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01-13 

1 

 

 

 

Article 

Microstructured pebble stone like Ni-NiO 

composite as anode of high-performance lithium-

ion batteries 
Safina-E-Tahura Siddiqui1, Md. Arafat Rahman1*, Md. Saiful Islam2, Jin-Hyuk Kim3, Nirjhor 
Barua1 

1Department of Mechanical Engineering, Chittagong University of Engineering and Technology, Chittagong-4349,  

Bangladesh 
2Department of Glass and Ceramic Engineering, Bangladesh University of Engineering and Technology, Dhaka, Bangladesh  
3Clean Energy R&D Department, Korea Institute of Industrial Technology, 89 Yangdaegiro-gil, Ipjang-myeon, Seobuk-gu,  

Cheonan-si, Chungcheongnam-do, 31056, Republic of Korea 

               A R T I C L E   I N F O 
 

Article history: 
Received 10 September 2023  
Received in revised form 
14 October 2023 
Accepted 27 October 2023 
 
Keywords:  
Thermal oxidation, NiO, Composite, 
Anode, LIBs 
 
*Corresponding author 
Email address: 
arafat@cuet.ac.bd  
 
 
DOI: 10.55670/fpll.fusus.2.1.1 
 

A B S T R A C T 
 

Ni-NiO electrodes were synthesized via thermal oxidation of pure nickel 

powder and evaluated as anode of lithium-ion batteries (LIBs). The composite 

synthesized at 600˚C, 800˚C, and 1000˚C exhibited nanochips, crushed gravel 

stone, and pebble stone-like morphology, respectively. The nanochips- and 

crushed gravel stone featured-like electrodes exhibited erratic behavior, and 

specific capacity faded rapidly from 754.49 mAh g -1 and 101.12 mAh g-1 to 

464.04 mAh g-1 and 9.55 mAh g-1, respectively over 10th cycle at a current rate 

of 1C as the electrode experiences internal short circuit. The pebble stone-like 

Ni-NiO electrode exhibited improved and stable cyclic performance with 1 st 

discharge capacity of 365.17 mAh g-1 and reduced to 67.42 mAh g-1 even after 

40th cycle at 1C current rate. The improved electrochemical performance of 

composite Ni-NiO with a pebble stone-like feature can be attributed to the 

mechanical stability of the electrode, which can buffer volume expansion, and 

the presence of more nanoparticles on the electrode surface allows more 

interaction with Li+.  

 

1. Introduction 
Lithium-ion batteries (LIBs) have acquired immense 

attention and popularity as rechargeable batteries for 
portable consumer electronics applications due to high 
gravimetric and volumetric energy density, zero memory 

effect, and low self-discharge rate [1]. Besides consumer 
electronics, LIBs are being employed in aerospace, military 

applications, grid energy storage, electric vehicles (EV), 
hybrid electric vehicles (HEV), and plug-in hybrid electric 
vehicles (PHEV) [1–4]. The implication of these batteries is 

that they mitigate the environmental pollution resulting from 

the burning of fossil fuels [5]. It is noted that graphite is 

employed as an anode in commercial LIBs as it is inexpensive, 
has high reversibility during the charge/discharge process, 
and has excellent stability. However, its cycling capacity is 

restricted due to possessing low theoretical capacity (372 

mAh g-1) [6,7], which cannot fulfill the market demand for 

next-generation rechargeable LIBs. Moreover, graphite anode 
experiences extensive structural deterioration upon cycling 

that leads to drastic capacity fading; high polarization  
initiates lithium dendrite formation and low operating 
voltage [8]. From that quest, establishing a favorable anode 

material with high capacity, environmentally benign, and rate 
performance is very crucial to advancing the performance of 

LIBs [9–12]. In addition, pure alloys as LIB anodes face some 
issues, for instance, volume expansion and electrode 
fracturing during the lithiation process, which causes 

mechanical fracture of active electrode particles, resulting in 

electrical detachment and capacity fade and unstable SEI 

formation [13–15]. However, titanium-based oxides are 
investigated as the anode; it can eradicate the issues 
regarding alloy anodes with a long cycle life since it has no SEI 

and just a 1% volume change. Unfortunately, with a 1.5V 

versus Li/Li+ operating voltage, as well as a limiting specific 

Future Sustainability 

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February 2024| Volume 02 | Issue 01 | Pages 01-13 

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SET. Siddiqui et al. /Future Sustainability                                                                           February 2024| Volume 02 | Issue 01 | Pages 01-13 

2 

 

capacity of 160 Ah kg-1, the battery energy density is reduced 
[16]. Among all anode materials, Transition metal oxides 

