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Results in Engineering 21 (2024) 101651

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Results in Engineering
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High power and thermal-stable of graphene modified LiNi0.8Mn0.1Co0.1O2


cathode by simple method for fast charging-enable lithium ion battery
Rosana Budi Setyawati a, b, Khikmah Nur Rikhy Stulasti b, Yazid Rijal Azinuddin b,
Windhu Griyasti Suci b, c, Harry Kasuma (Kiwi) Aliwarga d, Endah Retno Dyartanti a, b,
Agus Purwanto a, b, *
a
Department of Chemical Engineering, Faculty of Engineering, Universitas Sebelas Maret, Surakarta, 57126, Indonesia
b
Centre of Excellence for Electrical Energy Storage Technology, Universitas Sebelas Maret, Surakarta, 57146, Indonesia
c
Vocational School, Universitas Sebelas Maret, Surakarta, 57126, Indonesia
d
UMG Idealab, Jakarta, 12930, Indonesia

A R T I C L E I N F O A B S T R A C T

Keywords: The use of batteries in modern electronic devices and electric cars is becoming increasingly important. Batteries
Cathode with high energy density, high rate and cycle capability, as well as operational safety, are in high demand today.
Fast-charging The cathode of a lithium-ion battery is a part that significantly affects the performance of the battery.
Graphene
LiNiMnCoO2 (NMC) cathode, especially in the composition of LiNi0.8Mn0.1Co0.1O2 (NMC811), has high specific
Lithium-ion battery
NMC
capacity but not high thermal and electrical conductivity stability. To improve the temperature stability and
performance of the battery, conductive elements such as graphene can be added. The addition of graphene can
increase battery performance due to its high electrical conductivity characteristics. In this study, the addition of
graphene on NMC cathode through a simple solid-state technique along with direct mixing was shown to
improve the cathode characteristics. The addition of graphene on the NMC cathode also proved to be capable of
improving the cycle stability and rate capability. The retention capacity is 95.83 %, higher than that of the
cathode without graphene modification, which is 92.27 % after 100 cycles with 1C current, and comparable to
the capability of commercial batteries. The ability to work under rapid charge and discharge conditions was also
well demonstrated with a capacity drop of 5.44 % over 200 cycles at a charge and discharge current of 5C. The
addition of graphene was also shown to improve the safe use of NMC batteries. With the test at 5C current, the
highest temperature of the battery was 46.52 ◦ C, which is still considered safe for the operation of lithium ion-
based batteries at high currents. In this research, the use of a simple solid-state method to mix the graphene with
NMC811 cathode is proven to be able to produce lithium-ion batteries with superior performance. This offers
ease in terms for use in large-scale production of cathode preparation that can produce high-performance
cathodes.

1. Introduction solar system and transportation sector [8–11]. Along with its develop­
ment, energy storage in the form of electronic devices is required to be
Basically, all human activities require energy [1,2]. Energy sources efficient, lightweight, not oversized, and have high performance [12].
to fulfill human needs are still dominated by fossil fuels that are limited The solution to this problem is to use Li-ion batteries [13], which have
in availability and cause environmental problems [3,4]. In today’s era, advantages including high performance in the charge-discharge process,
energy can be stored so that its use becomes more practical [5]. One of high energy density, no memory effect, and small possibility of
the most efficient and popular energy storage devices used today is the self-discharge [14]. Improved Li-ion battery performance can be seen
battery [6]. Batteries are widely applied to electronic equipment such as from its ability to store large electrical capacity, produce good cycle
laptops, cell phones, drones, remotes, and so on [7]. In addition to this stability, and produce high energy density [15]. In addition, to fulfill the
mobile electronic equipment, batteries are also used in the mini-grid needs for electric vehicles, high-specification batteries are needed with

* Corresponding author. Department of Chemical Engineering, Universitas Sebelas Maret, Surakarta, 57126, Indonesia.
E-mail address: aguspurwanto@staff.uns.ac.id (A. Purwanto).

https://doi.org/10.1016/j.rineng.2023.101651
Received 4 July 2023; Received in revised form 15 November 2023; Accepted 1 December 2023
Available online 7 December 2023
2590-1230/© 2023 The Authors. Published by Elsevier B.V. This is an open access article under the CC BY license (http://creativecommons.org/licenses/by/4.0/).
R.B. Setyawati et al. Results in Engineering 21 (2024) 101651

