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Challenges with the Ultimate Energy Density with Li-ion Batteries

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Challenges with the energy density with Li-ion batteries are reviewed. At present, Li-ion batteries are widely used in electronic equipment and electric vehicles, but the energy density is not high. It is important to find out the limitations of the energy density with Li-ion batteries. This essay will start the research with the structure of Li-ion batteries, study the chemistry behind Li-ion batteries and give a summary of the limitations of each battery part which affect energy density. In conclusion, it is the chemistry behind batteries that limits the energy density.
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Challenges with the Ultimate Energy Density with Li-ion Batteries
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5th International Symposium on Resource Exploration and Environmental Science
IOP Conf. Series: Earth and Environmental Science 781 (2021) 042023
IOP Publishing
doi:10.1088/1755-1315/781/4/042023
1
Challenges with the Ultimate Energy Density with Li-ion
Batteries
Haoyu Fang*
School of Energy Power and Mechanical Engineering, North China Electricity Power
University, Baoding, China
*Corresponding author: 201804000304@ncepu.edu.cn
Abstract. Challenges with the energy density with Li-ion batteries are reviewed. At
present, Li-ion batteries are widely used in electronic equipment and electric vehicles,
but the energy density is not high. It is important to find out the limitations of the
energy density with Li-ion batteries. This essay will start the research with the
structure of Li-ion batteries, study the chemistry behind Li-ion batteries and give a
summary of the limitations of each battery part which affect energy density. In
conclusion, it is the chemistry behind batteries that limits the energy density.
Keywords: Challenges; Li-ion batteries; energy density; chemistry; limitations.
1. Induction
Today, the development of Li-ion batteries is limited by the energy density. Compared with the speed
of industrial scale expansion, although the energy density of Li-ion batteries is increasing steadily per
year, it is still too slow.
According to the Figure 1, the mass energy density (specific energy) of some substances is as
follows: liquid hydrogen: 141.6MJ/kg, gasoline: 46.4MJ/kg, diesel: 44.8MJ/kg, lithium: 43MJ/kg,
lithium-ion battery: 0.46-0.72MJ/kg. By comparison, it is evident that there is only a small difference
in mass energy density among gasoline, diesel and lithium but a big gap between lithium and lithium-
ion batteries. It is very useful and interesting to find out what happened from lithium to lithium-ion
batteries and the limitations of the ultimate energy density with Li-ion batteries so that we can solve
the problem accordingly.
An overview of the Li-ion battery and its limitations with energy density was given [2,3]. For the
electrolyte and separator, it is difficult to get rid of them. The basic reasons will be described in the
main body. For electrode materials, some challenges are listed and explained, such as the formation of
lithium dendrite and lithium extraction&insertion [4-6]. Electrode materials can not use lithium only
or add lithium simply.
On the basis of information above, the challenges with the energy density with Li-ion batteries will
be summarized from the working principle, chemical reactions and the inner structure.
5th International Symposium on Resource Exploration and Environmental Science
IOP Conf. Series: Earth and Environmental Science 781 (2021) 042023
IOP Publishing
doi:10.1088/1755-1315/781/4/042023
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Figure 1. Energy density and specific energy chart of some substances [1]
2. Method
To find out the limitations of the energy density with Li-ion batteries, the research starts with the
structure of Li-ion batteries. Then, I study the chemical process and summarize the reasons for energy
density with batteries by literature research and qualitative analysis.
3. Results & Discussion
3.1. Basic structure and working principle of Li-ion batteries
Figure 2. Basic structure of a lithium-ion battery [2]
5th International Symposium on Resource Exploration and Environmental Science
IOP Conf. Series: Earth and Environmental Science 781 (2021) 042023
IOP Publishing
doi:10.1088/1755-1315/781/4/042023
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Figure 3. Charging-discharge process of a lithium-ion battery [3]
A Li-ion battery (figure 2) is mainly composed of electrolyte, anode, cathode and separator. Figure
3 shows the charging and discharging progress of a Li-ion battery. During charging, lithium ions are
removed from the active material of the positive electrode (cathode), transferred from the electrolyte to
the negative electrode (anode) by external voltage, and embedded in the active material of the negative
electrode (anode). At the same time, the electrons flow from the positive electrode (cathode) to the
negative electrode (anode) through the external circuit. The battery is in the high energy state with the
negative electrode (anode) rich in lithium and the positive electrode (cathode) poor in lithium, which
realizes the conversion from electric energy to chemical energy. During discharging, the lithium ions
are removed from the negative electrode and migrated to the positive electrode and embedded in the
lattice. Simultaneously, the electrons flow from the negative electrode to the positive electrode
through the external circuit to form the current, which realizes the conversion from chemical energy to
electric energy [3].
