FIELD OF INVENTION
[0001] The present disclosure broadly relates to the field of battery. Particularly,
the present disclosure relates to a multi-ion battery comprising a blended cathode,
a multi-ion conducting electrolyte, and a fused anode. Further, the present
5 disclosure provides a process of preparing thereof.
BACKGROUND OF INVENTION
[0002] Rechargeable Li metal batteries (LMBs) have received a lot of attention
recently, because of their potential to meet the rapidly growing demand for high
energy density storage systems. Despite having a high specific capacity (3860 mA
h g-1
10 ) and a low electrochemical potential (-3.04 V vs the standard hydrogen
electrode, (SHE)), the Li metal anode has an unstable solid electrolyte interphase
(SEI) layer. Moreover, repeated Li plating/stripping processes hasten the cracking
and reforming of the SEI layer, consuming electrolyte and Li ions. This results in
low coulombic efficiency (CE), accumulated SEI layer, and increased interfacial
resistance. Furthermore, non-uniform Li+
15 flux causes uneven plating and Li
dendrites, posing serious safety concerns. Many studies have recently been
conducted to address these issues, such as three-dimensional scaffolds, artificial
SEI layers, highly concentrated electrolytes, and various additives. These methods
are critical in guiding Li plating, stabilizing the electrode/electrolyte interphase, and
20 limiting side reactions. Although Li metal anodes generally inherently exhibit large
voltage hysteresis, reducing energy efficiency and limiting the application of
LMBs, non-dendritic morphologies and high CE (>99%) could be obtained by
modifications and engineering of anode structure.
[0003] Cui's group discovered that Na is compatible with a liquid sodium-based
25 electrolyte (NaPF6 in ethers) for highly reversible and non-dendritic Na
plating/stripping with low voltage hysteresis in coin cells. Moreover, Sodium is less
expensive and eco-friendly. Sodium-ion batteries are non-flammable and less
sensitive to temperature changes than lithium-ion batteries, hence they are safer.
Besides, due to the heavier atomic mass and larger ionic radius of Na, cathode
30 materials for Na batteries generally exhibit poorer insertion kinetics and lower
capacity than those for lithium batteries. The major drawback is that compared to lithium-ion batteries, sodium-ion batteries have a lower energy density. This
implies that a sodium-powered electric vehicle (EV) with a battery of same size as
a typical lithium-ion battery would not be able to travel as far on a single charge. In
addition, sodium-ion batteries degrade more quickly when additional voltage is
5 applied to the same area. As a result of the high performance of both the Na metal
anode and the lithium cathode in various aspects, some researchers built an
advantageous Li-Na hybrid battery (LNHB). It is also worth noting that the
electrochemical behaviours of Li/Na metal anodes of these hybrid batteries, in
ether-based electrolytes are intrinsically different. But specific capacity and energy
10 density achieved by these lithium-sodium hybrid battery compositions are still
lagging behind. Therefore, there is a dire need in the art to develop a multi-ion LiNa hybrid battery comprising a cathode, multi-ion conducting solid electrolyte and
an anode with lower internal resistance and enhanced specific capacity working in
a wider potential window.
15 SUMMARY OF THE INVENTION
[0004] In a first aspect of the present disclosure, there is provided a battery
comprising: (a) a cathode composite; (b) an anode composite; and (c) an electrolyte
composite, wherein the cathode composite is a blended cathode comprising oxides
of lithium and sodium, the anode composite is a fused anode comprising metallic
20 lithium and metallic sodium, and the electrolyte composite is a multi-ion
conducting electrolyte composite sandwiched between the cathode composite and
anode composite.
[0005] In a second aspect of the present disclosure, there is provided a process of
preparing the battery as disclosed herein, comprising: a) independently preparing a
25 cathode composite, an anode composite and an electrolyte composite; and b)
stacking the cathode composite, the anode composite, and the electrolyte composite
under applied pressure to obtain the battery, wherein the electrolyte composite is
sandwiched between the cathode composite and anode composite.