good performance at high currents in both charging and discharging addition, Jan has also tried to modify NMC811 with graphene nano­
processes [16]. The fast-discharging capability of lithium-ion batteries is sheets by grounding followed by ultrasonication using ethanol [38]. The
needed in the use of equipment that requires high power. Fast charging performance improvement obtained by modifying the NMC cathode
capability is needed to compete with fuel-based vehicles [17]. Users will with graphene is quite good, but some of the methods that have been
compare the charging ability of fuel oil which only takes a few minutes done are difficult if they are to be used industrially. To be carried out on
to fully charge [18]. However, charging with high currents in lithium a large scale, a simple process and simple materials are needed, but it
ion batteries can decrease the energy efficiency value and cause rapid also produces a good product. Therefore, optimization of the method
capacity degradation [19]. and composition of adding graphene material to the NMC cathode is
The diffusion and ion transfer process at the electrode is the deter­ needed in the development of lithium-ion batteries to obtain the most
mining factor, so the selection the right electrode material is needed to optimal application formula for use on an industrial scale. This research
improve the diffusion kinetics of electrons and lithium ions at the was conducted by adding graphene to the NMC811 lithium-ion battery
electrode so that the charging and discharging process becomes faster cathode by means of simple solid-state mixing which is expected that
[18]. The cathode is a lithium ion battery component that has a major although the steps taken are only simple, it can facilitate its realization
role in the performance of a battery [20]. This is because the process of in the industry. In addition, the optimum composition of graphene
transferring lithium ions during the charging and discharging process is addition was also determined. To evaluate the results obtained, perfor­
strongly influenced by the structure of the cathode. Several types of mance testing is carried out which is expected to produce a battery that
lithium ion battery cathodes that have been widely used include LCO is able to demonstrate its ability in terms of fast charging and fast dis­
(Lithium Cobalt Oxide), LMO (Lithium Manganese Oxide), NCA charging needed in various applications including electric vehicles.
(Lithium Nickel Cobalt Aluminum Oxide), LFP (Lithium Iron Phospha­
te/LiFePO4), and NMC (Lithium Nickel Manganese Cobalt Oxide) [21, 2. Methods
22]. Among these cathode types, NMC is a cathode material in lithium
batteries that has excellent advantages such as high capacity [23], high The work consists of two stages, material preparation and battery
current stability, relatively high volume capacity, and long cycle life preparation, which are shown in Fig. 1. The material preparation con­
[24]. Cathode materials such as NMC, especially LiNi0.8Mn0.1Co0.1O2 sists of sieving, weighing, and drying the material. Meanwhile, battery
(NMC811), which have a high specific capacity, have the disadvantage preparation consists of making NMP-PVDF solution and mixing powder
of low electrical conductivity, causing a rapid decrease in specific ca­ by solid state method, then mixing, coating, drying, and assembly as a
pacity [25]. In addition, the result of low electrical conductivity also battery.
causes low rate ability, which limits the use of high-current batteries The first step in making NMC cathode material modified with gra­
[26]. To overcome these problems, several ways can be done, including phene is sieving the LiNi0.8Mn0.1Co0.1O2 (NMC811) material through a
by reducing the particle size to the nanomaterial scale [27], which can 200-mesh sieve. All materials including NMC, acetylene black (AB) and
help increase the surface area of the material, or by adding more PVDF, also graphene powder were weighed according to the required
conductive materials [28]. Polycrystalline NMC (PC NMC) is a type of composition. Considering that the materials used are very sensitive to
NMC cathode active material that has been widely commercialized, so it humidity and atmospheric conditions, pretreatment was carried out by
is easy to find on the market. However, PC NMC has poor stability when storing all materials in a vacuum oven at 90 ◦ C before use.
compared to the single-crystalline NMC (SC NMC) type [29]. Therefore, Then, the cathode was prepared by simple direct mixing. PVDF was
it is necessary to modify the PC NMC material to improve its perfor­ dissolved in NMP using a stirrer under vacuum. A mixture of active
mance. In this study, PC NMC811 material is used with the addition of material (NMC) powder , conductive material AB, and graphene was
conductive material to increase the conductivity of the material, which prepared with graphene composition of 0 % (NMC-G 0 %), 4 % (NMC-G
can improve its performance. 4 %), 7 % (NMC-G 7 %), and 10 % (NMC-G 10 %) of the total compo­
Improving the performance of Li-ion batteries with the addition of sition with NMC composition of 94 %, 90 %, 87 % and 84 % respectively
conductive materials has started at the LMO and LFP cathodes with the with AB composition fixed at 1 %. Then, NMC, AB, and graphene
addition of activated carbon [30,31]. Activated carbon is a relatively powders were mixed using the solid-state method using a mortar and
cheap material and has good cycling ability and rate ability, but has a pestle for 2 h under atmospheric conditions. The mixed solid materials
low specific capacity. Several studies have been conducted to improve were kept in a vacuum oven at 90 ◦ C while waiting for the PVDF to
the performance of NMC811 cathode by adding conductive materials dissolve homogeneously in NMP. The solid mixtures were then charac­
such as graphene oxide (GO) [32,33], reduced graphene oxide (rGO) terized to compare the material changes.
[34], carbon black [35], carbon nanotubes (CNT) [36], graphene [37, The powder mixture (NMC, AB, and graphene) was mixed with the
38], amorphous carbon [39], and carbon coating [40]. Graphene ma­ PVDF solution for 3 h at a constant speed of 1000 rpm until a homo­
terial is one of the promising materials that can be chosen because of its geneous slurry was formed. The mixing process was carried out under
material advantages. Graphene is a material that is widely used as vacuum conditions to avoid exposure to atmospheric air. The slurry was
supercapacitors, conductive coating component, catalysts, and for other casted on aluminium foil with a thickness setting of 200 μm. The slurry
purposes [41–43]. Graphene has a medium specific capacitance and was then dried overnight at 90 ◦ C in a vacuum oven. 18650 cylindrical
high electrical conductivity. The addition of graphene can increase cells underwent electrochemical tests with graphite anode which is a
battery capacity due to its high electrical conductivity characteristics commercial anode material in lithium-ion batteries [52], PP separator,
[44] and its large active surface material [45], so it has been widely used and 1 M LiPF6 in EC + EMC 3:7 (volume ratio) as the electrolyte. In this
to improve the electrochemical characteristics of anode and cathode study, the ratio of negative and positive electrode areal capacity (N/P
materials [46]. The addition of graphene can cause the electrochemical ratio) of 1.2 was used because it had been proven to produce the best
characteristics of the material to increase, especially in rate ability [47]. battery cycle among other ratios [53]. The type of separator used was PP
The graphene used must also be of superior quality so as not to degrade separator which has been widely commercialized, so it is easy to find.
battery performance [48]. The tests carried out consist of material characterization (raman
However, in some studies that have been conducted, the method of spectroscopy, XRD, FTIR, and SEM), electrochemical testing (EIS testing,
adding graphene must go through several long stages [49–51]. Fan capacity testing, lifecycle, and rate capability) and thermal stability
modified the NMC811 cathode by creating an ion-conducting layer testing. Raman spectroscopy testing was performed with Raman iHR320
made by reacting H3PO4 with lithium residue on the surface of NMC811 Horiba. An XRD (X-Ray Diffractometer) from D2 Phaser Bruker, Ger­
to form Li3PO4 and then forming an interface with high electronic many, was used for the analysis of the crystal structure of the powder
conductivity by attaching graphene fragments to NMC811 [37]. In mixture using CuKα radiation λ = 1.54 Å with 2θ range of 10–80◦ and a