(TMOs) are recognized as the most suitable anode materials 

for LIB due to their high theoretical capacity, natural 

affluence, eco-friendly nature, cost-effective fabrication 
procedure, and chemically durable [17–23]. Moreover, TMOs 
as anode material eliminate the problem of lithium dendrite 

formation, safety issues, and low specific capacity. It is noted 
that TMOs encounter some issues, such as rapid capacity 

depletion due to volume-induced strain during 
electrochemical cycling, resulting in intense polarization and 
electrode pulverization [24–27]. To address these issues, 

nanostructured TMOs are being employed because of their 
large electrode/electrolyte contact area, short diffusion 

length, and efficient strain accommodation [28,29]. NiO is a 
competitive candidate among other TMOs and is explored 
widely as an alternative electrode material for high-

performance LIBs due to its high theoretic capacity of 718 
mAh g-1, cost-effectiveness, environment benignity, and 

natural abundance [30]. The density of NiO is 6.81 g cm-3, 

which is three times higher as compared with graphite of 2.26 
g cm-3. The theoretical energy density of NiO is about 5.8 times 

higher than graphite [31]. Nevertheless, the practical 
application of NiO in LIBs is still obstructed because of its 

excessive volume variation and destruction of the active 

electrode material, as well as poor ionic conductivity, which 
results in poor electrochemical performance [32, 33]. To 

alleviate these issues, various morphologies of NiO are 
studied to analyze electrochemical performance, for instance, 

porous, mesoporous structures [36],  nanocomposite [31, 37, 
38], nanogravel [23], nanosheets [39, 40], nanowalls [41], 

nanofibers [42], hollow nanotubes [43], nanofilms [44], 

nanowires [45], hierarchical structures [46–50], nanocone 
array [51], composited with carbon [52–55] or conductive 

polymers [56,57] have been investigated, which in 
comparison to graphite and pure NiO exhibited improved 

electrochemical performance. In addition, several strategies 
such as hydrothermal, microwave hydrothermal, co-
precipitation, sol-gel method, pyrogenation, solvothermal, 

chemical emersion, spray pyrolysis, powder metallurgy and 
annealing is adopted to fabricate different NiO 

nanostructures [58,59]. Among these strategies, thermal 

oxidation of Ni powder is considered a facile and cost-
effective process, which can be adapted to synthesize unique 

morphological structures. Numerous investigations were 
carried out regarding electrochemical performance 

evaluation of NiO synthesized through thermal oxidation [31, 

51, 60, 61]. In some studies, NiO was combined with carbon 
to form composites, which exhibit excellent cycling stability 

[62–64]. However, the composite synthesis process is tedious 
and the existence of low-density carbon greatly reduces the 

volumetric specific capacity. In addition, the inclusion of high-
density metals can contribute to enhancing electrochemical 

performances [65,66]. Huang et al. prepared Ni-NiO 

nanocomposite through calcination in a tube furnace at 700⁰C 
[66]. The nanocomposite constitutes <10 nm of Ni particles 

and 100 nm of NiO particles. The enhanced electrochemical 
performance of electrodes due to the presence of the metallic 

Ni phase facilitates a more reversible reaction during the 

charging process. Comparatively, strong polarization was 
monitored owing to the presence of crystal defects. The rate 

capability and cycling performance were not satisfactory due 
to the slow kinetics of NiO particles and the transportation of 

electrons. Therefore, considerable research is required to be 

done to acquire stable cycling performance and rate 

capability of NiO as LIB anode material.  In this specific study, 
we synthesized microstructured composite of Ni-NiO through 
a single-step thermal oxidation process and mechanical ball 

milling. The composite structures were employed as anodes 
and provided efficient electrolyte access throughout the 

structure, which resulted in high discharge capacity and 
excellent cycling performance. In addition, the synthesized 
composite electrode exhibited different morphology at 

different oxidation temperatures. The presence of the 
metallic Ni phase facilitates the reverse decomposition  

process and improves electrical conductivity. It can be 
foreseen as a high-performance LIB electrode. 

2. Experimental 
2.1 Synthesis of Ni-NiO nanocomposite 

The composite Ni-NiO fabrication involves a single-step 

thermal oxidation process in an electric furnace (Nabertherm, 

USA) at three distinct temperatures, as shown in Figure 1.  

 

 

Figure 1. Schematic representation of Ni-NiO composite synthesis 
process 

 
Thermal oxidation is the method of growing a thin oxide 

layer on the surface of a wafer, which follows Wagner’s 

theory, as shown in Figure 2. The commercially available Ni 

powder (99.8% purity, maximum limit of impurities are Iron 

(Fe): 0.01%, Sulphur (S): 0.001%, Carbon (C): 0.08%, Oxygen 

(O): 0.15 %) of 20 gram was heated at 600⁰C, 800⁰C, and 

1000⁰C in the furnace for 2 hours. The oxidation of Ni powder 

was above 500⁰C [41,67]; hence, at the above temperatures, 

nickel was oxidized to NiO. The NiO film growth on the Ni 

powder surface was initiated via a step increase in the 

temperature of oxidation in the air. The samples were kept for 

day-long, and this cooling process was naturally inside the 

furnace after finishing the oxidation process. The product of 

thermal oxidation, a greenish NiO layer formed on the surface 

of Ni, which was mainly a chunk of Ni-NiO. The mass of the 

nickel powder before and after oxidation was measured using 

a precision electronic balance machine (SCIENTECH Inc., 



SET. Siddiqui et al. /Future Sustainability                                                                           February 2024| Volume 02 | Issue 01 | Pages 01-13 

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USA) with a readability of 0.001 mg. The chunk of Ni-NiO 

nanocomposite was ball-milled into the cylinder of the ball 

milling machine, which was filled with crushed oxidized 

particles and balls of two diameters in a 10:1 ratio. During the 

process of collision between balls and crushed particles, the 

particles got crushed, the size of the particles was reduced, 

and the ultimate composite powder of Ni-NiO was formed. 

