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Nanomaterials
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Advanced Materials for Lithium (and Post-Lithium) Batteries
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Advanced Materials for Lithium (and Post-Lithium) Batteries

A special issue of Nanomaterials (ISSN 2079-4991). This special issue belongs to the section "Energy and Catalysis".

Deadline for manuscript submissions: closed (20 October 2023) | Viewed by 11199

Special Issue Editor

Dr. Thomas Rüther

E-Mail Website
Guest Editor
Commonwealth Scientific and Industrial Research Organization, Melbourne, Australia
Interests: batteries; electro- and synthetic organometallic chemistry; ionic liquids; ion transport properties

Special Issue Information

Dear Colleagues,

Batteries, amongst other electrical storage technologies, are the crucial link for a rapid transition from CO2-intensive fossil fuels to renewable-based energy generation and consumption. If we are serious about this occurring on a large scale globally, current battery technology needs to be improved in terms of affordability, sustainability, safety, and performance, which includes lifetime, energy density, and power capability. At present, we are in a phase in which the increase in the energy performance of LIBs is approaching a plateau, and hence, new solutions and ideas are absolutely needed. At the core of inventing the batteries of the future lies the discovery of high-performance materials and components that enable the creation of batteries with higher energy and power.

Therefore, we invite researchers and innovators from the wider battery community to contribute their original work to this Special Issue in four key domains:

1 Electrode Materials

The discovery and description of new sustainable cathode and anode materials with high energy and/or power performance and high stability against unwanted degradation reactions is essential for the development of future batteries. Disruptive ideas in the area of Li-Sulfur and Li-Air are needed, and contributions towards “post-lithium” are also most welcome. Other aspects that need to be considered here are particle size, active material utilisation, and ion transport in electrodes with high material loadings to achieve high areal current densities.       

2 Material Interfaces

The interfaces between the electrode and electrolyte, where most of the critical battery reactions occur, are still an area surrounded by “mystery”. The advanced experimental characterisation of processes such as solid electrolyte interphase (SEI) formation, cathode–electrolyte interface (CEI) formation, and dendrite formation is needed for their description. This must also encompass studies of the mechanisms of ion transport through interfaces. Contributions relating to new materials facilitating interfaces are equally important.

3 Materials for Safer Operation

Battery safety has become a crucial aspect for manufacturers and their deployment in most applications. Due to repeated incidences of fires and explosions, LIBs are developing a bad reputation amongst end users and regulatory bodies. Furthermore, their “risky nature” requires additional engineering safety controls, which compromise energy density and cost. Therefore, efforts are required in the design of high-performing safe electrolyte systems such as solid-state and ionic-liquid materials.   

4 Experimental Operando Characterisation

Although this domain can be a subset of any of the other three domains, it is listed here separately because the experimental observation of processes occurring in electrode materials and interfaces during cell operation is vital for a deep understanding but, at the same time, a key challenge.

Dr. Thomas Rüther
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. Nanomaterials is an international peer-reviewed open access semimonthly 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 2900 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

  • lithium and Post-Lithium batteries
  • (nano) Materials and Interfaces
  • safer Electrolyte Systems
  • experimental (operando) characterisation and ion transport studies

Published Papers (4 papers)

