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Advances in Anode and Electrolyte Materials for Lithium-Ion Batteries and...
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Advances in Anode and Electrolyte Materials for Lithium-Ion Batteries and Beyond

A special issue of Batteries (ISSN 2313-0105). This special issue belongs to the section "Battery Materials and Interfaces: Anode, Cathode, Separators and Electrolytes or Others".

Deadline for manuscript submissions: 31 May 2024 | Viewed by 10630

Special Issue Editor

Dr. Argyrios Karatrantos

E-Mail Website
Guest Editor
Materials Research and Technology, Luxembourg Institute of Science and Technology, L-4362 Esch-sur-Alzette, Luxembourg
Interests: computational chemistry; batteries; organic solutions; polymer electrolytes; nanocomposites
Special Issues, Collections and Topics in MDPI journals

Special Issue Information

Dear Colleagues,

Lithium (Li) ion batteries have been used for a few decades as the main small- and medium-scale energy storage devices (electric vehicles), and as backup and smart-grid energy storage. However, sodium (Na), potassium (K) and multivalent (Mg, Ca, Al) ion batteries have emerged as candidates for medium- and large-scale stationary energy storage, mainly due to the abundance of Na+, K+, Mg2+, Ca2+, Al3+ ions in Nature, but also to the potential to surpass the energy density of lithium. Although many studies focus on lithium-ion batteries, only a few have been conducted in metal ion batteries beyond lithium.

One very important factor for the performance of metal-ion-based batteries and fast charge/discharge rates is the choice of organic electrolyte, since a good electrolyte can provide good ionic conductivity, high cycle life, and energy density, greatly reducing side reactions and electrochemical stability. Desirable properties for a good electrolyte include: (i) high polarity (dielectric constant ε > 15 is necessary for salt ion solvation and ion pairing limit), (ii) low viscosity to improve the cation mobility, (iii) chemical stability (to remain inert on the charged surfaces of the anode during cell operation), (iv) ability to remain liquid over a broad range of temperatures, and (v) safety (nontoxic and economical). Moreover, ionic liquids or ether-based electrolytes (polymer electrolytes) can be considered alternative electrolytes for high-performance rechargeable batteries. In addition, the research on anode materials and the passive layer between the electrolyte and anode (solid electrolyte interface, SEI) is also very limited for batteries beyond lithium. For instance, carbon-based materials (e.g., hard carbon, graphite, hollow carbon nanowires, carbon microspheres) represent a large category of anode materials, and are still considered the best, due to their natural abundance, low cost, and relatively good storage capacity. However, several other anode materials, such as nickel-titanium oxide, germanene nanosheets, phosphorus-based alloys etc., have recently been applied in novel rechargeable batteries.

There is therefore a need to develop research in this area in order to enable breakthrough development in beyond lithium-ion battery technology. This Special Issue of Batteries invites contributions addressing computational studies (DFT, molecular dynamics (ab-initio or classical), machine learning and theoretical models) in lithium-ion batteries and beyond, focusing on organic electrolyte phase, ionic liquids, ether-based electrolytes, anode materials, solid electrode interface, ion solvation, ion transport, transference number, and ionic conductivity.

Dr. Argyrios Karatrantos
Guest Editor

Manuscript Submission Information

Manuscripts should be submitted online at www.mdpi.com by registering and logging in to this website. Once you are registered, click here to go to the submission form. Manuscripts can be submitted until the deadline. All submissions that pass pre-check are peer-reviewed. Accepted papers will be published continuously in the journal (as soon as accepted) and will be listed together on the special issue website. Research articles, review articles as well as short communications are invited. For planned papers, a title and short abstract (about 100 words) can be sent to the Editorial Office for announcement on this website.

