Perspective

https://doi.org/10.1038/s41560-020-00728-y

Practical assessment of the performance of

aluminium battery technologies
Ehsan Faegh, Benjamin Ng, Dillon Hayman and William E. Mustain    ✉

Aluminium-based battery technologies have been widely regarded as one of the most attractive options to drastically improve,
and possibly replace, existing battery systems—mainly due to the possibility of achieving very high energy density with low
cost. Many reports have demonstrated primary or rechargeable Al-based battery chemistries in both aqueous and non-aqueous
electrolytes. However, the practical realization of these battery chemistries has been difficult over a long period of time (170
years). In fact, no Al-based battery has been shown with the required stability or touted energy density. Typically, the perfor-
mance of Al-based batteries is overstated in the literature due to imprecise considerations that do not fairly evaluate practically
achievable energy densities. Here we provide accurate calculations of the practically achievable cell-level capacity and energy
density for Al-based cells (focusing on recent literature showing ‘high’ performance) and use the results to critically assess
their future deployment.

T
here is an increasing demand for battery-based energy stor-
age in today’s world. Li-ion batteries have become the major
rechargeable battery technology in energy storage systems
due to their outstanding performance and stability. However, their
relatively high cost and safety issues still need to be addressed1,2.
For primary batteries, Zn–MnO2 alkaline cells are by far the most
well-established, though there is a desire to find alternatives with
improved capacity3. Al-based batteries are among the most attrac-
tive alternatives to compete with existing cell chemistries in both
primary (non-rechargeable) and secondary (rechargeable) applica-
tions due to the high natural abundance of Al, its wide availability,
ease in processing (including recycling), low cost and high theo-
retical volumetric (8056 mAh cm–3) and gravimetric (2981 mAh g–1)
capacity. A comparison of some of the most important properties
for metals that are attractive options as energy storage solutions is
provided in Fig. 1a.
Metallic Al has been used as an anode material in all four major
battery categories—aqueous primary and secondary as well as
non-aqueous primary and secondary. The deployment of Al began
in the1850s where it was coupled with a carbon cathode in the Buff
cell4. After that, Al anodes were investigated in different aqueous
media from saline cells to Leclanche-type dry cells5. In 1962, the
concept of the Al–O2/air battery was introduced for the first time
and in 1988 Al–Cl2 rechargeable cells were developed in molten salt
electrolytes6. Though conceptually interesting, many of these cells
showed a propensity towards corrosion and passivation, which led
to a significant amount of research into overcoming such hurdles
in both aqueous and non-aqueous cells. One such solution was the
invention of so-called Al-ion batteries (AIBs) in 20117 and research
in this area over the past several years has mostly focused on under-
standing their reaction mechanisms and searching for suitable
cathodes.
Today, the dominant Al-based primary batteries have been
Al-air batteries (AABs) and the dominant secondary batteries have
been AIBs. For primary battery applications, non-aqueous electro-
lytes are likely not economically feasible due to the high cost of ionic
liquid (IL)-based electrolytes compared to aqueous electrolytes.
Because of this, most AABs utilize a KOH-based aqueous electrolyte.
The vast majority of studies on non-aqueous rechargeable Al batter-
ies have been performed as AIBs, with only a few studies dedicated
to AAB rechargeables, since rechargeable AABs have invariably
shown inferior cycle life and reversibility than AIBs8. In the past few
years, AIBs have received increased attention as a possible solution
for fast charge/discharge applications with ultra-high efficiency and
energy density9.
Many of the studies on AABs or AIBs reported in the literature
end by claiming high energy density materials and/or successful
demonstrations of the technology have been achieved. However,
such claims have invariably failed to consider the comprehensive
implementation of the reported chemistry in practical full cells.
There is a need in the literature for a critical analysis of the realis-
tic deployment of Al anodes across different chemistries. Here we
provide a critical assessment of the electrochemical performances
of state-of-the-art Al batteries reported in the literature. Using all
of the available information about full cell materials and chemistry,
we first carry out an accurate estimation of the practically achiev-
able gravimetric capacity and energy density. This is followed by a
substantive discussion on their expected operational life.
Al–air batteries
The most common AABs typically consist of an Al (pure or alloyed)
anode, air cathode (comprised of a gas diffusion layer and catalyst
layer), and a KOH-based electrolyte that incorporates additives to
suppress corrosion and H2 evolution, such as ZnO (ref. 10) (Fig. 1b).
At the anode, Al metal is oxidized to Al(OH)4–, which subsequently
forms solid Al(OH)3 layers on the electrode surface as the solubility
limit is reached (Eqs. (1) and (2)).
Al þ 4OH� $ AlðOHÞ�
4 þ3e
�
E0 ¼ �2:34 V vs: SHE
ð1Þ
AlðOHÞ� �
4 $ AlðOHÞ3 þOH ð2Þ
At high pH, the passivation film can be dissolved, exposing the
reacting Al, but that also leads to high corrosion rates and H2 gas
evolution (Eqs. (1), (3) and (4))11.