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Research

18 pages, 7154 KiB  
Article
Effects of Pyrolysis on High-Capacity Si-Based Anode of Lithium Ion Battery with High Coulombic Efficiency and Long Cycling Life
by Yonhua Tzeng, Cheng-Ying Jhan and Yi-Hsuan Wu
Nanomaterials 2022, 12(3), 469; https://0-doi-org.brum.beds.ac.uk/10.3390/nano12030469 - 29 Jan 2022
Cited by 11 | Viewed by 3271
Abstract
We report a facile pyrolysis process for the fabrication of a porous silicon-based anode for lithium-ion battery. Silicon flakes of 100 nm × 800 nm × 800 nm were mixed with equal weight of sodium carboxymethyl cellulose (CMC) and styrene butadiene rubber (SBR) [...] Read more.
We report a facile pyrolysis process for the fabrication of a porous silicon-based anode for lithium-ion battery. Silicon flakes of 100 nm × 800 nm × 800 nm were mixed with equal weight of sodium carboxymethyl cellulose (CMC) and styrene butadiene rubber (SBR) as the binder and the conductivity enhancement additive, Ketjen Black (KB), at the weight ratio of silicon–binder–KB being 70%:20%:10%, respectively. Pyrolysis was carried out at 700 °C in an inert argon environment for one hour. The process converts the binder to graphitic carbon coatings on silicon and a porous carbon structure. The process led to initial coulombic efficiency (ICE) being improved from 67% before pyrolysis to 75% after pyrolysis with the retention of 2.1 mAh/cm2 areal capacity after 100 discharge–charge cycles at 1 A/g rate. The improved ICE and cycling performance are attributed to graphitic coatings, which protect silicon from irreversible reactions with the electrolyte to form compounds such as lithium–silicon–fluoride (Li2SiF6) and the physical integrity and buffer space provided by the porous carbon structure. By eliminating the adverse effects of KB, the anode made with silicon-to-binder weight ratio of 70%:30% exhibited further improvement of the ICE to approximately 90%. This demonstrated that pyrolysis is a facile and promising one-step process for the fabrication of silicon-based anode with high ICE and long cycling life. This is especially true when the amount and choice of conductivity enhancement additive are optimized. Full article
(This article belongs to the Special Issue Advanced Materials for Lithium (and Post-Lithium) Batteries)
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15 pages, 3699 KiB  
Article
Study of the Role of Void and Residual Silicon Dioxide on the Electrochemical Performance of Silicon Nanoparticles Encapsulated by Graphene
by Dimitrios-Panagiotis Argyropoulos, George Zardalidis, Panagiotis Giotakos, Maria Daletou and Filippos Farmakis
Nanomaterials 2021, 11(11), 2864; https://0-doi-org.brum.beds.ac.uk/10.3390/nano11112864 - 27 Oct 2021
Cited by 4 | Viewed by 1841
Abstract
Silicon nanoparticles are used to enhance the anode specific capacity for the lithium-ion cell technology. Due to the mechanical deficiencies of silicon during lithiation and delithiation, one of the many strategies that have been proposed consists of enwrapping the silicon nanoparticles with graphene [...] Read more.
Silicon nanoparticles are used to enhance the anode specific capacity for the lithium-ion cell technology. Due to the mechanical deficiencies of silicon during lithiation and delithiation, one of the many strategies that have been proposed consists of enwrapping the silicon nanoparticles with graphene and creating a void area between them so as to accommodate the large volume changes that occur in the silicon nanoparticle. This work aims to investigate the electrochemical performance and the associated kinetics of the hollow outer shell nanoparticles. To this end, we prepared hollow outer shell silicon nanoparticles (nps) enwrapped with graphene by using thermally grown silicon dioxide as a sacrificial layer, ball milling to enwrap silicon particles with graphene and hydro fluorine (HF) to etch the sacrificial SiO2 layer. In addition, in order to offer a wider vision on the electrochemical behavior of the hollow outer shell Si nps, we also prepared all the possible in-between process stages of nps and corresponding electrodes (i.e., bare Si nps, bare Si nps enwrapped with graphene, Si/SiO2 nps and Si/SiO2 nps enwrapped with graphene). The morphology of all particles revealed the existence of graphene encapsulation, void, and a residual layer of silicon dioxide depending on the process of each nanoparticle. Corresponding electrodes were prepared and studied in half cell configurations by means of galvanostatic cycling, cyclic voltammetry and electrochemical impedance spectroscopy. It was observed that nanoparticles encapsulated with graphene demonstrated high specific capacity but limited cycle life. In contrast, nanoparticles with void and/or SiO2 were able to deliver improved cycle life. It is suggested that the existence of the void and/or residual SiO2 layer limits the formation of rich LiXSi alloys in the core silicon nanoparticle, providing higher mechanical stability during the lithiation and delithiation processes. Full article
