batteries

Editorial
Lithium-Ion Batteries: Latest Advances and Prospects
Mohammad Rahimi

Department of Chemical Engineering, Massachusetts Institute of Technology, Cambridge, MA 02139, USA;

[email protected]

The anthropogenic release of greenhouse gases, especially carbon dioxide (CO2 ),

has resulted in a notable climate change and an increase in global average temperature
since the mid-20th century [1,2]. To arrive at the margin of a 2 ◦ C global temperature
rise, it is essential to design and execute a multiscale comprehensive action plan to effec-
tively mitigate climate change before its impacts overwhelm our ability to manage the
situation [3–5]. Electrochemistry is a powerful tool for designing diverse CO2 mitigation
approaches that can effectively help prevent dangerous anthropogenic interference with the
climate system. Several implementations of electrochemical systems are being considered
within the electrochemistry and climate change framework. Besides emerging tasks such
as CO2 capture [6–8] and conversion [9–11], electrochemical systems are mainly being
developed to help integrate renewable energy into electricity systems, through developing
electrochemical energy storage systems such as batteries. Batteries are currently being
developed to power an increasingly wide range of applications, including electrification
of transportation [12,13] and grid-scale energy storage [14,15]. Large-scale developments
and implementations of batteries offer sustainable energy supply based on renewables,
which is a major step toward reducing CO2 emissions associated with the energy sector
and ultimately assisting in climate change mitigation.



Among the developed batteries, lithium-ion batteries (LIBs) have received the most


attention, and have become increasingly important in recent years. Compared with other
Citation: Rahimi, M. Lithium-Ion
batteries, LIBs offer high energy density, high discharge power, high coulombic efficiencies,
Batteries: Latest Advances and
and long service life [16–18]. These characteristics have facilitated a remarkable advance
Prospects. Batteries 2021, 7, 8.
of LIBs in many frontiers, including electric vehicles, portable and flexible electronics, and
https://doi.org/10.3390/batteries
stationary applications. Since the field of LIBs is advancing rapidly and attracting an increasing
7010008
number of researchers, it is necessary to often provide the community with the latest updates.
Therefore, this Special Issue was designed to focus on updating the electrochemical community
Received: 15 January 2021
Accepted: 19 January 2021
with the latest advances and prospects on various aspects of LIBs. Researchers were invited
Published: 20 January 2021
to submit their original research as well as review/perspective articles for publication in the
Special Issue “Lithium-Ion Batteries: Latest Advances and Prospects”.
Publisher’s Note: MDPI stays neutral
In response to this call, twelve research papers [19–30] and one case report [31]
with regard to jurisdictional claims in
were thoroughly peer-reviewed and published. The published research papers covered
published maps and institutional affil- advances in several fronts of the technology, including detailed fundamental studies of
iations. the electrochemical cell and investigations to better improve parameters related to battery
packs. In the domain of fundamental studies, various components of the electrochemical
cell, including electrodes and electrolyte, were investigated. In this context, a lightweight
dense polymer–carbon composite-based current collector foil for applications in LIB was
Copyright: © 2021 by the author.
developed and evaluated in comparison to the state-of-the-art aluminum foil collector [19].
Licensee MDPI, Basel, Switzerland.
It was found that the resistance of the developed electrode based on this current collector to
This article is an open access article
be by a factor of five lower compared to the aluminum-based collector, which was attributed
distributed under the terms and to the low contact resistance between the proposed current collector and the other elements
conditions of the Creative Commons of the electrode. In addition, due to a 50% lower material density, the developed lightweight
Attribution (CC BY) license (https:// current collector offers the possibility to significantly decrease the mass loading of the
creativecommons.org/licenses/by/ electrode, which can be of special interest for bipolar battery architectures. In another
4.0/). study [20], the lithium intercalation dynamics in a cathode electrode with particles of

Batteries 2021, 7, 8. https://doi.org/10.3390/batteries7010008 https://www.mdpi.com/journal/batteries