The crushed particles were then strained to achieve a smooth 

and homogeneous composite powder.  

Figure 2. Schematic representation of the thermal oxidation process 

 

2.2 Characterization techniques 

An X-ray diffractometer (XRD) (Empyrean, PANalytical-

Netherlands) with radiation from the copper target (kα, 

λ=0.15406 nm) was used to evaluate the crystal structure and 

composition of the Ni-NiO crystal structure. The diffraction 

patterns were recorded over a 2θ range from 10 to 90⁰ at a 

step size of 0.1⁰. The morphology and structure of the 

nanocomposite Ni-NiO sample were examined using a high-

resolution scanning electron microscope (SEM) (JSM 7600F, 

JEOL-Japan) in combination with Energy Dispersive X-ray 

Spectroscopy (EDX) at 5 KV with different magnification.  

2.3 Electrochemical Measurements 
The synthesized and characterized nanostructured 

composites of Ni-NiO were employed as an anode of LIBs. The 

electrochemical performance of the synthesized anode was 

carried out by assembling the electrode into a CR2032-type 

coin cell (supplied by Xiamen TOB New Energy Technology 

Ltd., China) in the laboratory. The synthesized 

nanocomposites of Ni-NiO were used as working electrodes 

prepared through a slurry coating procedure, as shown in 

Figure 3. It is noted that the slurry constituted 70 wt. % of 

active material, 10 wt. % of polyvinylidene fluoride (PVDF) 

binder, and 20 wt. % of active carbon powder, which was 

dissolved in the required amount of N-methyl pyrrolidone 

(NMP) (Sigma-Aldrich). The prepared slurries were then 

pasted onto a copper foil (Changzhou DLX Alloy Co., Ltd., 

China). The counter electrode was recycled LiCoO2, and a 

porous polymeric separator of polyethylene was employed. 

The electrolyte was LiPF6 (supplied by Ximen Tmax Battery 

Equipment Ltd., China) of 1.0 M dissolved in ethylene 

carbonate (EC) and diethylene carbonate (DEC) at a volume 

ratio of 1:1. The assembled coin cells were crimped at 100 psi 

pressure using a hydraulic battery crimper (Metrology 

Laboratory, Dept. of ME, CUET). The galvanostatic 

charge/discharge tests were performed using a LAND-

CT2001A (LANDt Instrument, USA) battery testing system in 

a voltage range between 0.02 to 3 V at a 1C current rate.  

 

 

Figure 3. Schematic view of composite electrode preparation and 
coin cell assembly 

 

3. Results and Discussions 
3.1 Characterization of nanocomposite Ni-NiO as an 

anode of LIBs 

Figure 4 shows the XRD pattern of Ni-NiO 

nanocomposite at different oxidation temperatures, such as 

600̊ C, 800̊ C, and 1000 ̊C, respectively. To compare with the 

pure Ni, the XRD pattern of pure Ni is shown. The XRD pattern 

of pure Ni powder reveals that a face-centered cubic (FCC) 

structure with three main diffraction peaks at 44.54 ,̊ 51.92 ,̊ 

76.46  ̊corresponding to the (111), (200), and (202) miller 

indices of Ni (ICSD: 98-064-6085). The absence of any kind of 

impurity phases within the detection limit of the 

diffractometer confirms the purity of Ni powder. In addition, 

despite the oxidation of Ni at three distinct oxidation 

temperatures, no other diffraction peaks corresponding to 

the oxide phase are detected. It is noted that the XRD pattern 

of Ni shows high intensity and sharp peaks.  

 

Figure 4. XRD pattern of Ni-NiO composite after single-step thermal 
oxidation at 600˚C, 800˚C, and 1000˚C. 

 

 

 



SET. Siddiqui et al. /Future Sustainability                                                                           February 2024| Volume 02 | Issue 01 | Pages 01-13 

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At 600̊ C oxidation temperature, Ni (ICSD: 98-064-6092) 

exhibited three peaks at approximately the same 2θ angle 

with five additional diffraction peaks at 37.31 ,̊ 43.35 ,̊ 62.97 ,̊ 

75.49 ,̊ 79.51 ,̊ which reveals the formation of NiO (ICSD: 98-

002-8834). These peaks can be indexed to the (111), (200), 

(202), (311), and (222) diffraction planes. In addition, Ni 

(ICSD: 98-064-6089) and NiO (ICSD: 98-018-4918) peaks are 

observed with an increase in peak intensity of NiO and a 

decrease in diffraction peak of Ni due to the thermal oxidation 

of Ni powder at 800̊ C. It is noted that more oxidation of Ni 

with increasing temperature and the NiO peaks become sharp 

with temperature rise which indicates the degree of 

crystallinity increase of NiO particles. At the oxidation 

temperature of 1000̊ C, there are no obvious peaks of Ni, the 

diffraction peaks of NiO (ICSD: 98-018-4918) are observed 

with high intensity and sharp peaks, as shown in Figure 4. The 

major sharpening of peaks, mainly of 2θ = 37.31 ,̊ 43.35 ,̊ 

62.97  ̊indicates the increased degree of crystallization [68].  