4. Limitations of each part
In fact, there is not so much lithium in a Li-ion batteries because there are some limitations. And
lithium can not be simply added into a Li-ion battery to increase its energy density.
4.1. Electrolyte and separator
Electrolyte, which is generally made of high-purity organic solvent, electrolyte lithium salt and some
necessary additives, plays an important role as the carrier of the ion transport in the battery between
the two electrodes. However, too much electrolyte is a dead weight, resulting in a lower energy
density and unnecessarily increases the costs of the battery [7].
The separator separates the anode from the cathode, which prevents the short circuit caused by the
direct contact of electrodes and serves as the medium for the lithium ions in the electrolyte to pass free
between electrodes. A good separator is supposed to have: chemical stability (no reaction with
electrolyte and electrode materials), wettability (easy to permeate through electrolyte without
elongation and contraction), thermal stability (high temperature resistant and isolation performance),
mechanical strength (not easily punctured), ionic conductivity (high porosity)[3]. It affects the
chemical and safety properties of the battery.
Batteries need the electrolyte and separator to transfer lithium ions in order within the requirements.
Therefore, batteries can’t get rid of them, although they add extra weight and reduce the energy
density. Scientists are searching for the lighter electrolyte and the thinner separator.
4.2. Electrode materials
The problem with Li-ion batteries is that none of the existing electrode materials alone can deliver all
the required performance characteristics including high capacity, higher operating voltage, and long
cycle life [8].
5th International Symposium on Resource Exploration and Environmental Science
IOP Conf. Series: Earth and Environmental Science 781 (2021) 042023
IOP Publishing
doi:10.1088/1755-1315/781/4/042023
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4.2.1. Anode materials. For higher energy density with batteries, in the case of the same volume, a
good material of the anode should be as small and light as possible, and a molecule can release lots of
electrons.
As it is mentioned, we hope to transfer lithium ions through the electrolyte and separator in order
because it’s very important to maintain the stable chemical reaction. But there is no guarantee that
lithium ions will be evenly distributed on the anode surface during charging because lithium ions are
always disobedient without constraints. The lithium ions that arrive earlier are attached to the anode.
Then the subsequent lithium ions are attached to the earlier. Gradually, lithium dendrites are formed.
Figure 4. Schematic Summary of the Lithium Growth Mechanisms and Interactions with the
Nanoporous Ceramic Separator [6]
From figure 4, the growth of lithium dendrites depends on the applied current density. Under
different current densities, lithium grows in different modes and forms different shapes. When the
current density is too high, the dendrites will grow wildly [6]. They are thin spikes growing from the
anode, which will pierce through the SEI layer and even probably cause a short circuit. So we need to
dig some holes for lithium ions to jump in to prevent the phenomenon. Graphite is such a porous
material with sheet structure to hold lithium atoms. Therefore, it is widely used as anode materials
today. Besides, it is very necessary to reduce the current density and build a high strength protective
layer on the anode surface [6]. The problem is solved, but the energy density is diluted. Besides
graphite, silicon is also a good material with a much higher capacity than carbon. But it also has a
volume effect. Silicon placed in a battery swells as it absorbs positively charged lithium atoms during
charging, then shrinks during use as the lithium ion is drawn out of the silicon. This cycle typically
causes the silicon to pulverize, degrading the performance of the battery [8].
4.2.2. Cathode materials. At present, cathode materials are mainly LiCoO2, LiNiO2, LiMnO2,
LiFePO4, Li(NiCoMn)O2[3]. Among them, only about half of lithium ions can be reversible and
participate in the extraction and insertion during the charge-discharge process of LiCoO2 [5].