[0006] In a third aspect of the present disclosure, there is provided a use of the
30 battery as disclosed herein, for the manufacture of energy storage devices and
electronic appliances.
[0007] These and other features, aspects, and advantages of the present subject
matter will be better understood with reference to the following description. This
summary is provided to introduce a selection of concepts in a simplified form. This
summary is not intended to identify key features or essential features of the claimed
5 subject matter, nor is it intended to be used to limit the scope of the claimed subject
matter.

/We Claim:
1. A battery comprising:
a. a cathode composite;
b. an anode composite; and
5 c. an electrolyte composite,
wherein the cathode composite is a blended cathode comprising a layered
oxide of lithium and a layered oxide of sodium, the anode composite is a
fused anode comprising metallic lithium and metallic sodium, and the
electrolyte composite is a multi-ion conducting electrolyte composite
10 sandwiched between the cathode composite and anode composite.
2. The battery as claimed in claim 1, wherein the blended cathode comprises
a. a conducting additive; and
b. a binder.
3. The battery as claimed in claim 1, wherein layered oxide of lithium and
15 layered oxide of sodium in a weight ratio range of 80:20 to 60:40 with
respect to the cathode composite.
4. The battery as claimed in claim 1, wherein the layered oxide of lithium is
selected from LiNi0.8Co0.1Mn0.1O2, LiNi0.5Co0.2Mn0.3O2,
LiNi0.33Co0.33Mn0.33O2, LiNi0.6Co0.2Mn0.2O2, LiMnO, LiNiO, LiFePO4,
20 LiMnPO4, or LiNiPO4.
5. The battery as claimed in claim 1, wherein the layered oxide of sodium is
selected from NaNi0.33Fe0.33Mn0.33O2, NaNi0.33Ti0.33Mn0.33O2,
NaNi0.6Fe0.2Mn0.2O2, NaNi0.43Ti0.24Mn0.23O2, NaMnO, NaNiO, NaFePO4,
NaMnPO4, or NaNiPO4.
25 6. The battery as claimed in claim 2, wherein the conducting additive is
selected from carbon black, graphite, acetylene black, carbon nanotube
(CNT), or combinations thereof.
7. The battery as claimed in claim 2, wherein the binder is selected from
polytetrafluoroethylene (PTFE), polyether ether ketone (PEEK),
30 poly(tetrafluoroethylene-co-perfluoropropyl vinyl ether) (PFA),
polypropylene, polyacrylonitrile (PAN), tetrafluoroethylene-co hexafluoropropylene-co-vinylidene (THV), poly(tetrafluoroethylene-cohexafluoropropylene) (FEP), polyvinyl difluoride (PVDF), vinyl difluoride
(VDF), or combinations thereof.
8. The battery as claimed in claim 1, wherein the cathode composite is in the
5 form of a thin film having thickness in a range of 50 to 150 µm.
9. The battery as claimed in claim 1, wherein the anode composite comprises
metallic lithium and metallic sodium in a weight ratio range of 99:1 to 1:99.
10. The battery as claimed in claim 1, wherein the anode composite is in the
form of a film having thickness in a range of 60 to 150 µm.
10 11. The battery as claimed in claim 1, wherein the anode composite further
comprises Li-Sn alloy, Na-Sn alloy, Na-Sb alloy, Li-C alloy, Na-C
composite, Si-C composite, or combinations thereof.
