Ti<sub>3</sub>C<sub>2</sub> MXene Nanosheets/Vanadium Nitride@Carbon Composite Electrodes for High-Performance Lithium-Ion Batteries

Nunna, Guru Prakash; Pitcheri, Rosaiah; Al-Asbahi, Bandar Ali; Sangaraju, Sambasivam; Khan, Baseem; Jo, Ko Tae

doi:https://doi.org/10.1155/2023/8091900

International Journal of Energy Research

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Abstract Introduction Results and Discussion Conclusion Data Availability Conflicts of Interest Authors’ Contributions Acknowledgments Supplementary Materials References Copyright Related Articles

Research Article | Open Access

Volume 2023 | Article ID 8091900 | https://doi.org/10.1155/2023/8091900

Ti₃C₂ MXene Nanosheets/Vanadium Nitride@Carbon Composite Electrodes for High-Performance Lithium-Ion Batteries

Guru Prakash Nunna,^1,2Rosaiah Pitcheri ,^1,3Bandar Ali Al-Asbahi,⁴Sambasivam Sangaraju,⁵Baseem Khan,⁶and Ko Tae Jo¹

Academic Editor: Ahmad Azmin Mohamad

Received25 May 2023

Revised17 Aug 2023

Accepted17 Oct 2023

Published31 Oct 2023

Abstract

Lithium-ion batteries have delivered outstanding charge storage performance due to their high energy density and low cost and also more specialized energy conversion device for next-generation electrical appliances. Herein, we offered the ultrathin Ti₃C₂ MXene (titanium carbide) nanosheets/vanadium nitride (VN)@carbon (C) nanocomposites for lithium-ion storage application as a high-capacity anode material. The proposed anode material is Ti₃C₂ MXene nanosheets/VN@C composite as synthesized via chemical precipitation. The real-time half-cell of Ti₃C₂ MXene nanosheets/VN@C composite shows the excellent initial discharge specific capacity of 1237 mAh g^-1 at a current density of 0.1 A g^-1 with a reverse rate capacity of 685 mAh g^-1. The high specific capacity of 645 mAh g^-1 has been attained even after 500 cycles at a current density of 0.1 A g^-1. This type of rich reverse rate capacity and stability of the anode electrode is responsible due to the high conductivities and surface areas of Ti₃C₂ MXene nanosheets/VN@C composite, which is provided easy accessibility of Li⁺ ions.

1. Introduction

Lithium-ion batteries (LIBs), being the most common electrochemical energy storage technology, are widely employed in electric cars and other portable devices [1–3]. To gratify the need for longer life, quicker charging, and long service life of energy storage devices, existing lithium-ion batteries must be improved urgently. Present days, graphite has been employed as an anode in commercial Li-ion batteries, but the working potential of graphite is low than the Li, which causes the creation of a solid electrolyte interface on graphite anode due to the breakdown of organic electrolyte, posing a safety risk and depleting active Li for electrochemical cycle process. Moreover, considerable research has been conducted on tin and silicon as anode materials as an alternative to graphite due to their greater energy densities [4]. Nevertheless, usage of these materials in practical applications of LIBs is limited because of the considerable volume changes during the cycling process, high irreversible capacity loss, and low cycling stability [5]. MXenes are transition metal carbides and nitrides that have been widely used as anode materials in electrochemical charge storage applications [6–8]. Among the other MXenes, Ti₃C₂ MXene offers several advantages over other MXenes in Li-ion battery anode applications. It has high theoretical specific capacity (~660 mAh g^-1) that can store a significant amount of lithium ions per unit mass, leading to higher energy storage capability and longer-lasting batteries. It also has some drawbacks, which are limited volume expansion, voltage window, and lower lithium storage capacity. It is worth noting that research and development efforts are continually addressing these disadvantages. Researchers are actively exploring strategies to mitigate volume expansion, widen voltage window, and enhance lithium storage capacity. Furthermore, combining MXene with other high-capacity materials as a LIB electrode not only reduces the self-stacking of MXene but also dramatically improves its high-rate capability and long-term stability [9–11].