Batteries 2021, 7, 8 2 of 4

distributed size was studied using the phase-field model, aiming to better understand the
effect of this particle size distribution on the LIBs’ dynamic performance.
To advance the electrolyte-related research, a first principle-based modeling framework
was developed to identify the physical manifestation that electrolyte degradation has on
the battery and the response observed in the terminal voltage [21]. The developed frame-
work relates the different kinds of side reactions in the electrolyte to the material properties
affected due to these side reactions—these material property changes directly impact the
electrochemical reactions, and ultimately the voltage across the terminals of the battery.
Internal resistance is one of the important parameters in LIBs, which requires develop-
ing precise experimental procedures and/or theoretical frameworks to accurately evaluate
this parameter. In this context, two different methods were investigated in the research
paper published in this Special Issue: electrochemical impedance spectroscopy (EIS) and
parameter estimation based on equivalent circuit model (ECM) [22]. It was found that
unlike the conventional parameter estimation method that yields a different value than
EIS, internal resistances estimated based on ECM match the values obtained from EIS.
The proposed methods will be supplementary in tracking the internal resistance properly
which can improve the accuracy of battery performance prediction.
An experimental investigation was performed to evaluate the effect of the current rate
and prior cycling on the coulombic efficiency of LIBs [23]. The determination of coulombic
efficiency of LIBs can contribute to comprehend better their degradation behavior. There-
fore, a detailed understanding of the effect of these parameters would be beneficial to
further optimize the cell charge/discharge procedures.
Experiments were performed at high temperatures to provide better insights regarding
battery performance at elevated temperatures. In this context, advanced in-operando
measurement techniques such as fast impedance spectroscopy and ultrasonic waves as well
as strain-gauges were employed to evaluate the cell performance at these temperatures [24].
These methods have the potential to be integrated into the battery management system
in the future, making it possible to achieve higher battery safety even under the most
demanding operating conditions. In addition, comprehensive hazard analysis of failing
LIBs used in electric vehicles was evaluated experimentally at elevated temperatures [25].
In this investigation, several hazard-relevant parameters were quantified, including the
temperature response of the cell, the maximum reached cell surface temperature, the
amount of produced vent gas, the gas venting rate, the composition of the produced gases,
and the size and composition of the produced particles. The results are valuable for all
who deal with batteries, including firefighters, battery pack designers, and cell recyclers.
The effect of cell manufacturing parameters was also investigated on the performance
of the produced LIBs. For example, a theoretical framework was developed to highlight
the considerable impact of electrode porosity, electrode internal void volume, cell capacity,
and capacity ratio that result from electrode coating and calendering tolerance (as the
manufacturing parameters) on the cell-to-cell and lot-to-lot performance variation [26]. In
another study published in this Special Issue, the impact of manufacturing parameters
in laser cutting, which is a promising technology for the singulation of conventional and
advanced electrodes for LIBs, was investigated [27]. In specifics, it was shown how cutting
edge characteristics affect electrochemical performance. These types of information would
be beneficial to manufacture better LIBs.
In addition to improving individual LIB cells, several researches were focused on
strategies to obtain better battery packs. Every single cell in the battery pack needs a contact
for its cell terminals, which raises the necessity of an automated contacting process with low
joint resistances to reduce the energy loss in the cell transitions. A capable joining process
suitable for highly electrically conductive materials like copper or aluminum is laser beam
welding. In the research paper published in this Special Issue, a theoretical examination of
the joint resistance and a simulation of the current flow dependent on the contacting weld’s
position in an overlap configuration was performed [28]. This investigation highlighted
the influence of the shape and position of the weld seams as well as the laser welding
Batteries 2021, 7, 8 3 of 4

parameters, and how these parameters can be leveraged to further reduce the cell-to-cell
joint resistances.
For LIB packs, it is necessary to understand how to best replace poorly performing
cells to extend the lifetime of the entire battery pack. In a comprehensive investigation [29],
cell replacement strategies were studied considering two scenarios: early life failure, where
one cell in a pack fails prematurely, and building a pack from used cells for less demanding
applications. Early life failure replacement found that a new cell can perform adequately
within a pack of moderately aged cells. The second scenario for the reuse of lithium-ion
battery packs examines the problem of assembling a pack for less-demanding applications
from a set of aged cells, which exhibit more variation in capacity and impedance than their
new counterparts. The cells used in the aging comparison part of the study were deeply
discharged, recovered, assembled in a new pack, and cycled. The criteria for selecting the
aged cells for building a secondary pack were discussed in the paper and the performance
and coulombic efficiency of the secondary pack were compared to the pack built from new
cells and the repaired pack. The results showed that the pack that employed aged cells
performed well, but its efficiency was reduced.
The cooling system of LIB packs used in electric vehicles was also investigated in
the Special Issue. Thermal management systems of LIBs play an important role as the
performance and lifespan of the batteries are affected by the temperature. A detailed study
published in this Special Issue proposed a framework to establish equivalent circuit models
that can reproduce the multi-physics phenomenon of Li-ion battery packs, which includes
liquid cooling systems with a unified method. The developed equivalent circuit models
were found to be very accurate and computationally cost-effective [30].
Besides the detailed research papers, one case report on the future portable LIB recy-
cling challenges in Poland was published in this Special Issue [31]. This case report presents
the market of portable LIBs in the European Union (EU) with particular emphasis on the
stream of used cells in Poland by 2030. The report also draws attention to the fact that,
despite a decade of efforts in Poland, it has not been possible to create an effective manage-
ment system for waste batteries and accumulators that would include waste management,
waste disposal, and component recovery technology for reuse. This report highlights the
critical role of recycling strategies and challenges that need to be investigated to effectively
deal with used LIBs.