5th International Symposium on Resource Exploration and Environmental Science
IOP Conf. Series: Earth and Environmental Science 781 (2021) 042023
IOP Publishing
doi:10.1088/1755-1315/781/4/042023
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Figure 5. Structural changes of cathode materials during charging and discharging [5]
From figure 5, if lithium ions are excessively extracted from the cathode, the stability and cycle
performance of the structure will decrease. Some lithium ions are needed to maintain the structure.
Accordingly, the storage capacity of cathode material of lithium-ion batteries is far lower than that of
anode material, so the energy density with Li-ion batteries is mainly limited by the cathode material.
There are two ways to increase the energy density of cathode materials, one is to increase the specific
capacity of cathode materials, the other is to increase the lithium extraction-insertion potential [4].
The extraction or insertion of lithium ion is usually a single electron reaction during charging and
discharging. Multi-electron transfer reaction materials are considered to increase the energy density,
such as Li3V2 (PO4)3, Li2FeO4 and Li2FeSiO4 [9-11].
To increase the working potential of materials, among common transition metal, Ni4+/Ni3+、
Co3+/Co2+ with high redox potential are often considered(Figure 6). A research shows that Ni doping
can not only effectively improve the voltage plateau of LiMn2O4 material, but also significantly
reduce the concentration of Mn3 +, slow down the dissolution of Mn, effectively improve the
structural stability of the material, so as to improve the cycling performance of the material [12].
Figure 6. Redox potential of different transition metal [4]
Lithium-rich materials are also a kind of cathode materials with high energy density recently,
which have the advantages of high theoretical capacity, high working voltage and low cost. To
improve the cycle performance, he most effective structural design method is nano-coating ZrO2,
TiO2, Al2O3. Experiment results show that by coating a suitable inorganic nano-layer on the surface
the side reaction between electrode materials and electrolyte can be inhibited and the structural and
thermal stability of electrode materials can be improved [13-14].
5. Conclusion
The challenges of energy density with Li-ion batteries have been summed up above. These are always
relevant to the chemical process in the batteries. The electrolyte and separator are essential as the
passageway of lithium ions. The electrodes need a big storage capacity for charging and discharging
repeatedly leading to some extra weight and volume inevitably. For the orderly lithium ions transport,
for the orderly distribution of lithium ions and atoms, for the orderly chemical reaction, Li-ion
batteries need various accessory materials, which usually are at the cost of energy density though.
5th International Symposium on Resource Exploration and Environmental Science
IOP Conf. Series: Earth and Environmental Science 781 (2021) 042023
IOP Publishing
doi:10.1088/1755-1315/781/4/042023
6
Therefore, from lithium to lithium-ion batteries, energy density is sacrificed. However, after knowing
the challenges, there is a long way to go. The current situation of energy density with batteries is not
optimistic. The perfect electrode materials have not been found yet. New types of lithium-ion batteries
still need to be studied further. But there are always some new directions and methods along with the
development of chemistry, materials and nanotechnology. The potential of Li-ion batteries is unlimited.
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Article
  • Oct 2008
Recently, there have been many reports on efforts to improve the rate capability and discharge capacity of lithium secondary batteries in order to facilitate their use for hybrid electric vehicles and electric power tools. In the present work, we present a ZrO2-coated Li[Li1/6Mn1/2Co1/6Ni1/6]O2. The bare Li[Li1/6Mn1/2Co1/6Ni1/6]O2 shows a high initial discharge capacity of 224 mAh g−1 at a 0.2 C rate. Owing to the stability of ZrO2, it was possible to enhance the rate capability and cyclability. After 1 wt% ZrO2 coating, the ZrO2-coated Li[Li1/6Mn1/2Co1/6Ni1/6]O2 showed a high discharge capacity of 115 mAh g−1 after 50 cycles under a 6 C rate, whereas the bare Li[Li1/6Mn1/2Co1/6Ni1/6]O2 showed a discharge capacity of only 40 mAh g−1 and very poor cyclability under the same conditions. Based on results of XRD and EIS measurements, it was found that the ZrO2 suppressed impedance growth at the interface between the electrodes and electrolyte and prevented collapse of the layered hexagonal structure.