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

  • beyond lithium batteries
  • electrolytes
  • ionic liquids
  • ether-based electrolytes
  • polymer electrolytes
  • anode materials
  • ion transport
  • solvation
  • transference number
  • conductivity
  • solid electrolyte interface
  • molecular dynamics
  • DFT
  • machine learning
  • ab-initio

Published Papers (4 papers)

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Research

18 pages, 7189 KiB  
Article
Lithium Metal under Static and Dynamic Mechanical Loading
by Ed Darnbrough and David E. J. Armstrong
Batteries 2024, 10(1), 20; https://doi.org/10.3390/batteries10010020 - 03 Jan 2024
Viewed by 1602
Abstract
Macro-scale mechanical testing and finite element analysis of lithium metal in compression have been shown to suggest methods and parameters for producing thin lithium anodes. Consideration of engineering and geometrically corrected stress experiments shows that the increasing contact area dominates the stress increase [...] Read more.
Macro-scale mechanical testing and finite element analysis of lithium metal in compression have been shown to suggest methods and parameters for producing thin lithium anodes. Consideration of engineering and geometrically corrected stress experiments shows that the increasing contact area dominates the stress increase observed during the compression, not strain hardening, of lithium. Under static loading, the lithium metal stress relaxes, which means there is a speed of deformation (engineering strainrate limit of 6.4×10−5 s−1) where there is no increase in stress during compression. Constant displacement tests show that stress relaxation depends on the initial applied stress and the amount of athermal plastic work within the material. The finite element analysis shows that barrelling during compression and the requirement for high applied stresses to compress lithium with a small height-to-width ratio are friction and geometric effects, respectively. The outcomes of this work are discussed in relation to the diminishing returns of stack pressure, the difficulty in closing voids, and potential methods for designing and producing sub-micron lithium anodes. Full article
(This article belongs to the Special Issue Advances in Anode and Electrolyte Materials for Lithium-Ion Batteries and Beyond)
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14 pages, 6035 KiB  
Article
The Effect of Different Amounts of Conductive Carbon Material on the Electrochemical Performance of the LiFePO4 Cathode in Li-Ion Batteries
by Debabrata Mohanty, Min-Jie Chang and I-Ming Hung
Batteries 2023, 9(10), 515; https://doi.org/10.3390/batteries9100515 - 20 Oct 2023
Cited by 1 | Viewed by 1877
Abstract
LiFePO4 (LFP) has undergone extensive research and is a promising cathode material for Li-ion batteries. The high interest is due to its low raw material cost, good electrochemical stability, and high-capacity retention. However, poor electronic conductivity and a low Li+ diffusion [...] Read more.
LiFePO4 (LFP) has undergone extensive research and is a promising cathode material for Li-ion batteries. The high interest is due to its low raw material cost, good electrochemical stability, and high-capacity retention. However, poor electronic conductivity and a low Li+ diffusion rate decrease its electrochemical reactivity, especially at fast charge/discharge rates. In this work, the volumetric energy density of lithium-ion batteries is successfully increased by using different amounts of conductive carbon (Super P) in the active material content. The particle size and morphology of the electrode material samples are studied using field emission scanning electron microscopy and dynamic light scattering. Two-point-probe DC measurements and adhesive force tests are used to determine the conductivity and evaluate adhesion for the positive electrode. Cyclic voltammetry, electrochemical impedance spectroscopy (EIS), and charge/discharge tests are used to analyze the electrochemical properties of the battery. The samples containing 88% LFP, 5.5% Super P, and 6.5% PVDF perform best, with discharge capacities reaching 169.8 mAh g−1 at 0.1 C, and they can also manage charging/discharging of 5 C. EIS indicates that this combination produces the lowest charge-transfer impedance (67 Ω) and the highest Li+ ion diffusion coefficient (5.76 × 10−14 cm2 s−1). Full article