Department of Chemical Engineering, University of South Carolina, Columbia, South Carolina, USA. ✉e-mail: mustainw@mailbox.sc.edu

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Perspective NATure Energy

a Standard potential
(V vs. SHE) Li+ + e– Li Na+ + e– Na K+ + e– K Zn2+ + 2e– Zn Al3+ + 3e– Al
–3.05 V –2.71 V –2.93 V –0.76 V –1.67 V
9000 25

Volumetric capacity (mAh cm–3)

Gravimetric capacity (mAh g–1)
8000
7000 20

Cost (US$ kg–1)

Abundance (%)
6000
15
5000
0.0018
4000
10
3000
2000 0.0075 5
1000
0 0
Li Na K Zn Al
Cation radius (A) 0.76 1.02 0.38 0.74 0.54
Charge density of cations (C mm–3) 52 24 11 112 364

b Al–air battery c Al-ion battery

e– e– e– e–

Discharge Discharge

OH– O2
H2 OH– AlCl4-
(GDL + catalyst layer)

O2

Graphite cathode
Al2Cl7- AlCl4-

(glassy carbon)
OH–
AlCl4-
Air cathode
Al anode

Al anode
OH– AlCl4-
O2
H2 OH– Al2Cl7-

Al(OH)4- O2 AlCl4-
AlCl4-
OH– AlCl4-
OH– O2
Al(OH)3
Al2Cl7-

KOH electrolyte AlCl3–[EMIm]Cl ionic liquid electrolyte

Fig. 1 | Attractive properties and chemistries of Al as an anode material for use in AABs and AIBs. a, Comparison of gravimetric and volumetric
capacities as well as cost, abundance, standard potentials, cation radius and charge density of cations for Li, Na, K, Zn and Al20,50. b, Schematic illustration
of the discharge process in an Al–air battery with aqueous KOH electrolyte showing the movement of hydroxide ions to the anode causing undesired
corrosion and passivation phenomena. c, Schematic of the discharge process in an Al-ion battery with non-aqueous ionic liquid electrolyte including a
representation of intercalated chloroaluminate anions in the graphite cathode.

2H2 O þ 2e� $ H2 þ 2OH�
2Al þ 2OH� þ 6H2 O $ 3H2 þ 2AlðOHÞ�
4 ð4Þ
At the cathode, the oxygen reduction reaction (ORR) occurs
(Eq. (5)).
O2 þ 2H2 O þ 4e� $ 4OH�
Combined, these reactions yield the overall cell reaction in
Eq. (6).
4Al þ 3O2 þ 6H2 O $ 4AlðOHÞ3
Al as an anode in aqueous media has two main problems. First is
the formation of a passivating oxide layer, which reduces the oper-
ating cell voltage and increases both the charge transfer and mass
transfer resistance. As shown theoretically by Nørskov. et al.12, this
causes the open circuit potential of the Al anode to drop from the
Nernstian value of –2.34 V to –1.87 V vs. SHE at pH = 14.6, which
limits the cell operating voltage and practical energy density. The
Eo ¼ �0:83 V vs: SHE ð3Þ theoretical cell voltage of an AAB is 2.74 V, but mainly due to cor-
rosion and the passivating layer, the operating cell voltage has been
shown to be between 1.2 V and 1.6 V. The second problem is a high
rate of corrosion when the oxide layer is removed, especially in alka-
line electrolytes.
Because the cathode reaction utilizes ambient air, there is
only a need to carry one of the reacting species, meaning that they
have the promise to achieve very high energy densities. In fact, the
E0 ¼ 0:40 V vs: SHE ð5Þ maximum theoretical gravimetric capacity of an AAB is second
only to a Li–air battery (Fig. 1a). In the literature, studies focused
on AABs have been quick use the high capacity and theoretical
open-circuit voltage to tout a high theoretical gravimetric energy
density of 4140 Wh kg–113. However, the reported energy densities
E0 ¼ 2:74 V vs: SHE have been much lower than 1000 Wh kg–1 and even these values
ð6Þ have often failed to consider the mass of all of the components
of the cell: anode, cathode, electrolyte, separator and packaging—
meaning that reported values are often not an accurate representa-
tion of what is actually achievable in full cells and true cell-level
discharge capacities and energy densities are reduced significantly
when properly assessed. This is shown in Table 1 using recent
studies utilizing novel chemistries on either the electrodes or the
electrolyte that claim either record discharge capacities or energy
densities.

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 NATure Energy

Table 1 | Comparison of aqueous and non-aqueous primary AABs

Anode/ Electrolyte Battery Reported Reported Average Area Current Al Consumed Cathode Electrolyte Separator Package Total Cell-level Cell-level Battery Ref.
Cathode type discharge energy voltage (cm2) density mass Al mass mass (g) mass (g) mass mass capacity energy operational
capacity density (V)b (mA (g) mass (g) (g) (g) (g) (mAh g–1)c density life (h)d
(mAh g–1)a (Wh kg–1)a cm–2) (Wh kg–1)c
3D printed 2M gelled Aqueous 239 227 0.95 1 0.5 0.011 0.001 - - - - 0.990 2.66 2.52 5.26 14
Al nano- KOH primary
particles/
Pt–C
coated
hydro­
phobic
carbon

