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Three-dimensional MoS2/Graphene Aerogel as Binder-free Electrode for Li-ion Battery


Hybrid MoS2/reduced graphene aerogels with rich micro-pore are fabricated through a hydrothermal method, followed by freeze-drying and annealing treatment. The porous structure could act as an electrode directly, free of binder and conductive agent, which promotes an improved electron transfer, and provides a 3D network for an enhanced ion transport, thus leading to an increased capacity and stable long cycle stability performance. Notably, the specific capacity of MoS2/reduced graphene aerogel is 1041 mA h g−1 at 100 mA g−1. Moreover, reversible capacities of 667 mA h g−1 with 58.6% capacity retention are kept after 100 cycles. The outstanding performance is beneficial from the synergistic effect of the MoS2 nanostructure and graphene conductive network, as well as the binder-free design. These results provide a route to integrate transition-metal-dichalcogenides with graphene to fabricate composites with rich micro-pores and a three-dimensional network for energy storage devices.


Nowadays, the rapid development of electric vehicles and flexible electronics opens up an opportunity for the development of energy storage devices in the industrial and research communities [1, 2]. Among the various energy storage devices, lithium ion batteries (LIBs) are paid more attention due to their outstanding energy storage capability as well as long cycle life [3,4,5].

Recently, many researches have focused on high-performance anode materials for LIBs. 2D transition metal dichalcogenides (TMDs), with outstanding electrochemical performance, have won much attention and showed great potential as anode materials for LIBs [6, 7]. Comparing with conventional metal oxides, the metal sulfides with higher conductivity and larger interlayer spacing promote an improved electron transfer and enhanced ion transport [8]. Among the metal sulfides, molybdenum disulfide (MoS2) shows great advantages as the anode of LIBs due to its unique layered structure and high capacity (ca. 670 mAh g−1). However, its structure is prone to deteriorate during the charge/discharge process due to volume change, leading to a poor cycling stability. Numerous attempts have been conducted to enhance kinetic behaviors of MoS2 as LIBs anode. One method is to synthesis nano-size structure, in order to shorten the diffusion distance of lithium ions [9, 10]. Another method is to incorporate carbon materials to improve the composite conductivity and repress the volume expansion during charge/discharge process [11,12,13]. Different carbon materials [14,15,16,17,18,19,20], including carbon nanotubes [18] and graphene [19, 20], are used to integrate with MoS2 and it proves to be in effect. Especially, graphene has drawn much attention benefiting from its outstanding conductivity and high surface area. Recently, graphene has been widely researched in many areas, such as conductive switching [21], photoluminescence [22], chemical cleaning [23], and gas sensing [24] as well as energy storage fields [25]. For instance, Teng et al. prepared MoS2 nanosheets on graphene sheets, and a capacity of 1077 mAh g−1 at 100 mA g−1 after 150 cycles was obtained [26]. Liu et al. fabricated a composite of MoS2 and graphene [27], and the reversible capacity of 1300–1400 mAh g−1 was obtained. How to incorporate graphene with MoS2 to obtain the high-capacity and stable anode material is still an ongoing task [11].

Herein, a facile and low-cost approach is used to prepare a hierarchical nanostructure of MoS2/reduced graphene (MoS2/RGO) aerogel. With a solvothermal and freezing-drying process, the MoS2/RGO aerogel is fabricated and directly acts as the binder-free anode. Such a structure endows the MoS2/graphene aerogel with several advantages as an anode material. First, the graphene acts as a matrix to support the MoS2 nanostructures, which is beneficial to preventing graphene sheets from restacking. Second, the hierarchical nanostructure provides a good adhesion between graphene and MoS2, which ensure a stable structure and thus guarantee a long cycling stability. Third, the graphene with high conductivity promotes an improved electron transfer and acts as a basis to alleviate volume expansion of MoS2 in the charge/discharge process. Fourth, such a binder-free design shortens the ion diffusion distance, leading to an enhanced ion transport. The reversible capacity of the as-prepared binder-free MoS2/RGO aerogel is up to 667 mA h g−1 at 100 mA g−1 after 100 cycles. This method provides a route to fabricate the high-performance lithium-ion anode material.