(This article belongs to the Special Issue Advanced Materials for Lithium (and Post-Lithium) Batteries)
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16 pages, 2695 KiB  
Article
Fluorinated Boron-Based Anions for Higher Voltage Li Metal Battery Electrolytes
by Jonathan Clarke-Hannaford, Michael Breedon, Thomas Rüther and Michelle J. S. Spencer
Nanomaterials 2021, 11(9), 2391; https://0-doi-org.brum.beds.ac.uk/10.3390/nano11092391 - 14 Sep 2021
Cited by 4 | Viewed by 2841
Abstract
Lithium metal batteries (LMBs) require an electrolyte with high ionic conductivity as well as high thermal and electrochemical stability that can maintain a stable solid electrolyte interphase (SEI) layer on the lithium metal anode surface. The borate anions tetrakis(trifluoromethyl)borate ([B(CF3)4 [...] Read more.
Lithium metal batteries (LMBs) require an electrolyte with high ionic conductivity as well as high thermal and electrochemical stability that can maintain a stable solid electrolyte interphase (SEI) layer on the lithium metal anode surface. The borate anions tetrakis(trifluoromethyl)borate ([B(CF3)4]−), pentafluoroethyltrifluoroborate ([(C2F5)BF3]−), and pentafluoroethyldifluorocyanoborate ([(C2F5)BF2(CN)]−) have shown excellent physicochemical properties and electrochemical stability windows; however, the suitability of these anions as high-voltage LMB electrolytes components that can stabilise the Li anode is yet to be determined. In this work, density functional theory calculations show high reductive stability limits and low anion–cation interaction strengths for Li[B(CF3)4], Li[(C2F5)BF3], and Li[(C2F5)BF2(CN)] that surpass popular sulfonamide salts. Specifically, Li[B(CF3)4] has a calculated oxidative stability limit of 7.12 V vs. Li+/Li0 which is significantly higher than the other borate and sulfonamide salts (≤6.41 V vs. Li+/Li0). Using ab initio molecular dynamics simulations, this study is the first to show that these borate anions can form an advantageous LiF-rich SEI layer on the Li anode at room (298 K) and elevated (358 K) temperatures. The interaction of the borate anions, particularly [B(CF3)4]−, with the Li+ and Li anode, suggests they are suitable inclusions in high-voltage LMB electrolytes that can stabilise the Li anode surface and provide enhanced ionic conductivity. Full article
(This article belongs to the Special Issue Advanced Materials for Lithium (and Post-Lithium) Batteries)
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11 pages, 3261 KiB  
Article
Stabilization of Li0.33La0.55TiO3 Solid Electrolyte Interphase Layer and Enhancement of Cycling Performance of LiNi0.5Co0.3Mn0.2O2 Battery Cathode with Buffer Layer
by Feihu Tan, Hua An, Ning Li, Jun Du and Zhengchun Peng
Nanomaterials 2021, 11(4), 989; https://0-doi-org.brum.beds.ac.uk/10.3390/nano11040989 - 12 Apr 2021
Cited by 5 | Viewed by 2468
Abstract
All-solid-state batteries (ASSBs) are attractive for energy storage, mainly because introducing solid-state electrolytes significantly improves the battery performance in terms of safety, energy density, process compatibility, etc., compared with liquid electrolytes. However, the ionic conductivity of the solid-state electrolyte and the interface between [...] Read more.
All-solid-state batteries (ASSBs) are attractive for energy storage, mainly because introducing solid-state electrolytes significantly improves the battery performance in terms of safety, energy density, process compatibility, etc., compared with liquid electrolytes. However, the ionic conductivity of the solid-state electrolyte and the interface between the electrolyte and the electrode are two key factors that limit the performance of ASSBs. In this work, we investigated the structure of a Li0.33La0.55TiO3 (LLTO) thin-film solid electrolyte and the influence of different interfaces between LLTO electrolytes and electrodes on battery performance. The maximum ionic conductivity of the LLTO was 7.78 × 10−5 S/cm. Introducing a buffer layer could drastically improve the battery charging and discharging performance and cycle stability. Amorphous SiO2 allowed good physical contact with the electrode and the electrolyte, reduced the interface resistance, and improved the rate characteristics of the battery. The battery with the optimized interface could achieve 30C current output, and its capacity was 27.7% of the initial state after 1000 cycles. We achieved excellent performance and high stability by applying the dense amorphous SiO2 buffer layer, which indicates a promising strategy for the development of ASSBs. Full article
(This article belongs to the Special Issue Advanced Materials for Lithium (and Post-Lithium) Batteries)
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