Funding: This research received no external funding.

Acknowledgments: At the end of this editorial, I would like to express my sincere gratitude to the
authors for their valuable contributions, and the reviewers for their efforts in analyzing the relevance
and quality of the papers that were submitted to this special issue. I would also like to thank the
editorial staff of Batteries for their help and support during the review process.
Conflicts of Interest: The author declares no conflict of interest.

References
1. Rogelj, J.; Huppmann, D.; Krey, V.; Riahi, K.; Clarke, L.; Gidden, M.; Nicholls, Z.; Meinshausen, M. A new scenario logic for the
Paris Agreement long-term temperature goal. Nature 2019, 573, 357–363. [CrossRef] [PubMed]
2. Luderer, G.; Vrontisi, Z.; Bertram, C.; Edelenbosch, O.Y.; Pietzcker, R.C.; Rogelj, J.; De Boer, H.S.; Drouet, L.; Emmerling, J.; Fricko,
O. Residual fossil CO2 emissions in 1.5–2 C pathways. Nat. Clim. Chang. 2018, 8, 626–633. [CrossRef]
3. O’Neill, B.C.; Carter, T.R.; Ebi, K.; Harrison, P.A.; Kemp-Benedict, E.; Kok, K.; Kriegler, E.; Preston, B.L.; Riahi, K.; Sillmann, J.
Achievements and needs for the climate change scenario framework. Nat. Clim. Chang. 2020, 10, 1–11. [CrossRef] [PubMed]
4. Fawzy, S.; Osman, A.I.; Doran, J.; Rooney, D.W. Strategies for mitigation of climate change: A review. Environ. Chem. Lett. 2020,
18, 1–26. [CrossRef]
5. Rahimi, M. Public Awareness: What Climate Change Scientists Should Consider. Sustainability 2020, 12, 8369. [CrossRef]
6. Rahimi, M.; Catalini, G.; Hariharan, S.; Wang, M.; Puccini, M.; Hatton, T.A. Carbon Dioxide Capture Using an Electrochemically
Driven Proton Concentration Process. Cell Rep. Phys. Sci. 2020, 1, 100033. [CrossRef]
7. Rahimi, M.; Diederichsen, K.M.; Ozbek, N.; Wang, M.; Choi, W.; Hatton, T.A. An Electrochemically Mediated Amine Regeneration
Process with a Mixed Absorbent for Postcombustion CO2 Capture. Environ. Sci. Technol. 2020, 54, 8999–9007. [CrossRef]
Batteries 2021, 7, 8 4 of 4