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Al foil/ 12 wt% Aqueous 128 77 0.6 4 0.005 0.011 0.003 0.004 0.001 0.001 0.005 0.014 98.50 59.10 69.12 13
carbon NaCl primary
compositee
Al foil/ PBGE Aqueous 900 900 1 1 1 0.004 0.001 0.001 0.040 0.003 0.019 0.065 48.69 48.69 3.15 15
carbon (Paper primary
paperf + SPA +
NaOH)
Al foil/ 5M NaOH Aqueous 1273 1273 1 1 10 0.004 0.001 0.001 0.050 0.004 0.024 0.081 55.17 55.17 0.45 16
carbon primary
paperf
Al/MnO2– 4M NaCl Aqueous 2336 1402 0.6 1 1 0.004 0.003 0.001 0.058 0.005 0.029 0.096 85.46 51.28 58.40 17
CNT air primary
electrode
Al/Porous EMIm(HF) Non- 2102 2300 1.1 1.13 1.5 0.076 0.054 0.049 0.176 0.065 0.147 0.491 326.18 358.80 94.50 48
carbon- 2.3F aqueous
based air primary
electrode
a
Reported values from corresponding study. bEstimated form discharge curves, if not mentioned explicitly in the corresponding study. cCalculated based on Eqs. (10) and (11) in the Methods. dCalculated from charge and load current if not mentioned explicitly in the corresponding
study. eAssumed 0.01 mm thickness for the Al foil and 5% of the total mass for electrolyte. fAssumed 1 mg cm–2 catalyst loading on cathode side.

23
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 Perspective NATure Energy

a packaging)—are considered for these cases, representing the dis-

10,000
charge capacities and energy densities that were actually realized,
AAB theoretical
the values are significantly lower. For many of the studies in Table
1, the achieved values are less than 5% of the reported values. Other
work can fail to consider the additional infrastructure required to
Practical energy density (Wh kg–1)

1,000 support new cell designs. For example, one recent report innova-
AIB theoretical
tively mitigates Al corrosion at open circuit through oil displace-
48 ment. In this case, an accurate estimate of energy density was made
100 True intercalation AIB practical limit 44 38 by the authors (for example, 680 Wh kg–1) for the AAB18 (~6 times
30
32 13 49 33 35
29
42 16
17
lower than the theoretical value); however, the components required
23
27
31 7 41
43
15
to facilitate the continuous flow of electrolyte and the storage and
26 34
25 36 37 handling of the oil were not considered. Of course, these would add
10 28
Aqueous AAB a significant amount of weight (a reasonable estimate could not be
Aqueous AIB made) to the AAB pack, limiting the practical application of this
14 Non-aqueous AAB type of battery. What is hopefully clear from the above discussion
Non-aqueous AIB
1 is that even in the best batteries there remains a huge gap between
1 10 100 1,000 10,000
the theoretical cell-level energy density that is often marketed for
Reported energy density (Wh kg–1) AABs (4140 Wh kg–1) with reported values (77–2300 Wh kg–1) and
b there is another large gap between reported values and what is actu-
1,000
Li-ion
ally practically-achievable or demonstrated (2.52–35880 Wh kg–1)
LiFeS2 as shown in Fig. 2a.
Cell-level energy density (Wh kg–1)

48

100
13
33
16 15 17
7
10
14
1
0 1 10 100
Battery operational life (h)
Fig. 2 | Evaluation of practical energy density and operational lifetime
of Al anode batteries. a, Illustration of reported versus practical energy
density of AABs and AIBs as well as a comparison of achievable versus
theoretical energy density of Al batteries. b, Comparison of cell-level
energy density and estimated battery operational life of state-of-the-art
Al-based batteries with well-established battery technologies. The
numbers indicate the corresponding references.
More specifically, one recent study using a three-dimensional
(3D) printed Al anode prepared by laser sintering14 reported an
achieved capacity of 239 mAh g–1 and a gravimetric energy density
of 227 Wh kg–1. However, in the study, all of the experimental data
was normalized only to the 11 mg of Al that was deposited, and the
mass of the rest of the battery components (that is, current collec-
tors, gelled electrolyte membrane, polyimide sheets as cell packag-
ing, anode substrate and cathode active material) were neglected.
When the total mass of the battery (assuming a generous capacity
ratio of the negative electrode to the positive electrode, N/P, of 1)
is considered, the resulting capacity and cell-level energy density
are much lower, 2.66 mAh g–1 and 2.52 Wh kg–1, respectively. Other
studies utilizing non-liquid electrolytes (gelled or paper based)15–17
have shown relatively low Al corrosion, which is desirable, and
have reported high achievable capacity (900–2336 mAh g–1) and
high energy density (900–1402 Wh kg–1). However, these values
were all based solely on the mass of the Al anode. Furthermore,
in some cases, the operating discharge time was limited—even as
low as 24 minutes—due to premature passivation accompanied by
a significant capacity decay16. When the mass of all of the battery
components — anode and cathode active materials, separator/elec-
trolyte, current collectors (Al foil on the anode side and, typically,
Ag or Cu foil on the cathode side), and battery shells (related to
38
Al-ion batteries
Zn–MnO2
32
42
44
41
35 The most common AIB configuration uses an Al foil anode, a
49
23
43
31 30 29 25
graphite cathode19, and an acidic room temperature non-aqueous
27 26
37
28
Lead–acid IL electrolyte (for example, AlCl3:[EMIm]Cl > 1; [EMIm]Cl is
34 36
1-Ethyl-3-methylimidazolium chloride), as illustrated in Fig. 1c.
Aqueous primary AIBs operate under similar principles as Li-ion batteries, with the
Aqueous secondary main idea that it is possible to intercalate a reacting species inside of
Non-aqueous primary
Non-aqueous secondary the carbon. The main assertion for these cells is that AIBs are able to
1000 10,000 100,000 1000,000
replace the standard one-electron process realized with lithium with
a three-electron process at the anode. However, the reaction is not a
simple dissolution of Al to Al3+ (theoretical capacity of 2980 mAh g–1)
followed by intercalation of Al3+ into the carbon. The redox reaction
in the most common AIBs is much more complicated and involves a
large number of additional reactants from the electrolyte, as shown
in Eq. (7).
Al þ 7AlCl� � �
4 $ 4Al2 Cl7 þ 3e ð7Þ
Therefore, in reality, AIBs require 8 Al atoms per 3 electrons, not
1 Al atom per 3 electrons, which has a huge effect on the theoretical
capacity and energy density of these systems. Considering the total
number of Al atoms (and Cl atoms) that are needed to drive this
reaction, the theoretical capacity of the anode reaction is actually
67 mAh g–1, not the commonly reported 2980 mAh g–1 (Eq. (16)).
AIBs are further limited by a lack of suitable cathode chemistries
(for intercalation or conversion reactions)20. Though it is interesting
from a fundamental perspective to understand how Al intercalates
into carbon, the low capacities that have been reported across the
board for these materials are all caused by the same main drawback:
Al3+ does not participate in noninteractive diffusion in the AlCl3:IL
electrolyte due to its low ionic radii (54 pm) and high valence state21.
This forces Al to coordinate with neighbouring anions (for example,
Cl, F) to form complexes within the room temperature IL. The car-
bon, therefore, intercalates an AlCl4– complex rather than Al3+, as
shown in Eq. (8).
Cn ½AlCl4  þ e� $ Cn þ AlCl�
4 ð8Þ
Such a large intercalating ion introduces structural limita-
tions that force the repeating unit to be very large, estimated to be
8–72 carbons for every intercalated AlCl4– anion22 (unlike LiC6 in
Li-ion batteries). Therefore, the gravimetric energy density of the
overall cell is significantly hindered by the diluting carbon mass.
In addition, the intercalation of such a large species leads to large