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R.B. Setyawati et al. Results in Engineering 21 (2024) 101651

Fig. 1. Research method Diagram of (a) material preparation and (b) battery preparation.

scanning speed of 0.02◦ per second. A Shimadzu (Japan) FTIR spec­ NMC raw materials, it is also in accordance with the reference. So, the
trometer with a mid-IR region (4000-400 cm− 1) was used to analyze the test results of raw materials show that the graphene material used is as
functional groups of the materials. A scanning electron microscope expected. Synthesis of NMC-Graphene composite material has been
(SEM) (JEOL JSM-6510 LA, Japan) was used in the morphs of the successfully carried out using solid state mixing method. Material
sample. EIS electrochemical testing was performed with the NuVant characterization tests were carried out to determine the structure of the
Systems EZstat Potentiostat. The electrochemical performance was material after the addition of graphene to the NMC material. X-Ray
further tested for battery performance in cylindrical cell batteries using Diffractometer (XRD) testing was carried out to determine the crystal
a NEWARE Battery Analyzer and BTS program with a voltage window of structure of the material formed. Fig. 2 shows the XRD test results of
2.6–4.2 V to test the capacity, lifecycle, and rate capability of the bat­ graphene-modified NMC cathode material.
tery. Battery temperature stability during the test was observed using The XRD pattern presented in Fig. 2 shows that all samples comply
thermocouples attached to each cell. After testing in the form of a single with the JCPDS standard (No. 82–1495) and do not have a secondary
cell, performance testing was carried out using assembled drone device phase. All samples have a diffraction pattern of hexagonal structure
with the F450 drone type. Testing is done by applying the battery as a α-NaFeO2 (space group R3m). The splitting of (006)/(102) and (108)/
source of driving energy on the drone. Tests were carried out with 2 (110) peaks at 38◦ and 65◦ were clearly identified, indicating that the
battery versions, the first with a 3S1P battery array and the second
version using a 3S2P array applied to the same drone.

3. Results and discussion

3.1. Material characterization

Material characterization testing was carried out for testing starting


materials and materials resulting from the solid-state process. Tests
carried out include raman spectroscopy, XRD, FTIR, and SEM. Previ­
ously, tests were carried out on the starting material to ensure its purity
and suitability for use. The tests carried out were Raman spectroscopy
and XRD, which are shown in Fig. S1 and Table S1 for Raman spec­
troscopy test results, and Fig. S2 for XRD test results. The specifications
of the graphene material used are attached in Table S2. Based on the
Raman test results, the graphene used has the same peak as the reference
in the D bands, G bands, and 2D bands with the ratio of the peak in­
tensity of the D to G bands (ID/IG) of 0.212 which is included in the
graphene material class [54]. As for XRD testing of AB, graphene, and
Fig. 2. XRD patterns of NMC-G in various graphene addition.