Materials and Methods

Synthesis of MoS2/RGO Aerogels

All reagents were of analytical grade. A modified Hummers’ method was used to prepare graphene oxide (GO) for further use [28]. The MoS2/RGO aerogels were prepared with a one-step hydrothermal method. In detail, 60 mg of (NH4)2MoS4 were dissolved in 10 mL of N, N-dimethylformamide (DMF) solvent. Five milliliters of GO aqueous (5 mg mL−1) were added, and a homogeneous solution was obtained under sonication for several hours. The solution was put to a Teflon-lined autoclave and sealed. Finally, it was heated in the oven at 200°C for 12 h. MoS2/RGO hydrogels were obtained through washing with ethanol and D.I. water. Through freeze-drying and annealing in 700°C for 2 h, the final MoS2/RGO aerogels were obtained. As a comparison, the MoS2 powder was prepared with the same steps except adding GO.


A thin piece of MoS2/RGO film which was cut from the MoS2/RGO aerogels was used to carry out further characterization. Field mission scanning electron microscopy (FESEM, JEOL JSM-6700F) and field-emission transmission electron microscopy (FETEM, FEI, Tecnai G2 F30) were used to characterize the obtained samples. XRD analysis (PANalytical PW3040/60) with Cu Kα radiation (λ = 1.5406 Å) from 10° to 80° was used to confirm the substance of the MoS2/RGO film and MoS2 powder.

Electrochemical Measurements

The MoS2/RGO film was directly used as a binder-free anode, without any binder and conductive agent. It was assembled into a coin-type half-cell in a glove box, with a lithium foil acting as counter electrode and Celgard 2400 polymer as separator. The electrolyte consisted of 1 M LiPF6 in ethylene carbonate (EC) and diethyl carbonate (DEC). After assembly, the cell was aged 24 h in the glove box for further measurements. The galvanostatic charge/discharge (GCD) measurements were carried out with a battery measurement system (Land, China), and cyclic voltammetry (CV) testings were conducted with Autolab workstation (PGSTAT-302N). The testing was conducted in the potential range of 0.01–3.0 V (vs Li1/Li). Electrochemical impedance spectra (EIS) experiments were carried out with 10 mV amplitude in the frequency from 100 kHz to 0.01 Hz.

Results and Discussion

The MoS2/RGO aerogels were fabricated with a hydrothermal method, freeze-drying and heat treatment. Figure 1 displayed the preparation process of the MoS2/RGO electrode. Detailed methods were described on the Materials and methods. As shown in Additional file 1: Figure S1 and Additional file 2: Figure S2, the obtained MoS2/RGO aerogel could keep integrate structure. The excellent mechanical behavior was beneficial from the rich porosity of the whole structure and the interconnection of graphene layers, showing great potential as a binder-free electrode.

Fig. 1
figure 1

Schematic of fabrication of hybrid nanostructure of MoS2/RGO

Figure 2 presented the morphology of MoS2/rGO aerogel. A porous structure with wrinkled graphene layers interconnected with each other was observed (Fig. 2a), where MoS2 nanostructures covered the whole graphene layers. The microstructure of MoS2/RGO aerogels was further confirmed with TEM (Additional file 3: Figure S3). As displayed in Fig. 2c and d, the MoS2 nanostructures were distributed on the graphene even after long-time ultrasonication, illustrating the strong interaction of MoS2 on graphene. The high-resolution TEM image was displayed in Fig. 2f. The graphene layers were covered with MoS2 nanostructures, where lattice spacings of 0.61 and 0.27 nm were observed, which were responsible for (002) and (100) planes of MoS2 [29]. The SAED pattern (inset of Fig. 2f) presented several diffraction rings, which was well corresponding to MoS2 planes [30]. These results illustrated that MoS2 nanostructures on graphene layer exhibited a good crystallinity. The elemental distribution of the aerogel was detected (Fig. 2g–j) where Mo, S, and C elements were almost overlapped with the whole structure, suggesting the successful fabrication of the composite.