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NATure Energy
volumetric expansions as the cell is cycled between 0 and 100% state
of charge that can diminish the structural integrity of the carbon–
carbon layering. For our energy density calculations, a moderate
repeating unit of 36 carbons per AlCl4– was assumed.
Care must also be taken to properly account for the electrolyte
mass needed (Eq. (15)) to enable the Al oxidation reaction in Eq. (7).
Because the electrolyte participates in the reaction, it is necessary to
add enough salt for both high ionic conductivity and consumption
during operation, which introduces a significant electrolyte mass to
real cells. Because of this, the achievable capacity of an AIB is greatly
dependent on the AlCl3:[EMIm]Cl ratio in the electrolyte (r) as well
as the number of electrons required to reduce 1 mol of the anodic
material (x)23,24. As an example, the overall reaction for a 1 electron
transfer is provided in Eq. (9), which shows that x = 0.75 (based on
AlCl3).
1 4
Cn ½AlCl4  þ Al $ AlCl3 þ Cn
3 3
If r = 1.3, the energy density of the AIB is only 33 Wh kg–1.
Though increasing the r value does lead to an increase in the energy
density, r = 2 (62 Wh kg–1)23 is essentially a practical limit as the
electrolyte would be 64.5 wt% AlCl3. It should also be noted that the
value of r changes over the life of the device as the reaction proceeds.
For example, when r = 1.5 at the beginning of cell operation, 6 g of
electrolyte is required per gram of carbon (~60 g of electrolyte per
gram of Al). After a full cell discharge, the r value is reduced to 1.1
due to the depletion of AlCl4– from reaction with Al (Eq. (7))25. As
a result of its participation in the redox reactions, and the need to
maintain ionic conductivity during the charge/discharge, the major-
ity of the cell mass and volume in this battery system is comprised
by the electrolyte, with significant contributions from the carbon as
well. Therefore, accounting for the electrolyte mass and the cathode
mass, which is not commonly done in the AIB literature, is likely to
have catastrophic implications for the practically-achievable capac-
ity and gravimetric energy density.
Therefore, we have re-calculated the total cell capacities and
energy densities for several recent literature studies showing
state-of-the-art performance. Our analysis takes into account the
mass of the anode, cathode (assuming a best-case scenario N/P ratio
of 1), electrolyte (considering the effects of r and x), separator and
packaging. Taking the mass of all cell components into consider-
ation allows us to make practical cell-level estimations (based on
Eqs. (10) and (11) in the Methods) for capacity and energy den-
sity for AIBs and to compare our results with the literature claims.
The results are summarized in Table 2. It can be seen that when all
of the components are properly accounted for in Al/AlCl3:[EMIm]
Cl/graphite cells, the cell-level capacities lie in the range of
19–23 mAh g–1, which are considerably lower than the reported val-
ues (65–124 mAh g–1) —typically based on the mass of active mate-
rial on the cathode side23,25–31—and much lower than the often-cited
‘theoretical’ value of 2980 mAh g–1.
To combat the large gravimetric and volumetric issues of
graphitic cathodes, researchers have sought to find alterna-
tives that allow for smaller unit cells. This includes triangular
phenanthrene-quinone-based cathode materials that could increase
x from 0.75 to 1.5 (calculated cell-level capacity of 35 mAh g–1),
though stability was an issue32. Other attempts based on intercala-
tion reactions using 2D vanadium carbide (V2CTx) MXene cath-
odes33, or metal oxides such as VO2 (ref. 34) and V2O5 (ref. 7) showed
limited cycle life (<100 cycles) and capacity retention with calcu-
lated cell-level capacities in the range of 39–58 mAh g–1, which is
significantly lower than the reported unstable 116–305 mAh g–1
capacities (based solely on cathode mass).
Conversion cathodes have the potential to leverage more elec-
trons per Al than C and have higher intrinsic capacity because they
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Perspective
avoid intercalation. But, they do so at the cost of significant structural
transformation during cycling due to repeated bond-breaking and
bond-reformation steps, which sacrifice durability. Metal sulfides
such as MoS2 (ref. 35) (dual reaction mechanism via intercalation and
conversion), Co3S4 (ref. 36) (theoretical capacity = 702.8 mAh g–1),