8. Rahimi, M.; Zucchelli, F.; Puccini, M.; Hatton, T.A. Improved CO2 Capture Performance of Electrochemically Mediated Amine
Regeneration Processes with Ionic Surfactant Additives. ACS Appl. Energy Mater. 2020, 3, 10823–10830. [CrossRef]
9. Zheng, Y.; Vasileff, A.; Zhou, X.; Jiao, Y.; Jaroniec, M.; Qiao, S.-Z. Understanding the roadmap for electrochemical reduction of
CO2 to multi-carbon oxygenates and hydrocarbons on copper-based catalysts. J. Am. Chem. Soci. 2019, 141, 7646–7659. [CrossRef]
10. Lee, G.; Li, Y.C.; Kim, J.-Y.; Peng, T.; Nam, D.-H.; Rasouli, A.S.; Li, F.; Luo, M.; Ip, A.H.; Joo, Y.-C. Electrochemical upgrade of CO2
from amine capture solution. Nat. Energy 2020, 6, 46–53.
11. Sun, Z.; Ma, T.; Tao, H.; Fan, Q.; Han, B. Fundamentals and challenges of electrochemical CO2 reduction using two-dimensional
materials. Chem 2017, 3, 560–587. [CrossRef]
12. Cano, Z.P.; Banham, D.; Ye, S.; Hintennach, A.; Lu, J.; Fowler, M.; Chen, Z. Batteries and fuel cells for emerging electric vehicle
markets. Nat. Energy 2018, 3, 279–289. [CrossRef]
13. Harper, G.; Sommerville, R.; Kendrick, E.; Driscoll, L.; Slater, P.; Stolkin, R.; Walton, A.; Christensen, P.; Heidrich, O.; Lambert, S.
Recycling lithium-ion batteries from electric vehicles. Nature 2019, 575, 75–86. [CrossRef] [PubMed]
14. Posada, J.O.G.; Rennie, A.J.; Villar, S.P.; Martins, V.L.; Marinaccio, J.; Barnes, A.; Glover, C.F.; Worsley, D.A.; Hall, P.J. Aqueous
batteries as grid scale energy storage solutions. Renew. Sustain. Energy Rev. 2017, 68, 1174–1182. [CrossRef]
15. Jiang, L.; Lu, Y.; Zhao, C.; Liu, L.; Zhang, J.; Zhang, Q.; Shen, X.; Zhao, J.; Yu, X.; Li, H. Building aqueous K-ion batteries for energy
storage. Nat. Energy 2019, 4, 495–503. [CrossRef]
16. Manthiram, A.; Yu, X.; Wang, S. Lithium battery chemistries enabled by solid-state electrolytes. Nat. Rev. Mater. 2017, 2, 1–16.
[CrossRef]
17. Manthiram, A. A reflection on lithium-ion battery cathode chemistry. Nat. Commun. 2020, 11, 1–9. [CrossRef]
18. Xiao, J.; Li, Q.; Bi, Y.; Cai, M.; Dunn, B.; Glossmann, T.; Liu, J.; Osaka, T.; Sugiura, R.; Wu, B. Understanding and applying
coulombic efficiency in lithium metal batteries. Nat. Energy 2020, 5, 561–568. [CrossRef]
19. Fritsch, M.; Coeler, M.; Kunz, K.; Krause, B.; Marcinkowski, P.; Pötschke, P.; Wolter, M.; Michaelis, A. Lightweight Polymer-Carbon
Composite Current Collector for Lithium-Ion Batteries. Batteries 2020, 6, 60. [CrossRef]
20. L’vov, P.; Sibatov, R. Effect of the Particle Size Distribution on the Cahn-Hilliard Dynamics in a Cathode of Lithium-Ion Batteries.
Batteries 2020, 6, 29. [CrossRef]
21. Balagopal, B.; Chow, M.-Y. The Physical Manifestation of Side Reactions in the Electrolyte of Lithium-Ion Batteries and Its Impact
on the Terminal Voltage Response. Batteries 2020, 6, 53. [CrossRef]
22. Islam, S.; Park, S.-Y.; Balasingam, B. Unification of Internal Resistance Estimation Methods for Li-Ion Batteries Using Hysteresis-
Free Equivalent Circuit Models. Batteries 2020, 6, 32. [CrossRef]
23. Madani, S.S.; Schaltz, E.; Knudsen Kær, S. Effect of Current Rate and Prior Cycling on the Coulombic Efficiency of a Lithium-Ion
Battery. Batteries 2019, 5, 57. [CrossRef]
24. Zappen, H.; Fuchs, G.; Gitis, A.; Sauer, D.U. In-Operando Impedance Spectroscopy and Ultrasonic Measurements during
High-Temperature Abuse Experiments on Lithium-Ion Batteries. Batteries 2020, 6, 25. [CrossRef]
25. Essl, C.; Golubkov, A.W.; Gasser, E.; Nachtnebel, M.; Zankel, A.; Ewert, E.; Fuchs, A. Comprehensive Hazard Analysis of Failing
Automotive Lithium-Ion Batteries in Overtemperature Experiments. Batteries 2020, 6, 30. [CrossRef]
26. Yourey, W. Theoretical Impact of Manufacturing Tolerance on Lithium-Ion Electrode and Cell Physical Properties. Batteries 2020,
6, 23. [CrossRef]
27. Jansen, T.; Kandula, M.W.; Hartwig, S.; Hoffmann, L.; Haselrieder, W.; Dilger, K. Influence of Laser-Generated Cutting Edges on
the Electrical Performance of Large Lithium-Ion Pouch Cells. Batteries 2019, 5, 73. [CrossRef]
28. Hollatz, S.; Kremer, S.; Ünlübayir, C.; Sauer, D.U.; Olowinsky, A.; Gillner, A. Electrical Modelling and Investigation of Laser Beam
Welded Joints for Lithium-Ion Batteries. Batteries 2020, 6, 24. [CrossRef]
29. Nenadic, N.G.; Trabold, T.A.; Thurston, M.G. Cell Replacement Strategies for Lithium Ion Battery Packs. Batteries 2020, 6, 39.
[CrossRef]
30. Yamanaka, T.; Kihara, D.; Takagishi, Y.; Yamaue, T. Multi-physics equivalent circuit models for a cooling system of a lithium ion
battery pack. Batteries 2020, 6, 44. [CrossRef]
31. Sobianowska-Turek, A.; Urbańska, W. Future Portable Li-Ion Cells’ Recycling Challenges in Poland. Batteries 2019, 5, 75.
[CrossRef]