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R.B. Setyawati et al. Results in Engineering 21 (2024) 101651

material has a highly ordered layered structure [55]. A well-ordered


layered structure is required for efficient lithium-ion inter­
calation/deintercalation during discharge [56]. In addition, the sharp
peaks of 2θ in 15 – 20◦ and 40 - 46◦ show high crystalline properties.
Data presented in Table 1.
The layered material can be evaluated using the lattice, the results
are presented in Table 1. In the hexagonal structure, the values of a and c
can be determined by equations (1) and (2):
[ (a)2 ] 1
1 4 ( 2 )
2
= h + k2 + hk + l2 (1)
dhkl 3 c a2

1 4 1 ( 2 ) 1
2
= h + k2 + hk + 2 (2)
dhkl .l2 3 a2 .l2 c
Based on the calculation, all samples have a c/a value of >4.89,
which proves the existence of a regular hexagonal layered structure. The
better the hexagonal ordering, the higher the c/a ratio [57]. In this case,
the highest c/a value was obtained by NMC-G 0 %, followed by NMC-G
7 %, NMC-G 4 %, and NMC-G 10 %. In addition, cation mixing may
occur due to a small amount of Ni2+ at the Li+ site. Cation mixing occurs
due to the presence of Ni2+ during phase formation, which has a nega­ Fig. 3. FTIR patterns of NMC-G in various graphene addition.
tive impact on the performance of the NMC cathode material. The
substitution of Li+ with Ni2+ causes blocking of the Li-ion pathway and distribution of NMC particles without significant agglomeration is
results in poor electrochemical performance. The higher the value of I clearly observed. The particle shape is like a regular polyhedron with a
(003)/I(104), the lower the cation mixing of the material [58]. The ideal smooth surface, implying high crystallinity of the material [63]. Fig. 4
cation mixing value is > 1.2, where NMC-G 7 % has the highest value (b), (c), and (d) show images of NMC material with graphene added with
[59]. This means that the level of cation mixing in NMC-G 7 % is lower 4 %, 7 %, and 10 % composition. With a magnification of 1000 times, we
than the other compositions, so it can produce the best cycling perfor­ can see flake particles which are graphene material [64] around the
mance when applied to lithium-ion batteries. The XRD pattern of gra­ NMC material, the more the amount of graphene added, the graphene
phene has a sharp peak at 25◦ [60]. Graphene diffraction peaks are also material attached to the NMC material is more clearly visible.
found, which can be observed in the XRD pattern of NMC-G with fairly To further visualize the morphology of graphene on the surface of
low peaks, indicating that graphene material envelops the NMC mate­ NMC, TEM testing was carried out, which is shown in Fig. 4e. Based on
rial. The greater the amount of graphene added, the higher the peak the test results, it is clear that NMC particles with graphene flakes are
formed. This shows that the surface treatment of graphene has an effect attached to the side of the NMC material surface. This shows that the
on the crystal structure [61]. However, in some previous studies it was graphene material is distributed on the surface of the NMC material.
also found that the addition of graphene did not affect the original Based on testing of this material, mixing the material with a simple solid-
crystal structure of pure NMC [25,49]. state method is able to mix the material evenly. However, the addition of
FTIR (Fourier Transform Infra-Red) testing is carried out to deter­ graphene with a simple solid-state method has not been able to make the
mine whether or not there are changes in the functional groups on the NMC material perfectly coated with graphene material. The addition of
cathode as a result of the addition of graphene material to the NMC conductive material to the material with a simple method is difficult to
cathode. The spectra of the FTIR sample test results are shown in Fig. 3. make the conductive material and binder able to envelop the active
With the addition of graphene to the NMC cathode material, the sharp material properly. To find out further effects in the form of electrodes,
peak at 760 cm− 1 is reduced, and the slope of the basin is sloping. This cross-section SEM testing was carried out on the resulting electrodes.
shows the increase of the C– –O bond between graphene material and The test results are shown in Fig. S3f for 2000x magnification and Fig. 4
NMC cathode material formed due to solid state mixing between gra­ (f and g) for 10000x magnification. Based on the test results of NMC-G 7
phene and NMC [62]. The greater the amount of graphene added, the % electrodes, graphene material is seen to stick and spread evenly on the
greater the change in the peak formed. This is predicted to be caused by surface of NMC material (Fig. 4g), which looks different from electrodes
the greater the amount of graphene added, the more bonds formed be­ that do not use graphene (NMC-G 0 %) which are still clearly visible
tween graphene and NMC particles. However, further research is still NMC particles (Fig. 4f). This shows that the effect of graphene addition
required regarding the atomic relationships that occur between particles can be observed quite clearly when it is already applied in the form of
that are bound together physically and chemically in a battery electrode. electrodes. Other methods offer better results of enveloping NMC ma­
To determine the morphology and size of the material, SEM and TEM terials with graphene. As in previous studies, the addition of graphene
testing was conducted. SEM images were taken with 1000 times by solution dispersion method can make the material well coated and
magnification. Fig. 4a shows an image of NMC material before the produce >70 % capacity stability up to 300 cycles and resistance up to
addition of graphene. From the figure, it can be observed that the NMC 10C current [65].Thus, in terms of morphological test results, the se­
particles are uniform and the NMC material grains are very clear. NMC lection of a simple solid-state method is seen to have disadvantages
particles with a size range of 1–20 μm are obtained. The uniform size compared to other methods. The performance of the active material can
be further enhanced by adding graphene with a large surface area to the
surface of NMC cathode. This will increase the area of contact of the
Table 1 electrolyte and the cathode material. Furthermore, during the dis­
The lattice parameter of NMC-G samples. charging and charging process, lithium storage on graphene sheets
Sample NMC-G 0 % NMC-G 4 % NMC-G 7 % NMC-G 10 % might lessen electrochemical polarization [55]. The active material’s
a (Å) 2.850 2.852 2.848 2.856 surface layer of conductive material serves as an electrical conductor
c (Å) 17.408 16.667 16.667 16.440 that ions can pass through, facilitating transfer process of the electron
c/a 6.108 5.843 5.852 5.756 [66]. Therefore, the NMC active material’s conductivity will rise if
I(003)/I(104) 1.826 1.906 1.939 1.836
graphene particles can cover its surface, improving battery performance