and 3D Ni3S2 (ref. 37) (theoretical capacity = 462 mAh g–1) could
achieve calculated cell-level capacities in the range of 28–47 mAh g–1.
However, there is a large disparity between the cell-level capacities
and their theoretical values due to poor mass transfer and kinet-
ics, structural degradation and irreversible side reactions that
sacrifice both coulombic efficiency and cyclability. Cells utiliz-
ing multi-ion-based electrolytes have shown 26 mAh g–1 cell-level
capacity, which results in 92 Wh kg–1 energy density38, owing to
higher operation voltages. However, more studies are needed
to explore the reaction mechanism of this battery chemistry to
determine if the higher voltage is a result of redox reactions or
electrolyte oxidation.
ð9Þ To avoid intrinsic chemistry issues with IL-based non-aqueous
AIBs, researchers have also explored aqueous AIB chemistries.
Aqueous secondary AIBs may be possible if they can avoid Al plat-
ing by utilizing intercalation reactions39,40, which can be coupled
with manganese dioxide chemistries41–43. It is also important to
avoid electrode passivation by aluminium oxides; this is a particu-
larly difficult problem for aqueous rechargeable AIBs. To sidestep
such passivation, pre-treating Al with an AlCl3-IL (TAl) electro-
lyte has allowed surface enrichment of Al with organic functional
groups and the formation of a protective artificial solid electrolyte
interphase42, which enabled a fresh Al surface during charge/dis-
charge. A TAl/2m Al(CF3SO3)3/α-MnO2 cell was able to achieve a
380 mAh g–1 capacity (reported first discharge) and 500 Wh kg–1
energy density (based on the MnO2 mass). However, the capacity
decayed rapidly to 200 mAh g–1 after 10 cycles. Another demon-
stration of aqueous rechargeable AIBs (Al/AlCl3/graphite) used
a ‘water-in-salt’ electrolyte (AlCl3·6H2O:H2O ≈ 12, mass ratio),
achieving an average discharge voltage of 1.44 V and discharge
capacity of 165 mAh g–1. This cell was able to achieve 1000 cycles,
and demonstrated that ‘water-in-salt’ electrolytes can be effective
at facilitating the uniform deposition of Al44. However, the cou-
lombic efficiency fluctuated around 95% during cycling, which
indicated the presence of unwanted side reactions that would not
be tolerable in realistic full cells. Consequently, aqueous AIBs have
shown limited cycle numbers and capacity retention. Even though
the reported capacities for aqueous AIBs seem to be high (165–554
mAh g–1)41–44, more accurate calculations based on our analysis
dropped the cell-level capacities to 33–55 mAh g–1. The difference
is mainly due to imprecise evaluation of full cell conditions in the
literature.
A graphical comparison of calculated versus reported energy
densities for AIBs is shown in Fig. 2a. It can be seen that most of the
datapoints lie well below the parity line (solid grey line with slope
= 1), even on a log scale, showing the wide disparity between the
reported and achieved energy densities that was discussed above. It
is worth noting that all of the datapoints are also significantly lower
than the theoretical limits for AIBs calculated using Eq. (12) (463
Wh kg–1 with a C-based intercalation cathode to 796 Wh kg–1 with
a Co3S4 conversion cathode). However, Eq. (12) does not account
for the electrolyte contribution to the reaction chemistry. When
this is considered, the true upper limit for the energy density that
is practically achievable is only 80 Wh kg–1 for an AIB utilizing Al/
AlCl3–[EMIm]Cl/Graphite anode/electrolyte/cathode. The gap
between the practical energy density of AIBs and their theoreti-
cal limits is much larger than available chemistries in commercial
cells45 and even the calculated theoretical limits (from Eq. (12)) are
much lower than what is often quoted in the literature. Clearly, both
non-aqueous and aqueous AIBs are severely limited in terms of
their achievable capacity and gravimetric energy density.
25
26
Table 2 | Comparison of aqueous and non-aqueous secondary AIBs
Anode/ Electrolyte Battery type r x Current Capacity Coulombic Number Reported Reported Cell-level Cell-level Average Battery Ref.
Cathode rate retention efficiency of discharge energy capacity energy discharge operational
(mA %a %a Cyclesb capacity density (mAh g–1)d density capacity life (h)
–1 c
g–1) (mAh g–1)c (Wh kg ) (Wh kg–1)d (mAh g–1)e
Al/graphite AlCl3–[EMIm]Cl Non-aqueous secondary 1.3 0.75 4000 100 98 7500 65 40 19 27 65 246 26
Al/carbon AlCl3–[EMIm]Cl Non-aqueous secondary 1.3 0.75 100 100 100 100 70 98 20 28 70 140 27
paper
Perspective