Fig. 2
figure 2

a, b SEM images and c, d, e, f TEM and HRTEM images of the MoS2/RGO sample. gj TEM-EDX mapping of Mo, S, and C elements. The inset in f is the corresponding SAED pattern

X-ray diffraction (XRD) experiments were also carried out. As shown in Fig. 3a, the XRD patterns of the MoS2 powder could be responsible for hexagonal 2H–MoS2 (JCPDS 37-1492). The strong reflection peak at 2θ = 14.2o belonged to the (002) plane, with a d-spacing of 0.62 nm. MoS2/RGO composite showed the similar crystalline structure of pure MoS2, indicating a layered structure. Comparing with the MoS2 samples, an obvious peak in 26.3° was observed in the MoS2/RGO samples, which could be the (002) diffraction peak of graphene, revealing the graphene substance in the composites [31]. It was worth pointing out that the obvious peak at 14.4°, 32.7° and 58.3° were ascribed to the (002), (100) and (110) diffraction peak of MoS2, which was consistent with the previous SAED pattern results. Notably, the MoS2 (002) reflection peak, which indicated a stacked nature of layered MoS2, was weakened for the MoS2/RGO composite, suggesting the formation of a few-layer MoS2 structure [26, 32]. The peaks of graphene were more obvious than the MoS2, further confirming that the MoS2 was wrapped by graphene layer in the MoS2/RGO aerogels [26, 32].

Fig. 3
figure 3

a XRD patterns of MoS2/RGO and MoS2 samples. b Raman spectra of the MoS2/RGO and MoS2

To further confirm the nature of MoS2 nanostructure and graphene layer, Raman spectroscopy measurements were also carried out [33,34,35]. As shown in Fig. 3b, the MoS2/RGO aerogel showed the E2g and A1g peaks of MoS2 at the frequencies of 380.2 and 403.6 cm−1 [18, 36]. Notably, it had been reported that the single-layer MoS2 nanostructure with different fabrication method would display an A1g peak at 402–404 cm−1 [37,38,39], further identifying the few layer of MoS2 crystals in the MoS2/RGO aerogel. Besides, the peaks at 1354.3 cm−1 and 1591.6 cm−1 were observed in Fig. 3b, which were characteristic peaks of the D- and G-bands of graphene [40,41,42]. The intensity ratio ID/IG was usually associated with the graphene defects [35]. The value was calculated to be 1.08, indicating the reduced graphene with some defects [34].

To demonstrate the performance of MoS2/RGO electrode, CV measurements at a scan rate of 0.5 mV s−1 were carried out. Figure 4a showed the first three CV curves of MoS2/RGO composite. A broad shoulder peak was observed at 0.95 V when there were reduction peaks at 0.65 V in the first cathodic sweep of the MoS2/RGO electrode. The peak at 0.95 V was related with Li+ intercalation into MoS2 interlayer space to form LixMoS2, with a phase transformation process to become 1T(octahedral) structure of LixMoS2 from 2H (trigonal prismatic) [43, 44]. The other peak at 0.65 V was accompanied with the process to form Li2S and metallic Mo from LixMoS2 [45,46,47]. In the following discharge scans, there were reduction peaks located at 1.80 V and 1.05 V, indicating a different reaction process. One pronounced peak at 2.34 V was observed for the MoS2/RGO electrode in the reverse anodic scans, indicating the formation of sulfur [43]. It could be inferred that sulfur, Mo, and few MoS2 were formed after the first cycle and they were kept the same in subsequent cycles [36, 48,49,50]. In addition, the discharge curves were identical except for the first one, indicating the electrochemical stability for the MoS2/RGO composite. The first three GCD curves of the MoS2/RGO and MoS2 electrodes were shown in Fig. 4b and c. In the first discharge cycle of the MoS2 electrode, two potential plateaus were observed at 1.05 V and 0.65 V (Fig. 4b). The 1.05 V plateau was accompanied with the process of forming LixMoS2, and the plateau at 0.65 V was related with the reaction of forming Mo particles from MoS2. A slope potential curve was observed below 0.52 V in the first discharge cycles, meaning the appearance of gel-like polymeric layer due to the degradation of electrolyte [51,52,53]. The MoS2 electrode showed plateaus at 2.0, 1.20 and 0.45 V in the following discharge curves. In the charge process, an obvious plateau at 2.35 V was observed for the MoS2 electrode. For the MoS2/RGO electrode (Fig. 4c), there was no obvious potential plateau during the first discharge cycle, except for a week plateau at 1.1–0.6 V, which was mainly ascribed to the overlapping lithium process in MoS2 and RGO [54]. MoS2/RGO electrode displayed a plateau at 1.95 V in the following discharge cycles, in agreement with the CV results. During the charge cycles, the MoS2/RGO electrode showed a plateau at 2.2 V. Figure 4c showed the discharge and charge capacity of MoS2/RGO and MoS2 electrode. MoS2/RGO electrode delivered 2215 mAh g−1 discharge capacity in the first discharge cycle, with a reversible charge capacity of 1202 mAh g−1. The corresponding values for the MoS2 were 671.1 mAh g−1 and 680.5 mAh g−1, respectively. The irreversible processes in the first cycle, such as decomposition of electrolyte and the formation of SEI film, lead to irreversibility [55, 56].

