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From Liquid to Solid, the Alternation of Generations toward Solid-State...
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From Liquid to Solid, the Alternation of Generations toward Solid-State Batteries

A special issue of Batteries (ISSN 2313-0105).

Deadline for manuscript submissions: closed (31 March 2024) | Viewed by 6743

Special Issue Editors

Prof. Dr. Kai Peter Birke

E-Mail Website
Guest Editor
Chair for Electrical Energy Storage Systems, Institute for Photovoltaics, University of Stuttgart, Pfaffenwaldring 47, 70569 Stuttgart, Germany
Interests: battery cell research; battery system technology; battery block building kits; modeling of battery cells and battery systems; battery state estimation (state of charge, state of health, state of function); implementation of artificial intelligence for detrmination of battery cell parameters with enhanced accuracy; digital twins for battery cells and battery systems; high boiling point safety enhanced electrolytes; double layer capacitors; pseudo 3D-capacitors; power to X (X = gas, liquid, solid)
Special Issues, Collections and Topics in MDPI journals
Dr. Alexander Fill

E-Mail Website
Guest Editor
Chair for Electrical Energy Storage Systems, Institute for Photovoltaics, University of Stuttgart, Pfaffenwaldring 47, 70569 Stuttgart, Germany
Interests: battery cell research; novel battery diagnostics; battery modeling; battery characterization; battery cell state estimation; cell-to-cell variances; local cell state imbalances
Special Issues, Collections and Topics in MDPI journals

Special Issue Information

Dear Colleagues,

Batteries are anticipated to become an indispensable part of the CO2-free value chain and energy supply, a development driven by the high cost involved in energy supply, which can be by energy density enhancement employing similar raw materials. Li-Ion technology is one of the most promising candidates, currently receiving the most attention. However, energy density can be further distinctly enhanced using Li-metal instead of graphite as a negative electrode. In optimal cases, Li containers are positive electrodes, and lithium is deposited upon first charge. Solid-state electrolytes are considered the only enabler because they guarantee comparable coulombic efficiencies vs. Li-Ion batteries. These efficiencies must exceed 99.9%—while 98% or 99% (the limits for liquid electrolytes) may seem high enough, they are still insufficient. However, the basic idea of solid electrolytes for such batteries is the immobilization of all species apart from lithium where side reactions are suppressed to fulfil the extraordinary demand for coulombic efficiencies. Thus, systems such as hybrid solid–solid batteries (HySolSol), hybrid solid–gel batteries (HySolGel), and hybrid solid–liquid batteries (HySolLiq) are also receiving a tremendous amount of interest. In addition, high-voltage cathodes could become also feasible employing such approaches. Success can only be achieved through effective dendrite suppression. Due to the incredible progress in the conductivity enhancement of solid electrolytes in the last four decades, we can conclude that the time has arrived for them to be pushed to the forefront, with focused research exploring the possibilities and challenges.

Prof. Dr. Kai Peter Birke
Dr. Alexander Fill
Guest Editors

Manuscript Submission Information

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Submitted manuscripts should not have been published previously, nor be under consideration for publication elsewhere (except conference proceedings papers). All manuscripts are thoroughly refereed through a single-blind peer-review process. A guide for authors and other relevant information for submission of manuscripts is available on the Instructions for Authors page. Batteries is an international peer-reviewed open access monthly journal published by MDPI.

Please visit the Instructions for Authors page before submitting a manuscript. The Article Processing Charge (APC) for publication in this open access journal is 2700 CHF (Swiss Francs). Submitted papers should be well formatted and use good English. Authors may use MDPI's English editing service prior to publication or during author revisions.

Keywords

  • solid-state batteries employing one electrolyte
  • hybrid solid–solid batteries (HySolSol)
  • hybrid solid–gel batteries (HySolGel)
  • hybrid solid–liquid batteries (HySolLiq)
  • prerequisites for electrolytes for the abovementioned battery types (review papers)
  • electrolytes and electrolyte systems for the abovementioned battery types
  • stabilizing phase boundaries
  • negative electrodes made from in situ Li deposition upon first charge (“Anode free” set up)
  • dendrite suppression
  • high-voltage electrodes with solid electrolytes as enabler
  • tuning the SEI (Solid Electrolyte Interphase) by novel anode constructions

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Published Papers (4 papers)