Recently, metal nitrides such as TiN, MoN, and vanadium nitride (VN) have attracted attention due to their broad working potentials of 0.8-3 V, high specific power, and excellent electrical conductivity [12–14]. Among these, VN has garnered particular attention due to its diverse surface structures like nanotubes, nanobelts, nanowires, and a wide range of physicochemical properties, which suggest VN as an alternative anode material [15, 16]. Also, VN materials offer the potential to enhance the performance of LIBs due to their unique properties. Moreover, the combination of VN with 2D materials (like graphene, transition metal dichalcogenide materials, transition metal carbide materials, carbonatites, and nitrides) is of great attention for LIBs due to their larger surface area, higher theoretical capacitance, and better electrochemical behavior [17–19]. Particularly, the VN materials combined with Ti₃C₂ for Li-ion battery anode can offer several advantages due to the synergistic effects of their unique properties. These two-material combinations can enhance the specific capacity, rate capability, and cyclability due to its high lithium storage capacity, fast diffusion, and excellent electronic conductivity, respectively. The blend of Ti₃C₂ MXene and VN materials leverages their individual advantages, resulting in a synergistic effect that can significantly improve the performance of Li-ion battery anodes. This combination shows promise for achieving high energy density, fast charging, long cycle life, and improved overall battery performance. When Ti₃C₂ is composite with VN@C, several possibilities could contribute to overcoming the volume expansion. VN@C, with its unique structure and mechanical properties, can act as a mechanical support or scaffold for Ti₃C₂. This reinforcement can help accommodate the volume changes that occur during cycling, reducing the strain on the Ti₃C₂ layers and preventing their delamination or agglomeration. The lattice structure of VN@C could be compatible with Ti₃C₂, facilitating the accommodation of volume changes without inducing significant stress or distortion. VN@C, being a conductive material, can improve the overall electrical conductivity of the composite. This enhanced conductivity allows for efficient electron transport within the material, diminishing the occurrence of unwanted side reactions and enhancing the electrochemical performance of the Ti₃C₂. VN@C might possess excellent ion transport properties, promoting faster and more uniform ion diffusion within the composite material. This improved ion transport can mitigate concentration gradients and minimize the volume changes during lithiation and delithiation processes. This compatibility can maintain the structural integrity of both components during charge-discharge cycles. The combination of Ti₃C₂ and VN@C may result in a synergistic effect that enhances the electrochemical stability of the composite. VN@C could serve as a protective layer, preventing direct contact of Ti₃C₂ with the electrolyte and reducing the degradation of the Ti₃C₂ structure during repeated cycles. In addition, Ti₃C₂ nanosheets can provide quick electron transfer pathways and prevent the VN@C from aggregation. Carbon matrix could also significantly reduce volume expansion and stop structural deformation. More crucially, this structure can prevent Ti₃C₂ from being stacked again while still offering plenty of active sites for Li⁺ storage [20]. Based on abovementioned advantages of Ti₃C₂ MXene and VN materials, we concluded that the fabrication of Ti₃C₂ MXene-based VN anode materials for LIBs is familiar chosen for achieving the highest specific capacity along with electrochemical energy storage systems.

In the present study, Ti₃C₂ MXene nanosheets/VN@C composites are prepared using a facile chemical precipitation route. The structure, composition, and surface architecture of the synthesized materials are studied in detail. The optimized materials are used to prepare an anode, which is then employed in the design of Li-ion battery half-cell. The electrochemical characteristics such as specific capacity, rate capability, and cycling stability of the designed half-cell are studied.

2. Experimental Section

We purchased Ti₃C₂ from Sigma-Aldrich, and the synthesis of VN@C is described in Elsevier [16]. Detailed characteristics of VN@C are available in the supporting file (Figure S1 & S2). For the composite synthesis, we first mixed 40 mg of Ti₃C₂ powders in a DMSO solution and ultrasonicated it for 20 minutes. Then, we added 20 mg of VN@C () to the DMSO solution and stirred it for 2 hours. Finally, we washed the resulting material several times with water and ethanol before drying it at 80°C. The detailed experimental details have been given in supplementary information.