The crystallographic parameters of Ni-NiO composite at 

different oxidation temperatures were determined by the 

Debey Scherrer equation,  

D= 0.94 λ / (βcosθ)                     (1)                                                                                                             

where D denotes the average dimension of crystallites, λ 

denotes the wavelength of X-ray, and β denotes the full width 

at half maximum of a reflation located at 2θ.  

The average crystal size of pure Ni before oxidation was 19.93 

nm, and after oxidation at 600⁰C and 800⁰C is 19.77 nm and 

18.13 nm, respectively. However, there is no visible Ni peak 

at the temperature of 1000̊ C. It is noted that, with the 

increase in oxidation temperature, the crystal size of Ni 

decreases. In contrast, five diffraction peaks of NiO at 600̊ C 

were found at 2θ = 37.31 ,̊ 43.35 ,̊ 62.97 ,̊ 75.49 ,̊ and 79.51  ̊

with an average crystal size of 17.13 nm while at 800̊ C and 

1000˚C, same five NiO peaks exhibited with average crystal 

size of 18.72 nm and 18.86 nm, respectively. Hence, the 

crystal size of NiO increases with an increase in oxidation 

temperature. The possible reason for the increasing 

crystallite size of NiO is due to oxidation, which leads to more 

NiO formation. A similar phenomenon was observed as the 

crystallite size of the metal oxides exhibited an increment 

with an increase in temperature until it achieved a constant 

crystal size [68].  Figure 5 shows the low- and high-

magnification images of Ni powder before and after oxidation 

at 600⁰C. The SEM of pure Ni, as shown in Figures 5 (a) and 

(b), revealed that the particles are spherical in shape as well 

as partially agglomerated and smooth, and there are spaces in 

between the particles. However, this powder was oxidized in 

the electric furnace at 600 ̊C continuously for 2 hours; the 

growth of oxide particles occurs in between the spaces 

because of the swelling of grains. A significantly different 

morphology was observed of Ni powder after oxidation in the 

furnace at 600 ̊C. The as-synthesized Ni-NiO composite 

showed a randomly ordered interconnected “nanochips” like 

structure, as shown in Figures 5 (c), (d), due to the formation 

of NiO in Ni powder. At a low oxidation temperature of 600 C̊, 

no obvious grain boundary was found, however, the oxide 

layer growth occurs due to oxidation. A rough surface was 

formed, which is seen in the high magnification SEM image of 

the surface, as shown in Figure 5 (d), due to oxide growth. The 

EDX spectrum confirms the presence of only the Ni phase 

before oxidation, both Ni and O phases after oxidation, as 

shown in Figures 5 (e) and (f).  

 
Figure 5. Low and high magnification SEM images and EDX spectra 
of Ni powder: (a), (b), (e) pure nickel powder, and (c), (d), (f) after 
oxidation at 600 ̊C 

 
Figure 6 shows low and high-magnification SEM 

images of nickel powder after oxidation at 800  ̊C and 1000 C̊ 

temperatures. At 800 ̊C oxidation temperature, the increased 

grain swelling causes the grain contact area to enlarge, which 

is responsible for the intergranular joint formation [69]. It is 

noted that the grains are bonded well as more NiO is formed 

when compared to the sample oxidized at 600  ̊C, and grain 

boundary is formed as shown in Figures 6 (a), (b). As the 

temperature of oxidation increases, more oxygen is diffused 

through the porosity of the sample [70,71]; hence, more NiO 

is formed in the structure. The surface exhibited a “crushed 

gravel stone” like morphology with a 0.855 μm average grain 

size. It is noted that there are some cracks and spaces in 

between the grains due to the diffusion of nickel as well as 

induced thermal stress. These kinds of cracks and spaces 

suggest that Li+ transportation could take place easily 

because of the access of electrolytes through them.  Figures 6 

(c) and (d) represent the low and high-magnification SEM 

images of nickel powder after oxidation at 1000 C̊ 

temperature. The grains are well interconnected with each 

other as the swelling of grains due to the oxidation process 

causes them to fill up the intergranular spaces. The high 

magnification image of the structure, as shown in Figure 6 (d) 

reveals that there are no visible pores or voids in the 



SET. Siddiqui et al. /Future Sustainability                                                                           February 2024| Volume 02 | Issue 01 | Pages 01-13 

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structure and it exhibits a “pebble stone” like feature with a 

mean diameter of 0.899 μm which is quite different from the 

other two oxidized samples. The generation of different 

thermal stress is the main reason for different morphology at 

different temperatures [72]. At 1000⁰C oxidation 

temperature, a visibly smooth surface is observed in the high 

magnification image, as shown in Figure 6 (d).  

