The development of energy storage devices, like rechargeable batteries, is important to produce environmentally friendly products (Huang et al., 2019; Shaqsi et al., 2020; Li et al., 2021). Nowadays, electrochemical energy storage devices such as supercapacitors and photovoltaic cells are commonly used (Kandasamy et al., 2021; Agrawal et al., 2022). Supercapacitors exhibit a quick charge storage property, which may contribute to their reduced charging times, greater cyclability, and therefore higher specific capacitance (Purkait et al., 2018; Narthana et al., 2021; Rajagopal et al., 2022; Rawat et al., 2022). The ongoing research effects focus on the production of a low-cost, long-life cycle, and high-specific capacitance material for the development of supercapacitors (Iro et al., 2016; Tomy et al., 2021). The selection of appropriate electrode material is important to improve the supercapacitor performance. Numerous materials have been used to store charges for electrochemical energy storage devices (Mohammed et al., 2019; Santoro et al., 2019). The store charges in supercapacitor devices are classified into three types, electrostatic double-layer capacitors, pseudocapacitors, and hybrid supercapacitors (Mathis et al., 2019; Atta and Fahim, 2021; Volfkovich, 2021). The double layer formed at the electrode surface is used for the storage of charges in electrostatic double-layer capacitors. In pseudocapacitors, charge storage occurs through a redox reaction (Fleischmann et al., 2022; Kour et al., 2022).

Biomass-derived carbon sources have natural renewable resources and are widely used because they are affordable, readily available, simple to prepare, and ecologically beneficial. Some examples of biomass that may be used as a resource for activated carbon for electrochemical energy storage include coconut oil, bamboo fiber, bean dregs, mango leaves, peanut shells, etc., (Madhu et al., 2014; Ruan et al., 2014; Gaddam et al., 2016; Ji et al., 2018; Bai et al., 2020) In contrast, activated carbons frequently exhibit less capacitive characteristics, such as low conductivity and restricted charge flow rates. Activated carbon exhibits poor conductivity and limited charge storage capacity (Gomes Ferreira de Paula et al., 2019; Mohammed et al., 2019; Santoro et al., 2019; Luo et al., 2021). To overcome these difficulties, it is necessary to develop structural modifications as well as hybrid materials (Khandare and Late, 2017; Tomboc et al., 2020).

The Lemon Grass (Cymbopogon citratus) plant is known for its long leaves, which are specially used for making oil and spices. In Asian countries, Lemon Grass (LG) is used to provide taste and flavor to drinks (including tea, coffee, etc.). Among them, it has been utilized as a biofertilizer and feedstock. LG consists mostly of cellulose, which is considered to be a carbon source material with high potential (Liakos et al., 2016; Thota et al., 2018). The production of carbon and inorganic-based composites is a successful method for enhancing electrochemical energy storage by combining various inorganic materials, including transition metal oxides, and transition metal dichalcogenides, with carbon-based materials (Wang et al., 2020; Kour et al., 2022).

Molybdenum (Mo) has a variable oxidation state that can vary from +2 to +6. Molybdenum disulfide (MoS₂) has a layered structure that shows pseudocapacitive behaviour to obtain high specific capacitance (Cook et al., 2017). Mo has been stacked in between two sulfur atoms (S-Mo-S) by weak van der Waals forces, which allow the electrolyte ions to intercalate in MoS₂ (Kukkar et al., 2016). The ion diffusion works with MoS₂ to store the charge in its faradic capacitive nature, which helps to improve the chance of storing the charge (Mahmood et al., 2016).

In this work, we report the low-cost synthesis of MoS₂/Lemon Grass-derived carbon (MoS₂/LG-C) hybrid material for enhancing the electrochemical performance. In situ growth of MoS₂ nanobelts on surfaces of the LG-C through a facile redox reaction between ammonium molybdate and thiourea with carbon. The morphology and structural properties of LG-C and MoS₂/LG-C hybrid materials are examined. The electrochemical measurements performed with cyclic voltammetry, galvanostatic charge-discharge testing, and cyclic stability to obtain the superior charge storage capacity in supercapacitors are discussed.