Al/natural AlCl3–[EMIm]Cl Non-aqueous secondary 2 0.75 20000 70 99 250000 110 60 21 29 96 2418 25

graphite
Al/natural AlCl3–[EMIm]Cl Non-aqueous secondary 2 0.75 100 100 90 100 124 62 21 30 124 262 23
graphite
Al/graphene AlCl3–[EMIm]Cl Non-aqueous secondary 1.3 0.75 5000 97 98 25000 100 60 22 31 97 980 28
Al/natural AlCl3–[EMIm]Cl Non-aqueous secondary 1.3 0.75 660 100 99.5 6000 110 69 23 32 60 1094 29
graphite flakes
Al/trihigh AlCl3–[EMIm]Cl Non-aqueous secondary 1.3 0.75 100000 100 98 250000 120 66 23 32 120 606 30
tricontinuous
graphene film
Al/Porous 3D AlCl3–[EMIm]Cl Non-aqueous secondary 1.3 0.75 5000 100 98 10000 123 172 23 33 123 497 31
graphene
Al/PQ-triangle AlCl3–[EMIm]Cl Non-aqueous secondary 1.5 1.5 2000 50 99 2000 110 54 35 50 84 168 32
with graphite
flakes
Al/V2CTx AlCl3–[EMIm]Cl Non-aqueous secondary 1.3 - 200 56 96 100 160 192 39 47 110 112 33
Al/VO2 AlCl3–[EMIm]Cl Non-aqueous secondary 1 - 50 73 99 100 116 48 43 26 125 503 34
Al/V2O5 AlCl3–[EMIm]Cl Non-aqueous secondary 1 - 125 89 99 20 305 183 58 35 270 87 7
Al/MoS2-carbon AlCl3–[EMIm]Cl Non-aqueous secondary 1.3 - 100 43 95 200 293 293 47 47 155 636 35
nanofibres
Al/Co3S4 AlCl3–[EMIm]Cl Non-aqueous secondary 1.3 - 50 100 100 150 90 72 36 29 90 540 36
Al/Co9S8@ AlCl3–[EMIm]Cl Non-aqueous secondary 1.3 - 1000 56 96 6000 154 154 45 45 100 1225 49
CNT-CNF
Al/Ni3S2 AlCl3–[EMIm]Cl Non-aqueous secondary 1.5 - 10 17 100 100 236 189 28 22 50 1000 37
Al/graphite LiPF6+AlF3 EMC– Non-aqueous secondary - - 100 98 99 600 100 350 26 92 100 659 38
DMC, VC
Al/graphite AlCl3.6H2O Aqueous secondary - - 500 100 95 1000 165 220 55 79 165 677 44
Al/AlxMnO2·nH2O Al(OTF)3-H2O Aqueous secondary - - 30 58 85 20 467 481 42 46 409 593 41
IL-treated Al(CF3SO3)3 Aqueous secondary - - 100 44 100 40 380 500 41 54 250 200 42
Al/α-MnO2
IL-treated Al/ Al(OTF)3+MnSO4 Aqueous secondary - - 100 58 99 25 554 620 33 37 470 236 43
Birnessite–MnO2
a
Capacity retention (last cycle) and coulombic efficiency values were estimated from the given plots if not mentioned explicitly in the corresponding study. bFor the studies with considerable capacity fade, the cut-off discharge capacity of 70–75% initial capacity was assumed, and
the number of cycles was estimated based on that cut-off capacity criteria. cReported values from corresponding study (discharge capacity is usually related to the initial cycle). dOur calculated values based on Eqs. (10) and (11) in the Methods. Note: in non-aqueous systems with