 
Figure 6. Low and high magnification SEM images and EDX spectra 
of Ni powder: after oxidation at (a), (b), (e) at 800 ̊C, and (c), (d), (f) 
at 1000 ̊C 

 

The EDX spectra exhibited that there are both nickel (Ni) 

and oxygen (O) is present, which confirms the formation of 

the NiO phase in the synthesized composite structures. 

During EDX measurement different areas were focused, and 

the corresponding peaks are shown in Figures 6 (e) and (f). It 

is noted that every spectrum confirms the presence of the Ni 

and O phases. 

3.2 Electrochemical performance of Ni-NiO composite as 

anode of LIBs 
The electrochemical performances of synthesized Ni-NiO 

composites were evaluated to assess their efficiency as 

anodes for LIB. The performance evaluation was 

accomplished by comparing the galvanostatic charge-

discharge profile for different composite anodes to figure out 

the effect of oxidation temperature on the battery 

performance. In this study, three types of batteries are 

assembled employing three kinds of composite. These three 

batteries are assembled by exerting- microchips (600⁰C, B-1), 

crushed gravel-stone (800⁰C, B-2), and pebble stone (1000⁰C, 

B-3) structured negative electrodes. It is noted that NiO is a 

conversion reaction-based anode that captures lithium 

possessing high specific capacities by reversibly replacing 

redox reactions within Li+ and transition oxide-based cation. 

The elementary conversion reaction mechanism of NiO can be 

given as NiO + 2Li+ + 2e- ↔ Ni + Li2O. During the discharge 

phase, NiO is reduced to highly dispersed metallic Ni 

nanoparticles and Li2O. In addition, the disintegration of Li2O 

and the reformation of metallic Ni nanoparticles into NiO 

nanograins take place during the charge phase.  

3.2.1 Electrochemical performance of Ni-NiO 

composite at 600⁰C and 800⁰C as anode of LIBs  

The galvanostatic charge-discharge voltage profiles 

within a potential window of 0.01-3.0V versus Li+ with cyclic 

performance and coulombic efficiency for the B-1 and B-2 

batteries (synthesis temperature of 600⁰C and 800⁰C) at a 

current rate of 1C is shown in Figures 7 (a)-(d). It is noted that 

the 1C rate signifies the accomplishment of charge/discharge 

in an hour. For battery B-1, the 1st cycle charge-discharge 

capacity was observed to be 754.49 mAh g-1 and 464.04 mAh 

g-1 with 61.50% coulombic efficiency. In addition, the B-1 

battery delivered charge-discharge capacities of 23.59 mAh g-

1 and 11.79 mAh g-1; 10.11 mAh g-1, and 10.67 mAh g-1 at the 

5th and 10th cycles, respectively. The consecutive coulombic 

efficiencies were observed to be 52.5% and 95%, 

respectively. In contrast, the capacities were 101.12 mAh g-1 

and 79.78 mAh g-1, with a coulombic efficiency of 127.46%, for 

battery B-2. In addition, the battery B-2 exhibited 5th and 10th 

cycle charge-discharge capacities of 25.28 mAh g-1 and 28.09 

mAh g-1; 7.30 mAh g-1 and 9.55 mAh g-1, respectively. The 

coulombic efficiency was observed as 111.11% and 130.77%, 

respectively. It is noted that the capacity exhibited drastic 

decay with cycling as cycled both batteries. In addition, only 

2.29% of the initial discharge capacity was retained for B-1, 

whereas 11.97% was retained for B-2 after the 10th charge-

discharge cycle. However, the coulombic efficiency fluctuated 

and increased after the 10th charge-discharge cycle of both B-

1 and B-2 batteries. There are a number of reasons why 

columbic efficiency exceeds 100%, including an imbalance in 

the amounts of Li+ absorbed and released, side reactions, and 

measurement error. This may be due to some structural 

interruptions that cause an uneven volume of Li+ to be 

transported. Particularly, the intercalation of less Li+ during 

charging and the de-intercalation of the maximum volume of 

Li+ during discharging cause the columbic efficiency to 

exceed 100%. The repeated occurrence of such phenomena 

causes the active material to fail and affect the battery's 

performance adversely [73–75]. 

It is evident from Figures 7 (a) and (c) that battery B-1 

exhibited erratic behavior, and the specific capacities 

decreased rapidly from the 1st to 10th charge-discharge cycle. 

Moreover, the specific charge/discharge capacity faded 

drastically with further cycling, and the battery became out of 

order. The predominant reason behind this extreme capacity 

fading is the short-circuiting phenomenon of the battery, as 

the instantaneous voltage drop occurred from around 1.0 to 

0.01V [76,77]. The unanticipated voltage drop is due to the 

short circuit of the composite Ni-NiO electrodes and the 

recycled LiCoO2 electrode due to swelling or perforation of 

the insulating polymeric separator, deflection of electrodes, 

or presence of impurities in the cell [78]. The incident of the 



SET. Siddiqui et al. /Future Sustainability                                                                           February 2024| Volume 02 | Issue 01 | Pages 01-13 