The one-step hydrothermal method was used to produce the MoS₂/LG-C hybrid material. Figure 1 illustrates a schematic representation of the synthesis process of LG-C and MoS₂/LG-C. LG-C nanosheets were associated with the formation of MoS₂ nanobelts on the surfaces of LG-C. The structural information of MoS₂ and the LG carbon was carried out using Raman spectroscopy and XRD analysis. Figure 2A shows the Raman spectra of LG-C and MoS₂-LG-C. The two strong peaks appeared at about 1,344.3 and 1,592.8 cm⁻¹ identified to the D and G vibrational modes of LG-C. The D band is associated with defects and disorders induced in sp² carbon (Medhat et al., 2021). The Raman spectra of MoS₂/LG-C show the E¹ _2g and A_1g vibrational modes, which conform to the layered 2H-MoS₂ structure (Dinh et al., 2021). The peak observed at 376.2 and 404.4 cm⁻¹ shown in the inset of Figure 2A corresponds to the E¹ _2g and A_1g modes of vibration containing in-plane and the plane-symmetric modes of Mo and S. The MoS₂/LG-C Raman spectra revealed a shift in D and G vibrating modes occurring at 1,337.9 and 1,594.7 cm⁻¹ which can be related to the stress caused in LG-C by the growth of MoS₂ nanobelts. The intensity ratio of I_D to I_G is widely recognised to characterise the graphitization and amorphous nature of LG-C. In MoS₂/LG-C, it was observed that the I_D/IG ratio was approximately similar to 1:1 (Kishore et al., 2014). This indicates that higher disorder and more active sites in MoS₂ allowed for the formation of amorphous carbon and defective sites in MoS₂/LG-C (Yu et al., 2020).

Figure 2B shows the XRD patterns of the as-synthesized LG-C and MoS₂/LG-C hybrid materials. The diffraction peaks observed in MoS₂/LG-C at 2θ values of 14.4°, 39.2°, and 49.0° have indexed the planes (002), (103), and (105) respectively, corresponding to the 2H hexagonal phase of MoS₂ (JCPDS no. 37–1492). The pristine LG-C XRD pattern revealed two peaks at 26.0° and 42.7°. The broad XRD peak was obtained for the pristine LG-C, while in MoS₂/LG-C, these peaks were found to be slightly shifted to 25.8° and 41.9° due to the presence of MoS₂ on the surface of LG-C (Shapira and Zucker, 2022).

FESEM images were taken at different magnifications, consisting of the micro-as well as nano-size surface morphology of pristine LG-C before and after the formation of MoS₂. FESEM images of pristine LG-C, (Figures 3A–C) showed a thick sheet with a scattered layer appearance. LG-C sheets revealed a rough surface with the ordered stacking of the sheets. MoS₂ nanobelts distributed in the interlayer of the LG-C materials (Figures 3D–F) produce nanobelts-like morphology. MoS₂ has several precise nanobelts of sizes ranging from 2 to 3 μm in length with smooth and even surfaces.

Further, the surface morphology was investigated by TEM and HR-TEM images. The TEM images shown in Figures 4A–E further conform the size of nanobelts is not uniform, which varies from 90 to 190 nm. A clear dispersion of the MoS₂ nanobelts in the LG-C matrix can be seen. The HR-TEM image (Figure 4F) shows a lattice spacing of ∼0.18 nm, which corresponds to the (105) plane of the hexagonal crystal structure of MoS_2, which matches with the XRD results. The selected-area electron diffraction (SAED) pattern of the MoS₂/LG-C is shown in the inset of Figure 4F. SAED pattern exhibited the polycrystalline nature of MoS₂/LG-C hybrid material is revealed. Some of the prominent reflections (105) are shown in SAED. The elemental composition determined with the help of EDS analysis is given in (Supplementary Figure S1). The observed composition of Mo and S was found to close to the ideal conditions (1:2).

The XPS spectrum of the MoS₂/LG-C hybrid material is depicted in Figure 5. Figure 5A shows the survey scan for four peaks conforming to Mo 3d, S 2p, C 1s, and O 1s, suggesting that the MoS₂/LG-C hybrid material was successfully formed. Apart from them, the peaks were obtained at 186.0 and 253.4 eV called plasmon loss peaks of S and Mo respectively. These peaks occur may be a higher probability of losing a specified amount of energy as a result of the photoelectron’s interaction with other electrons (Stevie and Donley, 2020). The doublet obtained 394.8 and 412.6 eV corresponds to Mo 3p_3/2 and Mo 3p_½ respectively. The Mo 3d XPS resolution scan (Figure 5B) shows the two primary peaks were obtained at 228.6 and 231.7 eV, corresponding to Mo⁴⁺ 3d_5/2 and Mo⁴⁺ 3d_3/2, respectively (Feng et al., 2019). The peaks obtained at 232.6 eV and 236.2 eV correspond to Mo⁶⁺ 3d_5/2 and Mo⁶⁺ 3d_3/2, respectively. The existence of sulphur atom level 2s in the MoS₂/LG-C was linked to the peak at 225.7 eV (Xiong et al., 2015). Figure 5C shows the high-resolution S 2p XPS spectra, indicating the presence of peaks conforming to the S 2p_3/2 and S 2p_1/2 situated at 161.5 and 162.5 eV. The peak attributed to 168.9 eV could be the presence of the sulphate group (Gnanasekar et al., 2020). The C1s XPS spectra in Figure 5D revealed three major peaks with binding energies of about 284.3, 284.8, and 286.1, eV, corresponding to the functional groups C-C, C-C, and C-O, respectively (Ji et al., 2018).