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R.B. Setyawati et al. Results in Engineering 21 (2024) 101651

Fig. 4. SEM and TEM test results: SEM morphology of the materials at magnification 1000 times of (a) NMC-G 0 %, (b NMC-G 4 %, (c) NMC-G 7 %, and (d) NMC-G
10 %; (e) TEM test results of the NMC-G 7 % material; SEM cross section test results of the electrode at magnification 10000 times for (f) NMC (NMC-G 0 %) cathode
and (g) NMC-G (NMC-G 7 %) cathode.

during cycles of charging and discharging. With the results obtained in graphite anode on 18650-type cylindrical cell. Fig. 5 shows the elec­
this study, the presence of graphene around the NMC material, which is trochemical test results of NMC-G materials with 0 % – 10 %wt graphene
quite evenly distributed, is expected to help improve electron transfer addition. NMC material with graphene addition using a simple direct
and result in better cathode performance [67]. mixing method with 7 % graphene addition produces the highest initial
specific capacity in this research, which is 158.1 mAh/g. Meanwhile,
NMC materials with the addition of 0 %, 4 %, and 10 % graphene pro­
3.2. Electrochemical analysis
duced initial specific capacities of 138.1, 141.6, and 145.7 mAh/g,
respectively. This research proves that NMC materials with the addition
Electrochemical analysis of the battery was performed by electro­
of conductive materials such as graphene can improve electrochemical
chemical impedance spectroscopy (EIS) test and charge and discharge
performance [55]. However, with the addition of 10 % by weight of
performance test, to test the battery capacity, rate capability, and cycle
graphene, the specific capacity decreases. This is because the more
capability test. The cathode film was prepared based on the mass
graphene added, the more it is possible to reduce the electrochemical
composition as presented in Table 2. The EIS test results are attached in
capacity during battery charge and discharge testing. The addition of too
Fig. S4 in the supporting information. The EIS test results provide
semicircular and straight-line plots showing that the NMC-G 7 % sample
has a very small Rct value indicating the high electrochemical perfor­
mance that can be produced by the NMC-G 7 % sample. Thus, the
addition of graphene with proper composition can reduce the imped­
ance efficiently.
To determine the electrochemical performance, NMC-Graphene
composite material was tested and applied as the cathode with

Table 2
The cathode’s material composition.
No Sample Composition of Material Mass ratio of NMC
to Graphene
NMC811 Graphene AB PVDF

1. NMC-G 0 0.94 0 0.01 0.05 1:0


%
2. NMC-G 4 0.90 0.04 0.01 0.05 1 : 0.04
%
3. NMC-G 7 0.87 0.07 0.01 0.05 1 : 0.08
%
4. NMC-G 0.84 0.10 0.01 0.05 1 : 0.12
Fig. 5. Specific initial discharge capacity test results of NMC-G in various
10 %
graphene addition.