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internal short circuit releases 70% of the battery energy 

within 60 seconds [79, 80], which causes a rigorous increase 

in the local temperature that, in turn triggers the chemical 

side reactions and causes thermal runaway [80]. This short-

circuiting tendency became more prominent with further 

cycling. Hence, long cycling may lead to thermal runway and 

irreparable cell damage. In contrast, for battery B-2 the 

charge/discharge curve exhibited improvement as compared 

to battery B-1 as shown in Figure 7(b). The curve portrayed 

capacitor-like profiles (no potential flat plateaus); however, a 

linear variation of the potential in correspondence to the 

lithium insertion/extraction. This occurrence indicated the 

pseudo-capacitive behavior, which signifies surface storage 

nature [81, 82]. The 1st cycle irreversible capacity loss of 

21.10% may be ascribed to the formation of a solid electrolyte 

interface (SEI) caused by the degradation of electrolytes. This 

irreversible capacity loss gradually dropped to 23.53% after 

the 10th cycle. The substantial capacity decrease from the 1st 

to the 10th cycle may be attributed to the structural collapse 

of the composite by large volume change during cycling, 

which pointed out the structural inefficiency of the battery. 

However, the battery capacity retention ability was higher 

than the previous battery, and therefore, the performance 

was not worth demonstrating. 

 

 

 

 

3.2.2 Electrochemical performance of Ni-NiO 

composite at 1000⁰C as anode of LIBs  

Figure 8 shows the galvanostatic charge/discharge 

voltage profiles of battery B-3 in a potential window of 0.01-

3.0V Vs. Li+. Interestingly, the initial discharge profile 

exhibited no obvious plateau region, similar to the typical 

capacitor-like curve where potential increases/decreases 

linearly with the lithium insertion/extraction [82]. This 

occurrence is attributed to the pseudo-capacitive behavior, 

which indicates the bulk surface storage characteristics [81, 

82]. The initial charge curve exhibits higher voltage with two 

sloping potential ranges at about 2.2 and 2.5V, respectively.  

The 1st cycle charge-discharge capacities were exhibited as 

292.13 and 365.17 mAh g-1, respectively. There was an 

irreversible capacity loss of 18.98% between 1st charge and 

discharge, which may be connected to the formation of solid 

electrolyte interface (SEI) and amorphous Li2O during the 

discharge process, due to the electrochemically driven 

electrolyte degradation. It is noted that both the SEI as well as 

Li2O are partially decomposed during the subsequent charge 

process. This irreversibility of SEI and Li2O formation-

decomposition is responsible for the decrease in the charge 

capacity. The aforementioned occurrence is observed in 

materials that obey the conversion reaction mechanism [33, 

67, 83, 84].  

 

 

 

 

Figure 7. (a, b) Charge-Discharge voltage profiles for 1st to 10th cycle; (c, d) Cycle performance and coulombic efficiency at 1C rate for 

battery B-1 and B-2 



SET. Siddiqui et al. /Future Sustainability                                                                           February 2024| Volume 02 | Issue 01 | Pages 01-13 

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In addition, the discharge capacities in the 5 th, 10th and 

20th cycles have appeared as 196.62 mAh g-1, 104.49 mAh g-1, 

and 95.50 mAh g-1 respectively with corresponding charge 

capacities were 162.92 mAh g-1, 123.59 mAh g-1, and 56.17 

mAh g-1. The capacities decreased rapidly over cycling and 

26.15% of the initial capacity was retained after the 20 th cycle 

for B-3. Moreover, the reversible discharge capacity loss for 

1st to 5th, 5th to 10th, 10th to 20th, 1st to 20th were 168.55 mAh 

g-1, 88.13 mAh g-1, 8.99 mAh g-1, and 269.67 mAh g-1, 

respectively. The average capacity loss per cycle was found to 

be 13.48 mAh g-1 and 26.15% of initial capacity was retained. 

The initial coulombic efficiency of battery B-3 seemed to be 

124.80% at a 1C rate. The coulombic efficiency fluctuated in a 

random manner throughout the 20 cycles and attained a 

value of 90.47% after the 20 th cycle. The aforementioned 

performance analysis of B-1, B-2, and B-3 batteries implied 

that all three batteries are functional and exhibited some 

capacities with coulombic efficiencies. The charge/discharge 

profile and cycle performance of B-1 and B-2 clearly indicated 

the infeasibility of the battery to be employed in practical 

application. The B-1 battery exhibited an error-prone 

tendency as an internal short circuit occurred, which was 

responsible for extreme capacity decay within a few cycles. 

This may be induced by perforation or crack in the separator, 

deformity in architecture, and/or defective assembly 

procedure. In the case of B-2 battery, low capacity resulted 

from conspicuous surface intercalation, which accounted for 

structural collapse. However, B-2 battery appeared to have a 

slight improvement in performance compared to B-1, the 

battery efficiency, which did not meet expectations. It is noted 

that the B-3 battery appeared to be a promising one. The B-3 

battery exhibited more efficient results than all other 

batteries, rather it requires high-temperature processing. 

This may be attributed to the well-ordered and highly 

crystalline microstructure. Hence, long-term cycling 

performance has been executed with B-3. As a consequence, 

more than 40 charge/discharge cycles can be achieved with 

B-3 at a 1C rate. 