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The effects of TiO2 coating on the electrochemical performance of Li[Li0.2Mn0.54Ni0.13Co0.13]O2 cathode material for lithium-ion battery
Article
  • Sep 2008
  • SOLID STATE IONICS
TiO2-coated Li[Li0.2Mn0.54Ni0.13Co0.13]O2 materials have been synthesized and investigated as cathode materials for lithium-ion batteries at both 25 °C and elevated temperature (55 °C). The structure and morphology of the coated samples were characterized and compared. The XRD results indicate that lattice parameters of the materials did not change distinctly after surface coating. The SEM images demonstrate that the surface of Li[Li0.2Mn0.54Ni0.13Co0.13]O2 samples were covered with nano-sized TiO2 particles. Differential scanning calorimetry (DSC) analysis results show that thermal stability of the materials was improved. It is also shown that the irreversible capacity loss of the materials was obviously reduced and their capacity retention behaviour was improved after surface modification.
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Electrochemical Performance of Li2FeSiO4 as New Li-Battery Cathode Material
Article
  • Feb 2005
  • ELECTROCHEM COMMUN
Phase-pure lithium iron silicate (Li2FeSiO4) has been prepared successfully. Its ambient temperature structure has been determined by X-ray diffraction and its electrochemical performance characterised at 60 °C. The resulting cyclic voltammogram suggests a phase transition to a more stable structure after the first cycle. This could involve a structural ordering process from a solid-solution to a long-range-ordered structure. The initial charge capacity of 165 mAh/g (99% of the theoretical value) stabilises after a few cycles to around 140 mAh/g (84% of the theoretical value).
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Analysis of the chemical diffusion coefficient of lithium ions in Li3V2(PO4)3 cathode material
Article
  • Feb 2010
  • ELECTROCHIM ACTA
The chemical diffusion coefficients of lithium ions (DLi+) in Li3V2(PO4)3 between 3.0 and 4.8 V are systematically determined by cyclic voltammetry (CV), electrochemical impedance spectroscopy (EIS) and galvanostatic intermittent titration technique (GITT). The DLi+ values are found to be dependent on the voltage state of charge and discharge. Based on the results from all the three techniques, the true diffusion coefficients measured in single-phase region are in the range of 10−9 to 10−10 cm2 s−1. Its apparent diffusion coefficients measured in two-phase regions by CV and GITT range from 10−10 to 10−11 cm2 s−1 and 10−8 to 10−13 cm2 s−1, respectively, depending on the potentials. By the GITT, the DLi+ varies non-linearly in a “W” shape with the charge–discharge voltage, which is ascribed to the strong interactions of Li+ with surrounding ions. Finally, the chemical diffusion coefficients of lithium ions measured by CV, EIS and GITT are compared to each other.
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Study of LiNi0.5Mn1.5O4 synthesized via a chloride-ammonia co-precipitation method: Electrochemical performance, diffusion coefficient and capacity loss mechanism
Article
  • Dec 2009
  • ELECTROCHIM ACTA
LiNi0.5Mn1.5O4 powders are prepared via a new co-precipitation method. In this method, chloride salts are used as precursors and ammonia as a precipitator. The impurity of chlorine can be removed via a thermal decomposition of NH4Cl in the subsequent calcination. X-ray diffraction pattern reveals that the final product is a pure spinel phase of LiNi0.5Mn1.5O4. Scanning electron microscopy shows that the powders have an octahedron shape with a particle size of about 2 μm. Electrochemical test shows that the LiNi0.5Mn1.5O4 powders exhibit an excellent cycling performance and after 300 cycles, the capacity retention is 83%. The lithium diffusion coefficient is measured to be 5.94 × 10−11 cm2 s−1 at 4.1 V, 4.35 × 10−10 cm2 s−1 at 4.75 V and 7.0 × 10−10 cm2 s−1 at 4.86 V. The mechanism of capacity loss is also explored. After 300 cycles, the cell parameter ‘a’ decreases by 0.54% for the quenched sample (LiNi0.5Mn1.5O4−δ) and by 0.42% for the annealed sample (LiNi0.5Mn1.5O4). Besides, it is the first time to identify experimentally that the Ni and Mn ions dissolved in the electrolyte can be further deposited on the surface of anode.
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Current Situation and Prospect of Lithium Ion Battery [J]
  • Jan 2017
  • 283
  • Wang