3. Results and Discussion

The physicochemical properties such as structural, phase crystalline, and chemical/electronic states were evaluated through powder XRD and XPS of as-prepared Ti₃C₂ MXene nanosheets/VN@C composite. Figure 1(a) illustrates the XRD pattern of Ti₃C₂ [21, 22], VN@C [23, 24], and Ti₃C₂ MXene nanosheets/VN@C composite. Herein, the strong characteristics planes of (002), (004), (006), (107), and (110) and (111), (200), (220), and (311) are well organized to the diffraction peaks of Ti₃C₂ (JCPDS no. #12-1272) [18] nanosheet and VN@C (JCPDS no. #35-0768) [19] nanobelt, respectively. The composite of Ti₃C₂ MXene nanosheets/VN@C clearly showed the formation of composite from this XRD pattern.

(a)

(b)

(c)

(d)

(e)

(f)

Figure 1(b) shows that the survey spectrum of as-synthesized Ti₃C₂ MXene nanosheets/VN@C composite, from this study, detected the presence of the following chemical states: Ti 2p, V2p, O1s, F1s, N1s, and C1s at respective binding energies. The existence of F and O in the Ti₃C₂ indicates the surface termination. The high-resolution Ti 2p spectrum consists of two chemical states of Ti 2p_3/2 and Ti 2p_1/2 located at their binding energies denoted as Ti-C (454.58 eV) and Ti-O (455.88 eV) for 2p_3/2 orbital states and Ti(II) (458.49 eV) and Ti-O (460.91 eV) for 2p_1/2 orbital states, respectively [25–27] as illustrated in Figure 1(c). The presence of Ti-O bonds indicates the partial surface oxidation, and Ti-C bonds come from the core level octahedral of Ti₃C₂ MXene [28, 29]. In addition, the C 1s spectra comprised of five deconvolution binding energies of Ti-C, C=N, C-C, C-O, and O-C=O/C-F are located to binding energies 281.23, 284.04, 285.21, 286.2, and 288.21 eV, respectively, which confirmed the formation of Ti₂C₃ (Figure 1(d)) [30]. The Ti-C bond reveals the interior atoms of Ti in the MXene layers, C-O bond indicates the oxidation of MXene, and the other bonds with C are carbon atom networks [31]. The high-resolution V 2p consists of two deconvoluted orbital states of V 2p_3/2 and V 2p_1/2 positioned at 515.2 and 521.4 eV, respectively, as displayed in Figure 1(e) [32]. The deconvoluted N 1s spectrum consists of three constitute binding energies V-N, N-C, and N-O located at 396.4, 399.7, and 403.6 eV, respectively [33] which confirmed the formation of Ti₂C₃ MXene/VN@C composite as presented in Figure 1(f).

The different magnification SEM images are displayed in the ultrathin Ti₃C₂/MXene nanosheets as depicted in Figure 2(a) (i, ii, and iii). Figure 2(b) (i, ii, and iii) SEM images show the nanosheet with nanobelt of Ti₃C₂/VN@C nanocomposites; it may be the influence of vanadium nitride. The EDS mapping spectrum indicates the presence of titanium, carbon, vanadium, and nitride elements of as-prepared Ti₃C₂/VN@C nanocomposites as shown in Figure 2(c) (i, ii, iii, iv, and v). The specific morphological influences of VN on ultrathin Ti₃C₂ MXene nanosheets can control the nanosheet size and shape, crystal structure, surface area, and interfacial properties. The introduction of VN can result in the decoration or coating of Ti₃C₂ MXene nanosheet surfaces with VN nanoparticles or thin layers. This surface modification can alter the surface energy, or chemical reactivity of Ti₃C₂ MXene nanosheets. It may also provide additional active sites for electrochemical reactions, leading to improve the storage capacity. The addition of VN can introduce the mechanical reinforcement, roughness, or surface irregularities, affecting the specific surface area and promoting better electrode-electrolyte interactions.