 

 

Figure 9 exhibits the high cycle charge-discharge profiles for 

battery B-3 within the voltage window 0.01-3.0V Vs. Li+. The 

25th cycle charge-discharge capacities were 73.03 mAh g-1 and 

112.36 mAh g-1. Similarly, the 30th, 35th, and 40th discharge 

capacities were 98.88 mAh g-1, 75.84 mAh g-1, and 67.42 mAh 

g-1 respectively with corresponding charge capacities of 61.79 

mAh g-1, 46.63 mAh g-1, and 35.39 mAh g-1, respectively. A 

considerable discharge capacity loss was noticed 13.48 mAh 

g-1 from 25th to 30th cycle. For 30th to 35th, 35th to 40th, and 25th 

to 40th cycle the discrepancies in discharge capacity became 

23.04 mAh g-1, 8.42 mAh g-1, and 76.97 mAh g-1. The average 

loss in discharge capacity per cycle was 5.13 mAh g-1, which 

was 13.48 mAh g-1 for the first 20 cycles. It is noted that 

discharge capacity loss followed a decreasing trend with an 

increase in cycle number. Moreover, the battery 

demonstrated a long-cycle performance and coulombic 

efficiency at the 1C rate as shown in Figure 9 (a). The 

coulombic efficiency for the 25th cycle was 95.55%, and the 

values were 88%, 88.82%, and 100% for 30 th, 35th, and 40th 

cycles. The coulombic efficiency showed a subsequent 

decrease up to the 35th cycle and attained 100% in the 40 th 

cycle. Furthermore, the retention of initial capacity was 

18.46% after the 40th cycle, which was 27.07% and 20.77% 

for the 30th and 35th cycles. The long-term cycling caused only 

7.69% capacity decay from the 20 th to 40th cycle. It can be 

stated that the capacity retention ability manifested a 

decreasing tendency with cycling. In order to clarify the 

capacity loss of the as cycled batteries, the surface 

morphology and elemental analysis of the Ni-NiO composite 

electrode were performed. It is noted that disassemble of LIBs 

was performed manually in such a way that the process was 

not allowed to short-circuit. In addition, Ni-NiO electrode was 

not washed after disassembling of LIBs, and its original 

morphology after respective cycling was observed with the 

presence of an SEI layer. Figure 10 shows the SEM images and 

EDX spectra of Ni-NiO electrodes of batteries B-1 and B-3 

after charge/discharge for 10 and 40 cycles, respectively.  

 

Figure 8. (a) Charge-Discharge voltage profiles from 1st to 20th cycle; (b) Cycle performance and coulombic efficiency at 1C rate for battery B-3 



SET. Siddiqui et al. /Future Sustainability                                                                           February 2024| Volume 02 | Issue 01 | Pages 01-13 

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Figure 9. (a) Charge-Discharge voltage profiles from 25th to 40th cycle; (b) Long cycle performance and coulombic efficiency at 1C rate for battery B-3 

Figure 10. SEM and EDX characterization of Ni-NiO electrodes after electrochemical cycling of: (a, b) B-1 and (c, d) B-3 



SET. Siddiqui et al. /Future Sustainability                                                                           February 2024| Volume 02 | Issue 01 | Pages 01-13 

9 

 

It is noted that the synthesis temperature of electrodes of B-1 

and B-3 is 600oC and 1000 oC, respectively. We didn’t observe 

and analyze the SEM images and EDX spectra of the electrode 

of B-2, which was synthesized at 800oC due to the similar 

electrochemical performances of B-1. The initial 

microstructure of Ni-NiO electrode of B-1 enormously 

changed to agglomerated and cracked surface, as shown in 

Figure 10(a). It is noted that the width of some cracks 

increased and subsequently crushed due to the volume 

change of NiO and came off the current collector, leading to 

the drastic capacity fade of B-1. However, the original pebble 

stone microstructure of Ni-NiO electrode of B-3 entirely 

changed to a compressed honeycomb-like structure, as 

shown in Figure 10(c). It is noted that these both electrodes 

exhibited different morphology with few nanometer diameter 

pores after charge/discharge cycles at 1 C current rate. This 

could be attributed by the structural change during the first 

lithiation process when NiO structure converted to Ni 

nanoparticle inside Li2O and gel-like matrixes [17, 29, 85]. A 

similar morphological change is observed in NiO electrode as 

anode after the electrochemical cycling of LIBs [23, 78, 84]. It 

is noted that the decomposition of electrolyte is substantial, 

which can be another reason for the drastic capacity fading of 

Ni-NiO. The EDX spectra of Ni-NiO electrodes after 10 and 40 

charge/discharge cycles are shown in Figures 10 (b) and (d), 

respectively. It is observed that the presence of elements 

fluorine (F) and phosphorus (P) is due to the decomposition 

of LiPF6 along with the impurities elements of manganese 

(Mn), calcium (Ca), silicon (Si), and sulfur (S). In addition, 

carbon (C) is observed due to the decomposition of 

carbonate-based organic solvents. A similar decomposition 

phenomenon was observed in carbonate-based lithium salt 

electrolytes such as 1.2 M LiPF6/EC [86], 1 M LiPF6/EC-DEC 

[87], and 1 M LiPF6/EC-DEC-DMC [88]. From the above 

discussion, it can be noted that the B-3 has appeared as the 

propitious one among other batteries. It is noted that the 

synthesis required high-temperature (1000⁰C) processing; 

however, it exhibited noteworthy performance. The 

contribution of this specific research is to establish a 

convenient synthesis technique and undoubtedly unique 

architecture. In addition, the battery assembly operation was 

simple without any glovebox facility. The achieved capacity is 

lower than the NiO itself and other nanostructures; however, 

higher than the practical capacity of graphite anode. 