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NATure Energy

graphite-based cathodes, the average voltage for all cases was assumed to be 1.4 V except the multi-ions system, which was 3.5 V. eAverage discharge capacity of initial and cut-off capacity was considered for the studies where the capacity retention (last cycle) was not close to
100%. Note: average discharge capacity was only used to calculate battery operational life.
NATure Energy
Battery life assessment
In addition to energy density, the durability of Al batteries was ana-
lysed in terms of battery operational life and compared with four
well-known aqueous and non-aqueous battery technologies. The
details for the battery operational life calculations are provided in
Methods. Of course, the lifetime of commercial batteries can range
widely depending on the current rate that is dictated by the applica-
tion. For the purpose of fair comparison, this study considered a
moderate rate (0.1 to 1 mA) for primary commercial batteries and
250–300 cycles per year were assumed for secondary commercial
batteries to be comparable with testing conditions of Al batteries in
the literature. Therefore, there is a specific range that can be calcu-
lated for battery life and energy density. In Fig. 2b, it can be seen that
aqueous primary AABs have considerably lower energy density and
operational life compared to Zn–MnO2 alkaline batteries—their
main competitor in the commercial space. Non-aqueous primary
AABs can operate for longer times and higher voltages compared
to aqueous AABs, and the achievable energy density is higher for
non-aqueous AABs (Table 1). Though the cell-level energy density
of the highest performing non-aqueous primary AAB is compara-
ble with industry-leading LiFeS2, the operational lifetime remains
orders of magnitude lower.
In rechargeable aqueous AIBs, utilizing AlCl3-based water-in-salt
electrolytes might be promising—presently delivering a 79 Wh kg–1
cell-level energy density. Batteries with Al(OTF)3-based aqueous
electrolytes have shown energy densities that are comparable with
lead–acid batteries. However, the operational life for aqueous AIBs
is significantly lower than lead–acid batteries. Also hampering com-
mercial deployment is the fact that Al(OTF)3 based aqueous elec-
trolytes are ~130 times more expensive than AlCl3-based aqueous
electrolytes and are double the cost of non-aqueous AlCl3-[EMIm]
Cl electrolytes44. For non-aqueous AIBs with an Al/AlCl3-[EMIm]
Cl/graphite chemistry, the achievable lifetimes are much lower than
the incumbent technology, Li-ion batteries, which have substan-
tially longer operational life than any other non-aqueous AIB.
Outlook
In this Perspective, the recent development of Al battery technol-
ogy was highlighted from a practical perspective and a quantitative
analysis of current energy density values in Al battery technology
was performed. It was realized that in aqueous alkaline electro-
lytes, anodes that are principally comprised of Al metal have seri-
ous corrosion and gassing issues in addition to poor solubility of
Al(OH)4–—leading to passivation as either Al(OH3) or Al2O3. For
Al-based batteries with non-aqueous acidic IL electrolyte, a huge
amount of supporting electrolyte needs to be carried which signifi-
cantly reduces the gravimetric and volumetric energy density.
A comparison of battery performance of aqueous and
non-aqueous AIBs clarifies that aqueous systems can deliver high
capacities but short cycle life and poor capacity retention. In con-
trast, non-aqueous AIBs have a higher operation and cycle life,
but have limited capacity. They also rely on IL electrolyte, which is
likely a non-starter for most applications, since they are expensive
and require highly specialized, expensive cell materials to avoid cor-
rosion (Ti, Ta, Mo)—though it may be possible to develop coatings
to enable stainless steel hardware, and more stable current collec-
tors. Furthermore, ILs have not been produced at the required scale
and may require non-ambient cell construction and materials pro-
cessing. Another issue with non-aqueous AIBs is mass transport,
because ion movement occurs in the opposite direction of diffusion.
Finally, the fundamental chemistry of Al in existing ILs requires a
significant electrolyte mass to be carried, which limits the achiev-
able energy density values. For example, the practical energy density
of an Al/AlCl3–[EMIm]Cl/Graphite AIB is 27–50 Wh kg–1. The con-
tribution of significant electrolyte mass in this battery system is an
inevitable fact, making its future deployment doubtful.
Nature Energy | VOL 6 | January 2021 | 21–29 | www.nature.com/natureenergy
Perspective
Related to AABs, in addition to poor achievable life their practi-
cal energy densities remain ~10–15 times lower than their theoreti-
cal values. In addition to the limitations of Al, the low energy density
is caused by the ORR at the AAB cathode which is kinetically slow,
and product instability leads to the formation of a barrier layer with
a gel-like consistency comprised of aluminum–oxygen-organic spe-
cies. This causes generally poor performance (that is, low discharge
voltage even at low rates). Moreover, AABs are not cost effective,
since all modern high performing, long life ORR cathodes rely on
expensive electrocatalysts. Therefore, there should be more of a
focus on other types of battery chemistries than AAB, though it is
questionable whether primary battery technologies with metal Al
anodes (even using corrosion inhibitors or alloying with other met-
als) can ever be deployed.
Hopefully, this Perspective benefits the battery research com-
munity by presenting a more realistic picture regarding the status
of Al battery technologies. There are many attractive features for
Al-based batteries and there are obvious possible advantages over
existing batteries, including Li-ion. However, there is clearly a size-
able gap between the current state of rechargeable AIBs and existing
Li-ion technologies. Today, it appears that this gap may inevitably
prove insurmountable. For that statement to be wrong, it is likely
necessary for the community to completely rethink the chemistry
of existing Al batteries, revisit the cathode materials and electrolytes
that would enable the use of Al in the future, and carefully evaluate
the cell balancing for practicality by adjusting the N/P ratio.
Methods
AAB cell-level energy density. The methodology to calculate cell-level capacity,
energy density and battery operational life is provided in this section. One of the
essential points in our analysis was to consider the mass of every component in a
cell: anode, cathode, electrolyte, separator and packaging, though packaging was not
extensively discussed in the main text. The average voltage was estimated based on the
discharge curves in the original paper, if not mentioned explicitly in the given study.
For AABs, the amount of charge passed for the Al anode (Q) was calculated based on
the reported capacity and the mass of the Al used. Then, the mass of consumed Al was
estimated by dividing Q by the theoretical capacity of Al. It was assumed that the N/P
ratio is equal to 1. The mass (mi) of the cathode and electrolyte were estimated based
on the information provided in each study. The mass of the separator and packaging
were assumed to take 5% and 30% of the total mass, respectively, based on available
estimations for these components of AABs18. This allowed the cell-level capacity and
energy density to be calculated using Eqs. (10) and (11).
Ccell�level ¼
Q
ð10Þ
manode þ mcathode þ melectrolyte þ mseparator þ mpackage
Energy density ¼ Ccell�level ´ Vavg ð11Þ
Where Vavg is the average is the average discharge voltage.
AIB cell-level energy density. For AIBs, a slightly modified version of the AAB
method was used in the calculations that can be generalized easily for any AIB
system that aims to become commercialized. Again, it was assumed that the N/P
ratio is 1, though here a common Al mass (1 g) was assumed. Then, the amount
of charge passed for the anode was calculated based on the reported conditions.
The charge passed and the reported cathode capacity were used to determine the
cathode mass. Next, using the electrolyte molecular weights, concentration or
density of dissolved reactant, r value (ratio of AlCl3:[EMIm]Cl in the electrolyte,
needed in the chemistries that involve AlCl3–[EMIm]Cl electrolyte) and number
of electrons, the mass of electrolyte was estimated and it was found that the
approximate ratio of the electrolyte mass to the cathode mass is ~3 in most cases,
which is consistent with the calculations done by Elia et al.25. Finally, we estimated
the mass of the separator and packaging to be 5% and 10%, respectively, based on
available estimations for these components of AIBs25.
AIB theoretical energy density. For comparison sake, in addition to the achieved
energy density, it is important to calculate the maximum theoretical energy density
for an AIB battery, which is given by Eq. (12)46.
CA CC
Theoretical energy density ¼ ´V ð12Þ
CA þ CC
Where CA and CC are the theoretical capacities for the anode and cathode,
respectively, and V is the cell voltage.
27
Perspective
Battery operational life. For primary Al batteries the battery operational life is the
same as discharge time. In the studies that the discharge time was not mentioned
explicitly, the battery operational life was calculated using Eq. (13).
Qdis
Battery operational lifeðprimary Þ ¼ ð13Þ
idis
In which Qdis is the charge passed during discharge (mA) and idis represents the
load current (mA). For commercial Zn–MnO2 and LiFeS2 batteries the
rated capacity to cut-off voltage of 0.8 V at 21 ̊C between 0.1 and 1 mA was
considered.
For secondary Al batteries, Eq. (14) was used to estimate the battery
operational life.
 