Fig. 4
figure 4

The first three cyclic voltammograms of MoS2/RGO aerogel at a scan rate of 0.5 mV s-1 (a). Galvanostatic charge and discharge curves of MoS2/RGO aerogel (b) and MoS2 (c) electrodes at a current density of 100 mA g-1. d Rate performances of MoS2/RGO aerogel and MoS2 electrodes at different current densities. e Cycling performance of MoS2/RGO aerogel and MoS2 electrodes at a constant current density of 100 mA g-1

The rate performances of MoS2/RGO electrode and MoS2 electrodes were shown in Fig. 4d. Comparing with single MoS2 electrodes, MoS2/RGO electrodes delivered higher capacities. A capacity of 1041 mAh g−1 at 100 mA g−1 was kept after 50 discharge/charge cycles for the MoS2/RGO electrode, indicating a good electrochemical reversibility as well as a long cycle stability. By comparison, the MoS2 electrode only kept 512 mAh g−1 capacity at 100 mA g−1 after 50 cycles. Moreover, the specific capacity of the MoS2 electrode decreased a lot when the current decreased from 2000 mA g−1 to100 mA g−1. The cycling results conducted at 100 mA g−1 were shown in Fig. 4e. The MoS2 electrode showed a poor cycling performance. There was nearly no decrease in its initial 20 cycles. However, the reversible (charge) capacity decreased from 892 mAh g−1 to 110 mAh g−1 after 100 cycles, with only 12.3% capacity retention. On the contrary, the MoS2/RGO electrodes displayed an improved cyclic stability. A reversible capacity of 667 mAh g−1, with a 58.6% capacity retention was obtained after 100 cycles. The rate performances and cycling stability of pure RGO electrode were also displayed in Additional file 4: Figure S4. The RGO electrode delivered a reversible charge capacity of 297.8 mAh g−1 at 100 mA g−1. When the current density reversed from 2000 mA g−1 to100 mA g−1, the specific capacity of 202.2 mAh g−1 was kept for the RGO electrode. Table 1 showed a comparison of the capacity performance about the binder-free MoS2/RGO and other materials based on MoS2/rGO listed in the literature [57,58,59,60,61,62,63]. It could be seen that the binder-free MoS2/RGO electrode showed high capacity compared with other porous MoS2/RGO composites ever reported. These results illustrated the successful introduction of RGO, and the important role it played in the delithium-lithium process [57]. Firstly, the graphene layer with highly porous architecture provided rich active sites for the MoS2 nanostructure, which was beneficial to preventing aggregation of MoS2. Secondly, the graphene with good conductivity reduced transfer resistance and promoted electron transmission and ion transport, leading to an improved rate capability. Thirdly, the RGO aerogel with multi-scale porous structure acted as an elastic buffer layer, which effectively restrained the volume expansion during the delithium-lithium process, and thus lead a better cycling stability.

Table 1 Comparison of the capacity of MoS2-graphene composites materials for Li-ion Battery

Electrochemical impedance spectra (EIS) measurements were also conducted for the samples. Figure 5a showed the Nyquist plots of MoS2/RGO and MoS2 electrodes after 100 discharge-charge cycles at 100 mA g−1. The first semicircle represented lithium ion migration resistance through the SEI films (R1), while the second semicircle stood for the resistance of charge transport (Rct). R2 was related with the resistance of electrolyte [26]. ZView software was used to fit the curves of MoS2/RGO and MoS2 electrodes. The fitted values were listed in the Fig. 5b. From the table, the Rct of the MoS2/RGO electrode (10.74Ω) was smaller than MoS2 (44.07 Ω), indicating that rGO could bring an improved charge transfer process during discharge-charge actions and thus show a good rate capability.