Moreover, replacing graphite with Ni-NiO composite will 

eliminate the safety issues regarding graphite anode with 

considerably high specific capacity. Furthermore, the 

remarkable performance stimulated the execution as a 

battery anode in practical application with no probable 

hazard.  

4. Conclusions 
In summary, we have fabricated microstructured 

composite of Ni-NiO through a simple and single-step thermal 
oxidation approach and subsequent mechanical ball milling 

process. At three distinct temperatures- 600˚C, 800˚C, and 

1000˚C oxidation of Ni powder was performed. The as-
synthesized microstructured composite of Ni-NiO was 

employed as an anode of LIBs, and the following conclusions 
are drawn from this study: 

• It was observed that the electrode synthesized at 600˚C (B-
1) delivered a discharge and charge capacity of 464.04 mAh 

g-1 and 754.49 mAh g-1 during 1st cycle which decreased 

drastically to 10.67 mAh g-1 and 10.11 mAh g-1 after 10th 
cycle at 1C rate. This electrode experiences an internal 

short circuit, which was the major reason behind the 
capacity fading. Moreover, the insufficient active 

nanoparticle loading in the electrode causes less reaction 
with lithium. However, the high elasticity of the electrode 

causes ease of electrolyte and ion access, and the 

brittleness of the electrode causes severe volume 
expansion and structural degradation of the electrode 

within 10 cycles.  

• The electrode synthesized at 800˚C (B-2) exhibited a 
specific discharge-charge capacity of 101.12 mAh g-1 and 

79.77 mAh g-1 during 1st cycle and faded rapidly to 9.55 

mAh g-1 and 7.30 mAh g-1 after the 10th cycle. Though 

irreversible capacity loss decreases from the previous 
electrode, the electrode cannot sustain long cycling. The 
more reversible capacity was due to the presence of Ni 

nanoparticles, possessing catalytic activity, facilitating the 

decomposition of Li2O and SEI layer during the charging 

process. However, the amount of active nanoparticles on 
the electrode increases with temperature increase, the 
electrode elasticity, and brittleness decrease, and the 

electrode was unable to buffer the volume-induced stress 
that resulted in the crack on the surface and structural 

degradation of the electrode.  

• One of the best electrochemical performances was 

observed in the electrode synthesized at 1000 C̊ 
temperature (B-3). The electrode delivered a specific 
discharge and charge capacity of 365.17 mAh g-1 and 

298.85 mAh g-1 during 1st cycle. A reversible capacity of 
67.41 mAh g-1 was achieved after the 40th cycle at a 1C rate. 

The discharge/charge capacity fluctuated randomly up to 
the 20th cycle as the electrode material became more 
ductile due to temperature increase, which impedes the 

smooth insertion of Li+. During continuous 
charging/discharging, the rapid lithium insertion/de-

insertion causes active electrode materials to get 

pulverized. After the 20th cycle, the electrode capacity 
fluctuated systematically and retained 18.46% initial 

capacity with coulombic efficiency of 100% after the 40 th 
cycle.  This may be due to continuous cycling; the structural 

reconstruction of the electrode causes a reduction in 

particle size of active material, and thus, nano-
crystallization improves the cycling performance. The 

prolonged cycling causes pulverization of the electrode, the 
active materials detached from the current collector, and 

the failure occurs.  

Ethical issue 

The authors are aware of and comply with best practices in 
publication ethics, specifically with regard to authorship 
(avoidance of guest authorship), dual submission, 
manipulation of figures, competing interests, and compliance 
with policies on research ethics. The authors adhere to 
publication requirements that the submitted work is original 
and has not been published elsewhere.  



SET. Siddiqui et al. /Future Sustainability                                                                           February 2024| Volume 02 | Issue 01 | Pages 01-13 

10 

 

Data availability statement 
The manuscript contains all the data. However, more data will 

be available upon request from the authors. 

Conflict of interest 

The authors declare no potential conflict of interest.  

Funding 

This work is co-supported by Chittagong University of 
Engineering & Technology (CUET), Bangladesh, through 

research grant no. CUET/CHSR-35/17(iii), University Grants 

Commission of Bangladesh-grant no. 37.01. 
0000.73.06.065.22.1607, and a grant (No. JB230001) from 

the Korea Institute of Industrial Technology (KITECH). The 
corresponding author is responsible for ensuring that the 

descriptions are accurate and agreed upon by all authors.  

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