(a)

(b)

(c)

Figure 3(a) depicts the N₂ adsorption/desorption isotherms of Ti₃C₂ MXene and Ti₃C₂/VN@C, which displays the surface area 3.09 and 12.39 m² g^-1, respectively. The pore size distribution of Ti₃C₂/VN@C is 42.12 nm which is higher than that of Ti₃C₂ MXene (17.04 nm), and the pore volume of the Ti₃C₂/VN@C is 0.0754 m³ g^-1 which is much higher than that of Ti₃C₂ MXene (0.0196 m³ g^-1). The increased pore volume significantly reduces volumetric expansion during the Li-ion insertion/deinsertion mechanism. The internal morphology and d-spacing of crystalline were taken by HR-TEM and SEAD of as-prepared Ti₃C₂/VN@C composite as demonstrated in Figure 4. The HR-TEM images identified the presence of vanadium nitrite nanobelts over Ti₃C₂ nanosheets of 2D multilayered structure as illustrated in Figures 4(a) and 4(b). The high-resolution TEM images displayed the interplaner distance of vanadium nitride as ~0.206 nm (Figure 3(c)). Continuously, the SEAD pattern shows the lattice fringes which could be attributed to the formation of crystal planes for the Ti₃C₂/VN@C composite.

(a)

(b)

The interconnected conductive network of ultrathin Ti₃C₂ nanosheets anchored with VN@C nanobelts could exhibit brilliant lithium-ion storage performance. Subsequently, the energy storage behavior was recorded using a CR2032 coin cell setup with 1 M LiPF₆ electrolyte, following the arrangement illustrated in Figure 5(a). Figures 5(b) and 5(c) display the 1^st and 2^nd and continue with 50^th cyclic voltammetry profile of Ti₃C₂ and Ti₃C₂/VN@C electrode with the potential windows 0.01 to 3.0 V at 1 mV s^-1 scan rate (vs. Li/Li⁺). The first lithiation process in the pure Ti₃C₂ MXene (Figure 5(b)) exhibits large irreversible reduction peaks at around 0.7 and 1.25 V, which subsequently vanish in subsequent cycles. The primary cause of this phenomenon can be attributed to the development of a solid electrolyte interface (SEI) resulting from the interaction between Ti₃C₂ and Li-ions [9]. The observed reversible peak at around 1.5 V may be attributed to the reaction between Li⁺ ions and the titanium-based molecule. In the case of Ti₃C₂/VN@C (Figure 5(c)), the SEI layer is significantly reduced, potentially due to synergistic effects arising from the combination of Ti₃C₂ and VN@C in the composite. VN@C serves as a protecting layer, effectively preventing direct contact of Ti₃C₂ with the electrolyte. This can reduce the degradation of Ti₃C₂ during repeated cycling and result in a more stable and thinner SEI layer. Also, VN@C, being a conductive material, can improve the overall electrochemical stability of the composite. This enhanced stability can lead to reduced side reactions and a more controlled SEI layer formation on the Ti₃C₂ anode. One oxidation and two reduction peaks can be detected during the 1^st cycle of lithium intercalation-deintercalation. From this lithiation process, the oxidative peaking was positioned at 2.25 V, and a reduction peak was observed at 1.7 V and 1.1 V, respectively, which can be attributed to the lithiation/delithiation of Ti₃C₂/VN@C nanocomposite. It should be measured that, in the consequent cycles, the shapes of CV curves are retained until the 50^th cycle. Moreover, through the anodic process, oxidative peak at 2.25 V, as well as 1.7 V and 1.1 V, can be ascribed to the reduction peaks for lithiation/delithiation of Ti₃C₂/VN@C nanocomposite. Consider that the reductive peaks at 1.7 and 1.1 V remain practically unaffected in intensity and position after the first scan, demonstrating the stability and high electrochemical activity of Ti₃C₂/VN@C nanocomposite. The electrochemical interaction between Li-ions and Ti₃C₂ can be regarded as the following equation [34]:

(a)

(b)

(c)

(d)

(e)

(f)

(g)

(h)

(i)

Figure 5

(a) Schematic of Ti₃C₂/VN@C half-cell, (b) Ti₃C₂ cyclic voltammetry curves at 1 mV s^-1 (50 cycles), (c) Ti₃C₂/VN@C cyclic voltammetry curves at 1 mV s^-1 (50 cycles), (d) Ti₃C₂ charge-discharge profiles at various current densities, (e) Ti₃C₂/VN@C charge-discharge profiles at various current densities, (f) rate performance of Ti₃C₂ and Ti₃C₂/VN@C anode, (g) long cycling and Coulombic efficiency of Ti₃C₂ and Ti₃C₂/VN@C anode at 0.1 A g^-1, (h) electrochemical impedance spectroscopy of Ti₃C₂ and Ti₃C₂/VN@C anode, and (i) relationship between and in the low frequency for Ti₃C₂ and Ti₃C₂/VN@C samples.

Likewise, Figure 5(d) displays the charge/discharge potential profile for Ti₃C₂ MXene at various current densities from 0.1 to 1 A g^-1. First discharge capacity is Ti₃C₂ MXene 721 mAh g^-1 at a current density of 0.1 A g^-1 and after that decreased to 246 mAh g^-1. Further, the obtained specific capacities are 165, 140, 130, 123, and 98 mAh g^-1 at 0.2, 0.3, 0.4, 0.5, and 1 A g^-1 current densities, respectively. Figure 5(e) represents the as-prepared charge/discharge curves of Ti₃C₂/VN@C nanocomposite at various current densities. The first discharge capacity of Ti₃C₂/VN@C is 1237 mAh g^-1 at 0.1 A g^-1 current density and further reduced to a high capacity of 763 mAh g^-1. The charge/discharge curves were measured at different current densities of 0.2, 0.3, 0.4, 0.5, and 1 A g^-1, and the obtained specific capacities of 623, 575, 517, 501, and 436 mAh g^-1, respectively (Figure 5(e)). Moreover, Figure 5(f) shows the rate capacity of the as-prepared Ti₃C₂ MXene and Ti₃C₂/VN@C nanocomposite at different current rates and the obtained high reverse rate capacity of 685 mAh g^-1 at 0.1 A g^-1 current density for Ti₃C₂/VN@C electrode. Equally, the long-term electrochemical stability was recorded for the Ti₃C₂ MXene and Ti₃C₂/VN@C anode electrodes at 0.1 A g^-1 constant current density over 500 cycles, as displayed in Figure 5(g). Moreover, the Ti₃C₂/VN@C anode delivered a 93% of capacity retention even after 500 cycles, which is higher than that of Ti₃C₂ electrode with coulombic efficiency of ~100%.

The electrical conductivity test was detected through the electrochemical impedance spectroscopy (EIS) technique (Figure 5(h)). We observed a semicircle in the high-frequency area and a linear spectrum in the low-frequency region from this Nyquist plot. The Ti₃C₂/VN@C anode electrode shows the lesser charge-transfer resistance () is ~21 Ω, when compared to the Ti₃C₂ electrode as shown in Figure 5(h). Figure 5(i) presents an equation for calculating the lithium-ion diffusion coefficient [10]:

The equation involves variables such as gas constant (), absolute temperature (), electrode surface area (), number of transfer electrons (), Faraday’s constant (), lithium-ion concentration (), and Warburg impedance coefficient (). To obtain the value of , one can calculate the slope of the lines between and in the low frequency region. The calculated values of lithium-ion diffusion coefficients () of the Ti₃C₂ MXene and Ti₃C₂/VN@C electrodes were and cm² s^-1, respectively. The outstanding results may be due to the 2D structure and an inadequate surface area of Ti₂C₃ MXene [21, 22].