Fig. 5
figure 5

a Nyquist plots of MoS2/RGO and MoS2 electrodes at fully charged state after 100 cycles at 100 mA g−1, and b values of R1, R2, and Rct obtained by fitting data according to the equivalent circuit model presented in a

To investigate the impact of repeated charge/discharge processes on the as-prepared samples, FESEM were conducted on the samples after 100 cycles at 100 mA g−1 (Additional file 1: Figure S1). MoS2/ RGO electrode kept a well structure without any cracks. The cross-sectional FESEM pictures in Additional file 1: Figure S1c and d showed the high-compressible graphene layer where nanoparticles were distributed. On the contrary, severe cracks were observed on the pristine MoS2 electrode in Additional file 1: Figure S1e and f. It was mainly because the volume expansion of active material during cycling, thus leading to particles aggregation. The above results illustrated the important role of graphene layer in inhibiting the volume expansion in the cycling process (Additional file 5: Figure S5).


In summary, hybrid MoS2/RGO aerogels with rich micropores have been fabricated. The prepared aerogels are used as electrodes without any binder and conducting agent. Such a nanostructure design with abundant micro-pores is not only beneficial to providing 3D network for enhanced electron transfer, but also can shorten the transport distance, thus leading to an improved electrochemical rate and stable performance as the anode electrodes for LIBs. MoS2/RGO aerogel delivers specific capacities of 1041 mA h g−1 at 100 mA g−1, which is ascribed to the synergistic effect of MoS2 nanostructure and conductive graphene, as well as the binder-free design with abundant micro-pores. The study offers useful insights for realizing high-performance anode electrodes for LIBs with high capacity and long cycle stability.



Trigonal prismatic


Cyclic voltammograms


Electrochemical impedance spectroscopy


Galvanostatic charge/discharge


Graphene oxide


High-resolution TEM


Lithium ion batteries

MoS2 :

Molybdenum disulfide


MoS2/ reduced graphene


Lithium ion migration resistance through the SEI films


The resistance of electrolyte


The resistance of charge transport


Selected area electron diffraction


2D transition metal dichalcogenides


X-ray diffraction


  1. Armand M, Tarascon J-M (2008) Building better batteries. Nature 451:652–657

    Article  CAS  Google Scholar 

  2. Scrosati B, Hassoun J, Sun Y-K (2011) Lithium-ion batteries. A look into the future. Energy Environ Sci 4:3287–3295

    Article  CAS  Google Scholar 

  3. Kim SW, Seo DH, Ma X, Ceder G, Kang K (2012) Electrode materials for rechargeable sodium-ion batteries: potential alternatives to current lithium-ion batteries. Adv Energy Mater 2:710–721

    Article  CAS  Google Scholar 

  4. Yabuuchi N, Kubota K, Dahbi M, Komaba S (2014) Research development on sodium-ion batteries. Chem Rev 114:11636–11682

    Article  CAS  Google Scholar 

  5. David L, Bhandavat R, Barrera U, Singh G (2016) Silicon oxycarbide glass-graphene composite paper electrode for long-cycle lithium-ion batteries. Nat Commun 7:10998

  6. Tan C, Zhang H (2015) Two-dimensional transition metal dichalcogenide nanosheet-based composites. Chem Soc Rev 44:2713–2731

    Article  CAS  Google Scholar 

  7. Zhu C, Mu X, van Aken PA, Yu Y, Maier J (2014) Single-layered ultrasmall nanoplates of MoS2 embedded in carbon nanofibers with excellent electrochemical performance for lithium and sodium storage. Angew Chem Int Ed 53:2152–2156

    Article  CAS  Google Scholar 

  8. Zhu C, Mu X, van Aken PA, Maier J, Yu Y (2015) Fast Li storage in MoS2-graphene-carbon nanotube nanocomposites: advantageous functional integration of 0D, 1D, and 2D nanostructures. Adv Energy Mater 5(4):1401170

  9. Liu C, Li F, Ma LP, Cheng HM (2010) Advanced materials for energy storage. Adv Mater 22(8):E28-E62.

  10. Wu Z-S, Zhou G, Yin L-C, Ren W, Li F, Cheng H-M (2012) Graphene/metal oxide composite electrode materials for energy storage. Nano Energy 1:107–131

    Article  CAS  Google Scholar 

  11. Reddy M, Subba Rao G, Chowdari B (2013) Metal oxides and oxysalts as anode materials for Li ion batteries. Chem Rev 113:5364–5457

    Article  CAS  Google Scholar 

  12. Ji L, Lin Z, Alcoutlabi M, Zhang X (2011) Recent developments in nanostructured anode materials for rechargeable lithium-ion batteries. Energy Environ Sci 4:2682–2699

    Article  CAS  Google Scholar 

  13. Guo YG, Hu JS, Wan LJ (2008) Nanostructured materials for electrochemical energy conversion and storage devices. Adv Mater 20:2878–2887