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R.B. Setyawati et al. Results in Engineering 21 (2024) 101651

much graphene can also reduce the composition of the active cathode To test the battery cycle life, Fig. 7a shows the cycling ability test
material used. Whereas the amount of active material contained in the results of NMC material with 7 % graphene addition (NMC-G 7 %)
cathode will determine the capacity of the battery [68]. compared to NMC material without battery addition (NMC-G 0 %). The
The test results of the rate capability of NMC materials with the battery cell was tested with a charge current of 0.5C and a discharge
addition of graphene variations are shown in Fig. 6a. First, the battery current of 1C. Based on the test results, it was found that the addition of
cells are tested for variations in discharging current from 0.5C to 3C with graphene can improve the cycle stability of the battery. The retention
a constant charging current 0.5C to test the ability of the battery at capacity of NMC-G 7 % battery is 95.83 %, which is greater than that of
various discharging currents. In testing up to 3C current, there is a NMC-G 0 % battery, which is 92.27 % after 100 cycles. In addition, tests
decrease in specific capacity of 16.3 %, 14.06 %, 8.4 %, and 13.4 % from were also conducted on commercial batteries that have been produced
the first cycle capacity for graphene addition of 0 %, 4 %, 7 %, and 10 % on an industrial scale, shown in Fig. 7b. The commercial cylindrical
respectively. Then, the battery cells are tested for variations in charging battery used is type US18650VTC5 (Green) with a theoretical capacity of
current from 0.5C to 3C with a constant discharging current at 0.5C to 2600 mAh and a nominal voltage of 3.6V. The commercial battery
test the ability of the battery at various discharging currents. In testing showed a retention capacity of 73.75 % after testing for 1000 cycles,
up to 3C current, there is a decrease in specific capacity by 43 %, 18.5 %, lower than the NMC-G 7 % battery which was able to retain 81.32 % of
12.9 %, and 20.5 % from the first cycle capacity for graphene additions its first discharge capacity at the same current. Based on the test results,
of 0 %, 4 %, 7 %, and 10 %. After testing up to 3C current, the battery is the NMC-G 7 % battery, which is the result of this research in the lab­
returned to testing at 0.1C current as in the initial capacity test. Based on oratory, has a capacity that is able to compare with commercially pro­
the test results, the battery with 7 % graphene composition has the best duced batteries, which are automated in the production process and
capacity resistance with the ability to return the same capacity as the have minimal errors also minimal impurities, and even have comparable
initial capacity. These findings demonstrate that NMC materials cycle stability. This result can be said to be very good, and the NMC-G 7
including up to 7 % by weight of graphene have improved rate capa­ % battery is able to compete in the market if it will be produced on an
bility, while compositions containing up to 10 % of graphene perform industrial scale.
slightly worse than those containing 7 % graphene. The charge/ Further cycle tests were conducted on the NMC-G 7 % battery for
discharge curve profile for the NMC-G 7 % battery at each C-rate is 3500 cycles. The results of the cycling ability test are shown in Fig. 8.
shown in Fig. 6b. With the addition of graphene up to the optimum The results show that the cycle endurance of the NMC-G 7 % battery is
composition, the irreversible capacity loss is smaller than the NMC very good as there is still a capacity retention of 64.75 % after 3500
cathode without graphene addition [69]. Batteries with 7 % graphene cycles, which is influenced by the presence of 7 % graphene in the
composition have been shown to maintain their capacity up to 3C cur­ cathode. This can be attributed to the high conductivity of graphene
rent. This opens up opportunities for the battery to be used at higher material which is able to build an effective conductive network with
currents. Testing at higher currents will be discussed in the next section. NMC and conductive particles [70] and the uniform size of graphene
offers easier access for electrolyte ions into the electrode [71], short­
ening the diffusion length of lithium ions and accelerating the diffusion
of Li+ ions from/to the lithium insertion site in the NMC material [72].
Thus, the addition of graphene can improve cycle stability and thus
increase battery life.
Some of the studies that have been conducted regarding the addition
of graphene to the cathode of Li-ion batteries are shown in Table 3.
Compared to the existing studies, graphene addition using simple solid-
state mixing is the easiest method and possible to be used on an indus­
trial scale. By fabricating 18650 cylindrical cell batteries, the resulting
batteries have a fairly good capacity and good rate capability, which can
be compared with existing research. In terms of lifetime, the battery has
superior durability so that its cycling ability is very good. Therefore, the
use of a simple solid-state method with the ease of battery production
process through this method makes it possible to be carried out on a
large scale and produce good quality batteries.