Recently, Tariq et al. prepared Ti₃C₂-TiO₂ nanocomposite via hydrolysis processes and exhibited the highest discharge capacity of 200 mAh g^-1 [35]. Liu et al. synthesized VO₂-NTs/Ti₃C₂ anode material via hydrothermal/ultrasonication and achieved a high specific capacity of 1425 mAh g^-1 [36]. The detailed comparison of recent works with current work is given in Table 1 [30–35]. In the present study, excellent electrochemical outcomes of the Ti₃C₂/VN@C nanocomposite for Li-ion battery anode have been ascribed to good interaction between VN nanobelts and Ti₃C₂ MXene. Especially, the VN nanocrystals confined into the Ti₃C₂ interlayer greatly increases the surface-active sites. The charge transfer resistance has been minimized in the Ti₃C₂/VN@C nanocomposite due to their good dispersion of VN nanobelts providing fast electron transfer during the charge/discharge process. However, the Ti₃C₂/VN@C nanocomposite provided a high reversible rate capacity and long cycling stability enabling the competition for the good anode electrode candidate for the high-power Li-ion battery applications.

4. Conclusion

In summary, we successfully designed a high-capacity anode material for Ti₃C₂/VN@C nanocomposite for LIBs. The suggested anode material is Ti₃C₂ MXene nanosheets/VN@C nanobelt composite as-synthesized via chemical precipitation. The half-cell of Ti₃C₂ MXene nanosheets/VN@C composite electroactive material shows brilliant charge storage performance with a high initial capacity of 1237 mAh g^-1 at a current density of 0.1 A g^-1 with high reverse rate capacity of 685 mAh g^-1. Moreover, it exhibited high cycling stability retention even after 500 cycles. The Ti₃C₂ MXene nanosheets/VN@C composite shows the highest capacity due to their high surface area; diffusivity enables the high insertion/deinsertion of Li⁺ when compared to the Ti₃C₂ MXene. These results revealed that the Ti₃C₂ MXene nanosheets/VN@C composite conductive network is a good competitor for the Li-ion battery anode. Furthermore, this novel research work is the base for the future development of MXene-based composites for lithium-ion batteries in electronic applications.

Data Availability

Data will be available on request.

Conflicts of Interest

The authors declare that they have no conflict of interest.

Authors’ Contributions

GPN was responsible for the conceptualization and wrote the original draft. RP was responsible for the methodology and data acquisition. BA was responsible for the data acquisition and wrote, reviewed, and edited the manuscript. SS was responsible for the preparation and data acquisition. BK and KTJ were responsible for the conceptualization and wrote and edited the manuscript.

Acknowledgments

One of the authors (Bandar Ali Al-Asbahi) acknowledges the Researchers Supporting Project (number RSP2023R348), King Saud University, Riyadh, Saudi Arabia. The authors thank the Core Research Support Center for Natural Products and Medical Materials (CRCNM) for the technical support regarding micro-Raman spectrophotometric and Brunauer-Emmett-Teller (BET) and Barrett-Joyner-Halenda (BJH) calculation analyses.

Supplementary Materials

Supplementary data includes the detailed experimental procedure. Figure S1: Raman spectrum of VN@C. Figure S2: (a) SEM images of VN@C, (b) TEM image of VN@C, (c) HR-TEM image of VN@C (inset SAED pattern), and (d–g) EDS and mapping images of V, N, and C. (Supplementary Materials)

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Copyright © 2023 Guru Prakash Nunna et al. This is an open access article distributed under the Creative Commons Attribution License, which permits unrestricted use, distribution, and reproduction in any medium, provided the original work is properly cited.

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International Journal of Energy Research

Ti3C2 MXene Nanosheets/Vanadium Nitride@Carbon Composite Electrodes for High-Performance Lithium-Ion Batteries

Abstract

1. Introduction

2. Experimental Section

3. Results and Discussion

4. Conclusion

Data Availability

Conflicts of Interest

Authors’ Contributions

Acknowledgments

Supplementary Materials

References

Copyright

Ti₃C₂ MXene Nanosheets/Vanadium Nitride@Carbon Composite Electrodes for High-Performance Lithium-Ion Batteries