    Article  CAS  Google Scholar 

  14. Chang K, Chen W, Ma L, Li H, Li H, Huang F, Xu Z, Zhang Q, Lee J-Y (2011) Graphene-like MoS 2/amorphous carbon composites with high capacity and excellent stability as anode materials for lithium ion batteries. J Mater Chem 21:6251–6257

    Article  CAS  Google Scholar 

  15. Wang C, Wan W, Huang Y, Chen J, Zhou HH, Zhang XX (2014) Hierarchical MoS 2 nanosheet/active carbon fiber cloth as a binder-free and free-standing anode for lithium-ion batteries. Nanoscale 6:5351–5358

    Article  CAS  Google Scholar 

  16. Wan Z, Shao J, Yun J, Zheng H, Gao T, Shen M, Qu Q, Zheng H (2014) Core–shell structure of hierarchical quasi-hollow MoS2 microspheres encapsulated porous carbon as stable anode for Li-ion batteries. Small 10:4975–4981

    Article  CAS  Google Scholar 

  17. Zhang L, Lou XWD (2014) Hierarchical MoS2 shells supported on carbon spheres for highly reversible lithium storage. Chem Eur J 20:5219–5223

    Article  CAS  Google Scholar 

  18. Shi Y, Wang Y, Wong JI, Tan AYS, Hsu C-L, Li L-J, Lu Y-C, Yang HY (2013) Self-assembly of hierarchical MoSx/CNT nanocomposites (2<x<3): towards high performance anode materials for lithium ion batteries. Sci Rep 3:2169

  19. Wang J, Liu J, Chao D, Yan J, Lin J, Shen ZX (2014) Self-assembly of honeycomb-like MoS2 nanoarchitectures anchored into graphene foam for enhanced lithium-ion storage. Adv Mater 26:7162–7169

    Article  CAS  Google Scholar 

  20. Wang Y, Kong D, Shi W, Liu B, Sim GJ, Ge Q, Yang HY (2016) Ice templated free-standing hierarchically WS2/CNT-rGO aerogel for high-performance rechargeable lithium and sodium ion batteries. Adv Energy Mater 6(21):1601057

  21. Wei J, Zang Z, Zhang Y, Wang M, Du J, Tang X (2017) Enhanced performance of light-controlled conductive switching in hybrid cuprous oxide/reduced graphene oxide (Cu 2 O/rGO) nanocomposites. Opt Lett 42:911–914

    Article  CAS  Google Scholar 

  22. Zang Z, Zeng X, Wang M, Hu W, Liu C, Tang X (2017) Tunable photoluminescence of water-soluble AgInZnS–graphene oxide (GO) nanocomposites and their application in-vivo bioimaging. Sensors Actuators B Chem 252:1179–1186

    Article  CAS  Google Scholar 

  23. Huang H, Zhang J, Jiang L, Zang Z (2017) Preparation of cubic Cu2O nanoparticles wrapped by reduced graphene oxide for the efficient removal of rhodamine B. J Alloys Compd 718:112–115

    Article  CAS  Google Scholar 

  24. Liu J, Li S, Zhang B, Xiao Y, Gao Y, Yang Q, Wang Y, Lu G (2017) Ultrasensitive and low detection limit of nitrogen dioxide gas sensor based on flower-like ZnO hierarchical nanostructure modified by reduced graphene oxide. Sensors Actuators B Chem 249:715–724

    Article  CAS  Google Scholar 

  25. Ramadoss A, Yoon K-Y, Kwak M-J, Kim S-I, Ryu S-T, Jang J-H (2017) Fully flexible, lightweight, high performance all-solid-state supercapacitor based on 3-dimensional-graphene/graphite-paper. J Power Sources 337:159–165

    Article  CAS  Google Scholar 

  26. Teng Y, Zhao H, Zhang Z, Li Z, Xia Q, Zhang Y, Zhao L, Du X, Du Z, Lv P (2016) MoS2 Nanosheets vertically grown on graphene sheets for lithium-ion battery anodes. ACS Nano 10:8526–8535

    Article  CAS  Google Scholar 

  27. Liu Y, Zhao Y, Jiao L, Chen J (2014) A graphene-like MoS 2/graphene nanocomposite as a highperformance anode for lithium ion batteries. J Mater Chem A 2:13109–13115