In Figure 6, all CV and GCD measurements were carried out using a 3-electrode system. Figures 6A, B shows the CV curves of LG-C and MoS₂/LG-C in 1 M Li₂SO₄ at scan rates of 5, 10, 20, 50, and, 100 mV s⁻¹. The CV curve of the LG-C electrode (Figure 6A), shows an almost rectangular nature with no identifiable redox peaks in the operating voltage range of 0.0–1.0 V. The rectangular nature of the CV curve of LG-C exhibits ideal behavior, showing the electric double-layer capacitor (Luo et al., 2015). MoS₂/LG-C hybrid material in Figure 6B has a dome-like quasi-rectangular shape that exhibits both electric double-layer capacitor behaviour as well as Faradic pseudocapacitance behaviour (Xu et al., 2018). MoS₂ nanobelts distributed in the interlayer of the LG-C sheets increased the entire area of the CV as well as peak current density with improved conductivity, which helps facilitate ion transport towards the electrochemical charge storage (Gopalakrishnan et al., 2020; Mahajan et al., 2022).

Figures 6C, D show the GCD curves of LG-C and MoS₂/LG-C at current densities of 0.5, 1, 2, and 3 A g⁻¹ with the applied potential voltage between 0.0 and 1.0 V. The specific capacitance (Cs in F g⁻¹) was calculated at various current densities using the following Eq. 1 (Lin and Zhang, 2015): C s = I ∆ t m ∆ V (1) where I is the current density, ∆ V is the applied potential window, m is the active mass of the electrode, and ∆ t is discharge time.

The Cs of LG-C and MoS₂/LG-C calculate to be 30.5 F g⁻¹ and 77.5 F g⁻¹ at a current density of 0.5 A g⁻¹, respectively. MoS₂/LG-C helps to increase the specific capacitance value of the hybrid electrode material due to the synergistic effects of MoS₂ as a conducting material with LG-C. Mo⁴⁺ in MoS₂ supplied the more active sites for charge transfer in MoS₂/LG-C, which provided a more interactive area between MoS₂/LG-C and the electrolyte for ion diffusion and increased the discharge time (Feng et al., 2019). The comparative CV and GCD curves of LG-C and MoS2/LG-C are shown in Supplementary Figures S2A, B at a scan rate of 20 mV s⁻¹ and a current density of 0.5 A g⁻¹. Electrochemical charge storage is obtained due to ions present in an electrolyte (Li⁺) interaction through MoS₂ and carbon sheets.

Figure 7A illustrates the plot of C_s versus the different current densities. At higher current densities, C_s were found to decrease, which could be due to the reduction in various activities at the electrode surface. The capacitance improvement occurs due to the favourable synergistic effect of MoS₂ as an active-site hybrid material, which helps to avoid the stacking of LG-C sheets and increases the surface area of MoS₂/LG-C. The increased surface area provided the path for electrochemical charge transformation and helped store the energy in the supercapacitor (Bi et al., 2019). The comparative data of different composite nanostructure materials with MoS₂/LG-C in the literature related to Cs and various electrolytes are shown in Table 1. (Brousse et al., 2007; Aradilla et al., 2014; Ho et al., 2014; Masikhwa et al., 2017; Choi et al., 2020; Bello et al., 2022). The EIS measurements of LG-C and MoS₂/LG-C were performed to study the transportation of ions in electrolytes with their electrochemical properties, equivalent series resistance (R_s), and charge transfer resistance (R_ct) (Dulyaseree et al., 2017). Figure 7B shows the Nyquist plot of LG-C and MoS₂/LG-C hybrid materials with an imaginary axis performed at a frequency range of 0.1 MHz–100 mHz. LG-C and MoS₂/LG-C achieved similar series resistance (R_s) for supercapacitors of about 12.09 Ω and 6.26 Ω which shows the MoS₂/LG-C has good electrical conductivity. In the high-frequency region, a clear semicircle was not observed, which indicates it may have a low R_ct (Niaz et al., 2020). MoS₂/LG-C has increased the conductivity of hybrid material because MoS₂ provided a more active site for LG-C, which helps improve electrochemical properties. The cyclic stability of LG-C and MoS₂/LG-C (Figure 7C was carried out using a GCD test in 1M Li₂SO₄ electrolyte at the current density of 3 A g⁻¹. MoS₂/LG-C exhibited superior cyclic stability and, 71.6% capacitance retaliation, and only 28.4% capacity degradation occurs up to 3,000 cycles at a current density of 3 A g⁻¹. In LG-C, 46.2% of the capacitance was retained up to 3,000 cycles. In MoS₂/LGC hybrid materials, sulphur bonded with MoS₂ forms a layer that is collected on the carbon surface and connected to the carbon structure covalently, which helps to provide excellent cyclic stability. The abrupt decrease in capacity observed in cyclic stability plot due to the measurement might be related to active material dissolving in the electrolyte, as well as difficulties with electrodes which include expansion and active material loss owing to poor binding.