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Research

18 pages, 2333 KiB  
Article
Proof of Concept: The GREENcell—A Lithium Cell with a F-, Ni- and Co-Free Cathode and Stabilized In-Situ LiAl Alloy Anode
by Kathrin Schad, Dominic Welti and Kai Peter Birke
Batteries 2023, 9(9), 453; https://doi.org/10.3390/batteries9090453 - 4 Sep 2023
Viewed by 1759
Abstract
Given the rising upscaling trend in lithium-ion battery (LiB) production, there is a growing emphasis on the environmental and economic impacts alongside the high energy density demands. The cost and environmental impact of battery production primarily arise from the critical elements Ni, Co, [...] Read more.
Given the rising upscaling trend in lithium-ion battery (LiB) production, there is a growing emphasis on the environmental and economic impacts alongside the high energy density demands. The cost and environmental impact of battery production primarily arise from the critical elements Ni, Co, and F. This drives the exploration of Ni-free and Co-free cathode alternatives such as LiMn2O4 (LMO) and LiFePO4 (LFP). However, the absence of Ni and Co results in reduced capacity and insufficient cyclic stability, particularly in the case of LMO due to Mn dissolution. To compensate for both low cathode capacitance and low cycle stability, we propose the GREENcell, a lithium cell combining a F-free polyisobutene (PIB) binder-based LMO cathode with a stabilized in -situ LiAL alloy anode. A LiAl alloy anode with the chemical composition of LiAl already shows a theoretical capacity of 993 Ah·kg−1. Therefore, it promises extraordinarily higher energy densities compared to a commercial graphite anode with a capacity of 372 Ah·kg−1. Following an iterative development process, different optimization strategies, especially those targeting the stability of the Al-based anode, were evaluated. During Al foil selection, foil purity and thickness could be identified as two of the dominant influencing parameters. A pressed-in stainless steel mesh provides both mechanical stability to the anode and facilitates alloy formation by breaking up the Al oxide layer beforehand. Additionally, a binder-stabilized Al oxide or silicate layer is pre-coated on the Al surface, posing as a SEI-precursor and ensuring a uniform liquid electrolyte distribution at the phase boundary. Employing a commercially available Si-containing Al alloy mitigated the mechanical degradation of the anode, yielding a favorable impact on long-term stability. The applicability of the novel optimized GREENcell is demonstrated using laboratory coin cells with LMO and LFP as the cathode. As a result, the functionality of the GREENcell was demonstrated for the first time, and thanks to the anode stabilization strategies, a capacity retention of >70% after 200 was achieved, representing an increase of 32.6% compared to the initial Al foil. Full article
(This article belongs to the Special Issue From Liquid to Solid, the Alternation of Generations toward Solid-State Batteries)
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17 pages, 7093 KiB  
Article
Comparison of Different Current Collector Materials for In Situ Lithium Deposition with Slurry-Based Solid Electrolyte Layers
by Tina Kreher, Fabian Heim, Julia Pross-Brakhage, Jessica Hemmerling and Kai Peter Birke
Batteries 2023, 9(8), 412; https://doi.org/10.3390/batteries9080412 - 7 Aug 2023
Cited by 3 | Viewed by 2860
Abstract
In this paper, we investigate different current collector materials for in situ deposition of lithium using a slurry-based β-Li3PS4 electrolyte layer with a focus on transferability to industrial production. Therefore, half-cells with different current collector materials (carbon-coated aluminum, stainless [...] Read more.
In this paper, we investigate different current collector materials for in situ deposition of lithium using a slurry-based β-Li3PS4 electrolyte layer with a focus on transferability to industrial production. Therefore, half-cells with different current collector materials (carbon-coated aluminum, stainless steel, aluminum, nickel) are prepared and plating/stripping tests are performed. The results are compared in terms of Coulombic efficiency (CE) and overvoltages. The stainless steel current collector shows the best performance, with a mean efficiency of ηmean,SST=98%; the carbon-coated aluminum reaches ηmean,Al+C=97%. The results for pure aluminum and nickel indicate strong side reactions. In addition, an approach is tested in which a solvate ionic liquid (SIL) is added to the solid electrolyte layer. Compared to the cell setup without SIL, this cannot further increase the CE; however, a significant reduction in overvoltages is achieved. Full article
