oxide)|LiNi1‐x‐y CoxMnyO2 Interface in Solid‐State Batteries.

Author

Yusim, Yuriy, Hunstock, Dirk F., Mayer, Alexander, Bresser, Dominic, Passerini, Stefano, Janek, Jürgen, and Henss, Anja

Subjects
SOLID electrolytes, HIGH voltages, SCANNING electron microscopy, IMPEDANCE spectroscopy, POLYELECTROLYTES, HIGH temperatures
Abstract

While solid‐state batteries (SSBs) comprising poly(ethylene oxide) (PEO) based electrolytes are successfully commercialized already for operation at elevated temperature, the selection of the cathode active material (CAM) has so far been limited to LiFePO4. When using high‐voltage CAMs such as LiNi1‐x‐yCoxMnyO2 (NCM), the cells experience fast capacity fading – the cause of which is not consistently understood in literature. In this study, electrochemical impedance spectroscopy measurements in a three‐electrode setup are applied to confirm that the NCM|PEO interface is indeed the Achilles' heel in PEO‐based SSBs at high voltages. In this regard, the interfacial stability on the cathode side depends not only on the upper cut‐off voltage, but also on the molecular weight of PEO, strongly affecting the cell performance. Scanning electron microscopy images of the cathodes after cycling suggest that at high voltages interfacial degradation leads to fragmentation of the polymer backbone and to a decrease in viscosity of the solid polymer electrolyte. Overall, the results help to understand the detrimental processes occurring in PEO‐based SSBs in combination with high‐voltage cathodes. [ABSTRACT FROM AUTHOR]

Published
2024
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42. Precipitation Stripping of V(V) as a Novel Approach for the Preparation of Two-Dimensional Transition Metal Vanadates.

Author

Sánchez-Loredo, María Guadalupe, Chekhonin, Paul, Ebert, Doreen, Fischer, Ulrike, Liu, Xu, Möckel, Robert, Labrada-Delgado, Gladis Judith, Passerini, Stefano, and Kelly, Norman

Subjects
TRANSITION metals, VANADATES, ALKALINE solutions, LITHIUM cells, VANADIUM, METAL ions
Abstract

Cobalt, nickel, manganese and zinc vanadates were synthesized by a hydrometallurgical two-phase method. The extraction of vanadium (V) ions from alkaline solution using Aliquat® 336 was followed by the production of metal vanadates through precipitation stripping. Precipitation stripping was carried out using solutions of the corresponding metal ions (Ni (II), Co (II), Mn (II) and Zn (II), 0.05 mol/L in 4 mol/L NaCl), and the addition time of the strip solution was varied (0, 1 and 2 h). The time-dependent experiments showed a notable influence on the composition, structure, morphology and crystallinity of the two-dimensional vanadate products. Inspired by these findings, we selected two metallic vanadate products and studied their properties as alternative cathode materials for nonaqueous sodium and lithium metal batteries. [ABSTRACT FROM AUTHOR]

Published
2024
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