3.3. Temperature stability analysis

Temperature testing is also carried out to test the safety of battery


operation because lithium-ion batteries can degrade at high tempera­
tures [73]. The performance, durability, and safety of lithium-ion bat­
teries are all greatly impacted by operating temperature [74,75]. The
results of temperature testing on batteries with and without the addition
of graphene are shown in Table S3 and Fig. S5. Test results with varia­
tions in discharge current show that the NMC-G 7 % battery temperature
produces a maximum operating temperature of 40.78 ◦ C at a current of
3C. While the NMC-G 0 % battery produces a maximum operating
temperature of 42.22 ◦ C. For charging current variations, the NMC-G 7
% battery temperature produces a maximum operating temperature of
40.78 ◦ C at 3C, while the NMC-G 0 % battery produces a maximum
operating temperature of 44.08 ◦ C at 3C current. Graphene can improve
battery performance in terms of operating temperature, increasing the
safety of the battery for use, according to these test results. In addition to
Fig. 6. Rate capability test results of (a) NMC-G in various graphene addition being safer, lower working temperatures can increase the specific ca­
and (b) NMC-G 7 % charge/discharge curves of each C-rate. pacity of reversible batteries. This is due to the fact that at high

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R.B. Setyawati et al. Results in Engineering 21 (2024) 101651

Fig. 7. Cycling ability test results at 0.5C charging current and 1C discharging current of (a) NMC-G 0 % and NMC-G 7 % for 100 cycles and (b) NMC-G 7 % and
commercial battery for 1000 cycles.

capacity stability and thermal stability in long cycles at high currents is


necessary [79], so that with the high quality of energy density, safety is
well maintained [80]. Further tests were conducted by operating the
NMC-G 7 % battery at high charging and discharging current operations
to determine its performance capabilities for fast charge and fast
discharge. Tests were conducted with a battery that has a discharge
formation capacity of 1260 mAh. Tests were done by operating the
battery at 5C charging and 5C discharging currents for 200 cycles. The
test results are shown in Fig. 9.
Based on the test results, the NMC-G 7 % battery is able to maintain
capacity well at high charge and discharge currents. During 200 cycles,
the battery capacity tends to be constant after being applied high cur­
rent, which is 5C for charge and 5C for discharge. With a charging
current of 5C and a discharging current of 5C, it can be said that the
current is quite high for battery applications, which supports fast
charging capabilities and can be fully charged for approximately 12 min.
The battery capacity becomes constant at around 900 mAh or still
operating at a stable 75 % of initial capacity. The capacity-drop after
Fig. 8. Cycling ability test results at 0.5C charging current and 1C discharging going through 200 cycles is 5.44 %. This capacity is relatively stable for
current of NMC-G 7 % for 3500 cycles. lithium-ion battery operation at large currents. This is proven by the
coulombic efficiency value shown by the red line which shows a rela­
temperatures, the presence of dissolved metals will then migrate to the tively constant value in the range of 100 %. The stable coulombic effi­
negative electrode surface, causing the SEI layer to continuously ciency value indicates the stability of ion transfer during the charging
reconstruct and discharge lithium [76], which decreases the reversible and discharging processes. With these test results, it can be concluded
specific capacity [77]. that the transfer of ions from the cathode and anode and the reverse
Lithium-ion batteries are required in various equipment that require occurs well. This shows that the presence of graphene on the NMC
large power and energy density, such as in electric vehicles. Therefore, cathode is able to improve the performance stability of lithium-ion
the ability to perform at high currents is one of the important criteria for batteries at high current usage. This shows that the presence of gra­
lithium ion batteries to be used optimally [78]. The ability to maintain phene on the NMC cathode is able to improve the stability of lithium-ion

Table 3
Summary of NMC-graphene cathode performances from previous studies.
Cathode material Methods Electro-chemical Initial Specific Retention Rate Performances Ref.
Testing Capacity (mAh/g) Capacity

NMC811-PTCDA/ Solid state Full cell (coin cell 194.1 (2.8–4.3 V) 92.8 % after 100 122 mAh/g at 10C (62 % initial [49]
Graphene CR2032) cycles capacity)
NMC811- graphene Grounding + ultrasonication Half cell (coin cell 212.9 (2.7–4.3 V) 92.2 % after 150 163.8 mAh/g at 5C (76 % initial [38]
nanosheet with ethanol CR2032) cycles capacity)
NMC811-graphene Mixed conducting interlayer Half cell (coin cell 184.9 (3.0–4.3 V) 94.3 % after 150 129 mAh/g at 10C (70 % initial [37]
CR2032) cycles capacity)
NMC811-CB/rGO Direct mixing method Half cell (coin cell 216.48 (2.5–4.5V) 85 % after 88 93.20 mAh/g at 3C (43 % initial [35]
CR2032) cycles capacity) and <50 mAh/g at 5C
NMC811-graphene Simple solid-state mixing 18650 cylindrical 158.1 (2.6–4.2 V) 95.83 % after 100 75 % initial capacity at 5C This
cell cycles study

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R.B. Setyawati et al. Results in Engineering 21 (2024) 101651