(This article belongs to the Special Issue Advances in Anode and Electrolyte Materials for Lithium-Ion Batteries and Beyond)
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13 pages, 4174 KiB  
Article
Fast Ion Transfer Associated with Dehydration and Modulation of Hydration Structure in Electric Double-Layer Capacitors Using Molecular Dynamics Simulations and Experiments
by Shunsuke Hasumi, Sogo Iwakami, Yuto Sasaki, Sharifa Faraezi, Md Sharif Khan and Tomonori Ohba
Batteries 2023, 9(4), 212; https://doi.org/10.3390/batteries9040212 - 01 Apr 2023
Cited by 2 | Viewed by 1468
Abstract
Carbon materials, such as graphite and activated carbon, have been widely used as electrodes in batteries and electric double-layer capacitors (EDLCs). Graphene, which has an extremely thin sheet-like structure, is considered as a fundamental carbon material. However, it was less investigated as an [...] Read more.
Carbon materials, such as graphite and activated carbon, have been widely used as electrodes in batteries and electric double-layer capacitors (EDLCs). Graphene, which has an extremely thin sheet-like structure, is considered as a fundamental carbon material. However, it was less investigated as an electrode material than graphite and activated carbons. This is because graphene is a relatively new material and is difficult to handle. However, using graphene electrodes can enhance the performance of nanodevices. Here, the performance of EDLCs based on single-layer and bilayer graphene electrodes in LiCl, NaCl, and KCl aqueous electrolyte solutions was evaluated using cyclic voltammetry, and the charging mechanism was evaluated using molecular dynamics simulations. KCl aqueous solution provided the highest capacitance compared to LiCl and NaCl aqueous solutions in the case of single-layer graphene electrodes. In contrast, the dependence of the capacitance on the ion species was hardly observed in the case of bilayer graphene. This indicates that Li and Na ions also contributed to the capacitances. The high EDLC performance can be attributed to the fast ion transfer promoted by the dehydration and modification of the second hydration shell on the bilayer graphene because of the relatively strong interaction of ions with the bilayer graphene. Full article
(This article belongs to the Special Issue Advances in Anode and Electrolyte Materials for Lithium-Ion Batteries and Beyond)
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15 pages, 3631 KiB  
Article
Localized High-Concentration Electrolyte (LHCE) for Fast Charging Lithium-Ion Batteries
by Jingru Yang, Xixiu Shi, Wenyang Wang, Zhaoping Liu and Cai Shen
Batteries 2023, 9(3), 155; https://doi.org/10.3390/batteries9030155 - 28 Feb 2023
Cited by 4 | Viewed by 4821
Abstract
The solid electrolyte interphase (SEI) significantly influences the electrochemical performance of lithium-ion batteries. Traditional electrolytes, particularly ether electrolytes, make it challenging to form a stable SEI film, and the corresponding lithium-ion batteries frequently exhibit poor electrochemical performance. In this paper, we develop a [...] Read more.
The solid electrolyte interphase (SEI) significantly influences the electrochemical performance of lithium-ion batteries. Traditional electrolytes, particularly ether electrolytes, make it challenging to form a stable SEI film, and the corresponding lithium-ion batteries frequently exhibit poor electrochemical performance. In this paper, we develop a stable SEI film to improve fast charging and cycle performance using a localized high concentration electrolyte (LHCE). A unique solvation sheath formed by the coordination of Li+, anion, and solvent in the LHCE caused the anion to migrate quickly to the surface of the graphite anode and decompose to form a LiF-rich SEI. A LHCE enabled the Li||C battery to maintain a capacity of 124 mAh g−1 at a rate of 5 C, and the capacity remained at 289 mAh g−1 after 150 cycles at a rate of 0.1 C, with a capacity retention rate of 73% and an average coulomb efficiency of about 99.8%, thus demonstrating excellent long-cycle performance. The LFP||Li battery capacity at a 5 C rate can also be maintained at 102 mAh g−1. Full article
(This article belongs to the Special Issue Advances in Anode and Electrolyte Materials for Lithium-Ion Batteries and Beyond)
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