Cdis 1
Battery operational lifeðsecondary Þ ¼ ´ m ´ 1þ ð14Þ
jdis CE
Where Cdis is the discharge capacity (mAh g–1), jdis is the current rate (mA g–1), m is
the number of cycles and CE is the coulombic efficiency (%). This calculation
takes all of the parameters that are important in evaluating battery performance
into consideration such as discharge/charge capacities, current rate, number
of cycles, capacity retention and coulombic efficiency. Basically, given the
discharge capacity (mAh g–1) and current rate (mA g–1), the discharge time for
each cycle can be calculated, and then using the number of cycles and coulombic
efficiency, the total operational time of the battery can be estimated. In studies with
overall low capacity retention, there is typically a region with somewhat
stable capacity; this region was used in our analysis to estimate discharge capacity.
For commercial lead–acid and Li-ion batteries the lifetime of 4–6 years and
~15–25 years was considered, respectively, based on the assumption of 250–300
cycles per year47.
Al/AlCl3–[EMIm]Cl/graphite battery configuration. The full-cell reaction for a 1
electron reaction is provided in Eq. (9), which shows that x = 0.75 (x is the number
of electrons used to reduce 1 mole of AlCl3). It was assumed that for every AlCl4–
intercalated, 36 C atoms are needed22 and the average operating voltage is
Vavg = 1.4 V. Then, the mass of cathode can be calculated based on reported
discharge capacity. For example, Lin. et al. reported 65 mAh g–1 (ref. 26). Therefore,
mCathode = 45.8 g. The overall number of electrons based on the charge passed is:
N ¼ xF Q
, with F being Faraday’s constant (96485 C mol e−1). The mass of electrolyte
isI then determined by considering 36 C atoms per AlCl4– and the value for r:
melectrolyte ¼ N ðrMAlCl3 þ MEMIMcl þ 36MC Þ ð15Þ
Where MAlCl3 = 133.34 g mole–1, MEMIMcl = 146.62 g mole–1 and MC = 12 g mole–1.
Next, it was
I assumed that the mass of the separator and the package mass
contributed to 5% and 10% of the total mass, respectively25. Finally, the cell-level
energy density was determined by multiplying Ccell-level = 19 mAh g–1 with Vavg,
which gives 27 Wh kg–1.
In addition, the theoretical capacity for this battery system is estimated to be
67 mAh g–1 (given in the primary text) as indicated below:
nF
Ctheoretical ¼ ð16Þ
3:6 ´ ðMAl þ 7MAlCl4 Þ
In Eq. (16), n is 3e–, MAl = 26.98 g mole–1, MAlCl4 = 168.8 g mole–1 and
F = 96485 C mol e–1. I high-quality natural graphite cathode. Nat. Commun. 8, 14283 (2017).
Received: 22 July 2020; Accepted: 26 October 2020;
Published online: 14 December 2020
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Competing interests
The authors declare no competing interests.
Additional information
Correspondence should be addressed to W.E.M.
Peer review information Nature Energy thanks Stanley Whittingham and the other,
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