Fig. 9. Cycle life profile on fast charging and fast discharging currents (5C
charging current and discharging current).
Fig. 11. 200 cycle profile of battery temperature on fast charging and fast
battery performance at high current usage. discharging currents (5C charging current and discharging current).
In addition to its ability in capacity and performance stability, the
addition of graphene to the NMC cathode is proven to be able to improve temperature tends to decrease again in the resting and discharging
the operating temperature stability of lithium-ion batteries at high phases.
currents. Besides in terms of capacity, battery temperature testing at In continuous battery temperature testing for 200 cycles, shown in
high currents needs to be carried out because battery power can Fig. 11, the battery temperature tends to show a constant value between
decrease at high temperatures [81]. Temperature testing was conducted 36 and 46 ◦ C. The highest temperature peak is at 46.52 ◦ C. This tem­
during performance testing at 5C charging and 5C discharging currents. perature can still be said to be safe for the operation of lithium ion-based
The test results are shown in Figs. 10 and 11. batteries in the use of charging and discharging at high temperatures
Temperature is one of the important factors affecting the durability because the safe limit for thermal runaway is when the temperature
of lithium-ion batteries. LiPF6 salt which is commonly used as an elec­ reaches 60 ◦ C [84]. This result is good enough, considering that the
trolyte in lithium-ion based batteries will decompose at temperatures separator used is a PP separator that is already widely found on the
above 60 ◦ C, thus reducing battery life [78]. In addition, the degradation market, not the type of tri-layer PP/PE/PP separator that helps prevent
of all components in Li-ion battery including the effectiveness of the thermal runaway of lithium-ion batteries [85]. Further research using a
cathode and anode and the presence of side reactions that can occur tri-layer PP/PE/PP separator needs to be done to produce batteries with
faster in the presence of high temperatures are problems in the devel­ the best performance and a better level of safety. This result supports the
opment of fast charging technology [82]. ability of lithium-ion battery applications to be used in fast-charging and
Based on the test results, the NMC-G 7 % battery is able to maintain fast-discharging-based technologies that only require about 12 min for
temperature stability while operating at high currents. As can be seen each step. The results of this study show that lithium-ion batteries with
from Fig. 10, which depicts the temperature and capacity profiles during an NMC811-type cathode with graphene addition modification on the
the test with a charging and discharging current of 5 C for 1 cycle, the cathode with the right composition, which is 7 % (NMC-G 7 %), produce
temperature rises during the charging process and reaches a peak to­ batteries with good capacity, which are equipped with the ability to
wards the end of the charging phase. It can be predicted that the final maintain capacity stability and temperature stability in operations with
process of the charging phase is a phase that must be monitored at the high currents up to 5C in the charging and discharging process. It is
battery security to avoid the possibility of overheating which can be shown that a graphene-modified NMC811 cathode with a simple
dangerous and resulting a safety risk so that the design of the battery for solid-state method can produce a high-power, thermally stable
fast charging capability must be seriously considered [83]. Then the lithium-ion battery with fast charging capability. The ability of
graphene-modified NMC batteries can be one of the solutions to the need
for lithium ion-based batteries that require the ability to charge with
high currents.
Battery testing is carried out for actual applications in electronic
devices in addition to testing battery cell performance. The device used
for testing is an assembled propeller drone. This test is carried out
because the drone requires a large current to be able to move and fly
upward. The results and details of the test are presented in supporting
information Figs. S6, S7, S8, and Table S4. According to test results, the
battery with an NMC cathode enhanced with graphene can deliver good
performance. Thus, a battery with a graphene-modified NMC cathode is
proven to be capable of being used in electronic equipment that requires
high current. Because of this, the battery with a graphene-modified NMC
cathode performs well and maintains a stable temperature in both
single-cell testing and in actual use with electrical devices.
In this study, the use of a simple solid-state method is proven to be
able to produce lithium-ion batteries with superior performance. Based
on the results of material testing, electrochemical testing, and thermal
stability testing that have been carried out, the addition of conductive
Fig. 10. 1 cycle profile of battery temperature on fast charging and fast dis­ material in the form of graphene to the NMC811 cathode with the right
charging currents (5C charging current and discharging current).

8
R.B. Setyawati et al. Results in Engineering 21 (2024) 101651

composition is able to improve the ability of lithium-ion batteries for Data availability
real applications in various equipment. With a simple solid-state
method, the resulting cathode material is able to produce better per­ Data will be made available on request.
formance compared to the NMC cathode without the addition of gra­
phene material. This research method proves to be better than existing Acknowledgements
research, especially for use in large-scale production, which offers
convenience in terms of cathode preparation capable of producing high- This paper is supported by Penelitian Fundamental Regular (Grant
performance cathodes. Numbers : 1280.1/UN27.22/PT.01.03/2023) and UMG Idealab.

4. Conclusions Appendix A. Supplementary data

Today, battery technology is more important than ever. There is a Supplementary data to this article can be found online at https://doi.
demand for batteries with high energy density, high rate and cycle org/10.1016/j.rineng.2023.101651.
capability, and operational safety. Battery performance is significantly
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