(This article belongs to the Special Issue From Liquid to Solid, the Alternation of Generations toward Solid-State Batteries)
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15 pages, 3931 KiB  
Article
High Flashpoint and Eco-Friendly Electrolyte Solvent for Lithium-Ion Batteries
by Marco Ströbel, Larissa Kiefer, Julia Pross-Brakhage, Jessica Hemmerling, Philipp Finster, Carlos Ziebert and Kai Peter Birke
Batteries 2023, 9(7), 348; https://doi.org/10.3390/batteries9070348 - 28 Jun 2023
Cited by 2 | Viewed by 2341
Abstract
Since Sony launched the commercial lithium-ion cell in 1991, the composition of the liquid electrolytes has changed only slightly. The electrolyte consists of highly flammable solvents and thus poses a safety risk. Solid-state ion conductors, classified as non-combustible and safe, are being researched [...] Read more.
Since Sony launched the commercial lithium-ion cell in 1991, the composition of the liquid electrolytes has changed only slightly. The electrolyte consists of highly flammable solvents and thus poses a safety risk. Solid-state ion conductors, classified as non-combustible and safe, are being researched worldwide. However, they still have a long way to go before being available for commercial cells. As an alternative, this study presents glyceryl tributyrate (GTB) as a flame retardant and eco-friendly solvent for liquid electrolytes for lithium-ion cells. The remarkably high flashpoint (TFP=174°C) and the boiling point (TBP=287°C) of GTB are approximately 150 K higher than that of conventional linear carbonate components, such as ethyl methyl carbonate (EMC) or diethyl carbonate (DEC). The melting point (TMP=−75°C) is more than 100 K lower than that of ethylene carbonate (EC). A life cycle test of graphite/NCM with 1 M LiTFSI dissolved in GTB:EC (85:15 wt) achieved a Coulombic efficiency of above 99.6% and the remaining capacity resulted in 97% after 50 cycles (C/4) of testing. The flashpoint of the created electrolyte is TFP=172°C and, therefore, more than 130 K higher than that of state-of-the-art liquid electrolytes. Furthermore, no thermal runaway was observed during thermal abuse tests. Compared to the reference electrolyte LP40, the conductivity of the GTB-based is reduced, but the electrochemical stability is highly improved. GTB-based electrolytes are considered an interesting alternative for improving the thermal stability and safety of lithium-ion cells, especially in low power-density applications. Full article
(This article belongs to the Special Issue From Liquid to Solid, the Alternation of Generations toward Solid-State Batteries)
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15 pages, 3807 KiB  
Article
Cycling of Double-Layered Graphite Anodes in Pouch-Cells
by Daniel Müller, Alexander Fill and Kai Peter Birke
Batteries 2022, 8(3), 22; https://doi.org/10.3390/batteries8030022 - 1 Mar 2022
Cited by 5 | Viewed by 3292
Abstract
Incremental improvement to the current state-of-the-art lithium-ion technology, for example regarding the physical or electrochemical design, can bridge the gap until the next generation of cells are ready to take Li-ions place. Previously designed two-layered porosity-graded graphite anodes, together with LixNi [...] Read more.
Incremental improvement to the current state-of-the-art lithium-ion technology, for example regarding the physical or electrochemical design, can bridge the gap until the next generation of cells are ready to take Li-ions place. Previously designed two-layered porosity-graded graphite anodes, together with LixNi0.6Mn0.2Co0.2O2 cathodes, were analysed in small pouch-cells with a capacity of around 1 Ah. For comparison, custom-made reference cells with the average properties of two-layered anodes were tested. Ten cells of each type were examined in total. Each cell pair, consisting of one double-layer and one single-layer (reference) cell, underwent the same test procedure. Besides regular charge and discharge cycles, electrochemical impedance spectroscopy, incremental capacity analysis, differential voltage analysis and current-pulse measurement are used to identify the differences in ageing behaviour between the two cell types. The results show similar behaviour and properties at beginning-of-life, but an astonishing improvement in capacity retention for the double-layer cells regardless of the cycling conditions. Additionally, the lifetime of the single-layer cells was strongly influenced by the cycling conditions, and the double-layer cells showed less difference in ageing behaviour. Full article
(This article belongs to the Special Issue From Liquid to Solid, the Alternation of Generations toward Solid-State Batteries)
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