12. The battery as claimed in claim 1, wherein the electrolyte composite
comprises:
15 a. at least one argyrodite-type solid electrolyte comprising lithium;
b. at least one NASICON-type ceramic electrolyte comprising sodium;
and
c. a polymer,
wherein weight ratio of the argyrodite-type solid electrolyte and the
20 NASICON-type ceramic electrolyte is in a range of 99:1 to 1:99.
13. The battery as claimed in claim 12, wherein the at least one argyrodite-type
solid electrolyte is selected from Li6PS5Cl, transition metal doped-Li6PS5Cl,
lithium aluminium titanium phosphate (LATP), lithium lanthanum
zirconium oxide (LLZO), lithium phosphorous oxynitride (LiPON), lithium
25 germanium phosphorous sulfide (LGPS), lithium phosphorous sulfide
(LPS), or combinations thereof.
14. The battery as claimed in claim 12, wherein the at least one NASICON-type
ceramic electrolyte is selected from Na1+xZr2SixP3−xO12, wherein 0 < x < 3,
optionally doped with Sc, Mg, Ni, La, or Hf, Na3Zr2Si2PO12 (NZSP);
30 sodium β-alumina; Na3PS4 (sodium thiophosphate); Na2B12H12 (sodium borohydride); sodium tin phosphorous sulfide (NSPS), or combinations
thereof.
15. The battery as claimed in claim 12, wherein the polymer is selected from
polytetrafluoroethylene (PTFE), polyether ether ketone (PEEK),
5 poly(tetrafluoroethylene-co-perfluoropropyl vinyl ether) (PFA),
polypropylene, polyacrylonitrile (PAN), tetrafluoroethylene-cohexafluoropropylene-co-vinylidene (THV), poly(tetrafluoroethylene-cohexafluoropropylene) (FEP) or combinations thereof.
16. The battery as claimed in claim 12, wherein the electrolyte composite is in
10 the form of a thin membrane having a thickness in a range of 50 to 100 µm.
17. A process of preparing the battery as claimed in claims 1 to 15, comprising:
a. independently preparing a cathode composite, an anode composite and
an electrolyte composite; and
b. stacking the cathode composite, the anode composite, and the
15 electrolyte composite under applied pressure to obtain the battery,
wherein the electrolyte composite is sandwiched between the cathode
composite and anode composite.
18. The process as claimed in claim 17, wherein, step (a), preparing the cathode
composite comprises:
20 i. mixing a layered oxide of lithium, and a layered oxide of sodium
with a conducting additive to obtain a first mixture;
ii. adding a binder to the first mixture, and shearing to obtain a second
mixture; and
iii. processing the second mixture to obtain the cathode composite.
25 19. The process as claimed in claim 18, wherein the mixing in step (i) is carried
out at a speed in a range of 500 to 1500 rpm for a time period in a range of
30 to 1200 seconds.
20. The process as claimed in claim 18, wherein the shearing in step (ii) is
carried out at a shear speed in a range of 0.1 to 1.5 m/min.
30 21. The process as claimed in claim 18, wherein processing the second mixture
is carried out by pressing, folding, roll-to-roll shearing, or combinations thereof; and the roll-to-roll shearing is carried out at a pressure in a range of
100 kN to 3000 kN.
22. The process as claimed in claim 17, wherein, step (a), preparing the anode
composite comprises:
5 i. mixing metallic sodium and metallic lithium under applied pressure to
obtain a blend; and
ii. rolling and pressing the blend to obtain the anode composite.
23. The process as claimed in claim 17, wherein, step (a), preparing the
electrolyte composite comprises:
10 i. grinding at least one argyrodite-type solid electrolyte and at least one
NASICON-type ceramic electrolyte together to obtain a powder
mixture;
ii. shear-mixing the powder mixture with a polymer to obtain a dough; and
iii. subjecting the dough to shearing under pressure to obtain the electrolyte
15 composite.
24. The battery as claimed in claim 1, wherein the battery exhibits a specific
capacity in a range of 180 to 230 mAh/g, capacity retention in a range of 97
to 99%, coulombic efficiency in a range of 85 to 99%, and operating
potential window in a range of 1.5 to 4.6 V.
20 25. Use of the battery as claimed in claim 1, for the manufacture of energy
storage devices and electric devices.