The electrochemical behaviour of the LG-C and MoS₂/LG-C hybrid nanomaterials were also studied by symmetric supercapacitor devices in 1M Li₂SO₄ electrolyte. The CV curves of LG-C and MoS₂/LG-C (Figures 8A, B) were measured at the potential window of 0.0–0.5 V at scan rates between 5 and 100 mVs⁻¹. All CV curves of LG-C have a quasi-rectangular shape, showing a good electric double-layer capacitor for fast ion transfer. While CV curves variations from an ideal rectangle with increasing the current density. The GCD measurements of LG-C and MoS₂/LG-C exhibit minor MoS₂/LG-C were carried out at different current densities are shown in Figures 8C, D, respectively. The charge-discharge durations of the MoS₂/LG-C hybrid material has longer than those of pure LG-C. The MoS₂/LG-C hybrid material has higher specific capacitance than pure LG-C. The specific capacitance values were calculated using Eq. 2 for symmetric supercapacitor devices. C s = 2 I ∆ t m ∆ V (2)

The MoS₂/LG-C hybrid material and LG-C show a specific capacitance of 59.2 F g⁻¹and 44.4 F g⁻¹, respectively at a current density of 1 A g⁻¹.

Furthermore, EIS measurements of MoS₂/LG-C hybrid material and LG-C (Figure 8E) were carried out in the frequency range of 100 kHz to 10 mHz. The Nyquist plot corresponding series resistance (R_s) and charge transfer resistance (R_ct) values of LG-C are 8.5 and 3.4 Ω respectively. In the MoS₂/LG-C Nyquist plot, Rs and R_ct were determined to be 6.6 and 2.2 Ω, respectively. The lower R_s value implies the internal resistance, electrolyte ionic resistance, and contact resistance of active electrode materials of the MoS₂/LG-C electrode is more conductive than the LG-C electrode. The R_ct may be ascribed to the MoS₂/LG-C electrode’s improved electron transportation and high surface area, which allows for quick redox reactions at the electrode/electrolyte interface.

The Ragone plot of LG-C and MoS₂/LG-C obtained at various current densities is depicted in Figure 8F. The relation between energy density (E in Wh kg⁻¹) and power density (P in W kg⁻¹) is an important parameter to examine energy devices. Energy density and power density are calculated from the following equations: 3 and 4, respectively (Raghu et al., 2018). E = 1 2   C s ∆ V 2 (3) P = E ∆ t (4)

The MoS₂/LG-C-based supercapacitor performance measured 273.2 W kg⁻¹ power density and 2.1 Wh kg⁻¹ energy density, whereas the LG-C sheets-based supercapacitor exhibited 234.7 W kg⁻¹ power density and 1.5 Wh kg⁻¹ energy density at a current density of 1 A g⁻¹. P and E were found to increase with increasing current density, and the maximum power density, 1,366.1 W kg⁻¹, and energy density, 1.3 Wh kg⁻¹ were obtained at a current density of 5 A g⁻¹ for MoS₂/LG-C symmetric device. The inset of Figure 8F shows the operating red light-emitting diode for symmetric supercapacitor devices.

In conclusion, we successfully synthesized the MoS₂ Nanobelts/LG-C nanohybrid structures by simple hydrothermal method. The low-cost and biodegradable LG leaves were used to form the nano-carbon by the pyrolysis method. The MoS₂ nanobelts help to provide pathways for ion transportation due to the interaction between active electrode materials and electrolytes. The specific capacitances of MoS₂/LG-C and LG-C were found to be 77.5 and 30.1 F g⁻¹, respectively, at a current density of 0.5 A g⁻¹. The cyclic stability of MoS₂/LG-C and LG-C was carried out by the GCD test, and 71.6% capacitance retention occurs up to 3,000 cycles at the current density of 3 A g⁻¹. The symmetric supercapacitor (MoS₂/LG-C//MoS₂/LG-C), the operating red light-emitting diode is illuminated. This method is favourable for the large-scale production of MoS₂/LGC as active electrode hybrid materials for electrochemical energy storage devices.