    Article  CAS  Google Scholar 

  28. Hummers WS Jr, Offeman RE (1958) Preparation of graphitic oxide. J Am Chem Soc 80:1339–1339

    Article  CAS  Google Scholar 

  29. Chang K, Chen W (2011) In situ synthesis of MoS 2/graphene nanosheet composites with extraordinarily high electrochemical performance for lithium ion batteries. Chem Commun 47:4252–4254

    Article  CAS  Google Scholar 

  30. Hou Y, Wen Z, Cui S, Guo X, Chen J (2013) Constructing 2D porous graphitic C3N4 nanosheets/nitrogen-doped graphene/layered MoS2 ternary nanojunction with enhanced photoelectrochemical activity. Adv Mater 25:6291–6297

    Article  CAS  Google Scholar 

  31. Zhao L, Hong C, Lin L, Wu H, Su Y, Zhang X, Liu A (2017) Controllable nanoscale engineering of vertically aligned MoS 2 ultrathin nanosheets by nitrogen doping of 3D graphene hydrogel for improved electrocatalytic hydrogen evolution. Carbon 116:223–231

    Article  CAS  Google Scholar 

  32. Hwang H, Kim H, Cho J (2011) MoS2 nanoplates consisting of disordered graphene-like layers for high rate lithium battery anode materials. Nano Lett 11:4826–4830

    Article  CAS  Google Scholar 

  33. Kudin KN, Ozbas B, Schniepp HC, Prud’Homme RK, Aksay IA, Car R (2008) Raman spectra of graphite oxide and functionalized graphene sheets. Nano Lett 8:36–41

    Article  CAS  Google Scholar 

  34. Caballero Á, Morales J (2012) Can the performance of graphene nanosheets for lithium storage in Li-ion batteries be predicted? Nanoscale 4:2083–2092

    Article  Google Scholar 

  35. Pimenta M, Dresselhaus G, Dresselhaus MS, Cancado L, Jorio A, Saito R (2007) Studying disorder in graphite-based systems by Raman spectroscopy. Phys Chem Chem Phys 9:1276–1290

    Article  CAS  Google Scholar 

  36. Frey GL, Tenne R, Matthews MJ, Dresselhaus M, Dresselhaus G (1999) Raman and resonance Raman investigation of MoS 2 nanoparticles. Phys Rev B 60:2883

    Article  CAS  Google Scholar 

  37. Ghatak S, Pal AN, Ghosh A (2011) Nature of electronic states in atomically thin MoS2 field-effect transistors. ACS Nano 5:7707–7712

    Article  CAS  Google Scholar 

  38. Lee C, Yan H, Brus LE, Heinz TF, Hone J, Ryu S (2010) Anomalous lattice vibrations of single-and few-layer MoS2. ACS Nano 4:2695–2700

    Article  CAS  Google Scholar 

  39. Lee HS, Min S-W, Chang Y-G, Park MK, Nam T, Kim H, Kim JH, Ryu S, Im S (2012) MoS2 nanosheet phototransistors with thickness-modulated optical energy gap. Nano Lett 12:3695–3700

    Article  CAS  Google Scholar 

  40. Xiong X, Wang G, Lin Y, Wang Y, Ou X, Zheng F, Yang C, Wang J-H, Liu M (2016) Enhancing sodium ion battery performance by strongly binding nanostructured Sb2S3 on sulfur-doped graphene sheets. ACS Nano 10:10953–10959

    Article  CAS  Google Scholar 

  41. Xiang H, Li Z, Xie K, Jiang J, Chen J, Lian P, Wu J, Yu Y, Wang H (2012) Graphene sheets as anode materials for Li-ion batteries: preparation, structure, electrochemical properties and mechanism for lithium storage. RSC Adv 2:6792–6799

    Article  CAS  Google Scholar 

  42. Wang Z, Chen T, Chen W, Chang K, Ma L, Huang G, Chen D, Lee JY (2013) CTAB-assisted synthesis of single-layer MoS 2–graphene composites as anode materials of Li-ion batteries. J Mater Chem A 1:2202–2210

    Article  Google Scholar 

  43. Li X-L, Li Y-D (2004) MoS2 nanostructures: synthesis and electrochemical Mg2+ intercalation. J Phys Chem B 108:13893–13900

    Article  CAS  Google Scholar 

  44. Liu Y, He X, Hanlon D, Harvey A, Khan U, Li Y, Coleman JN (2016) Electrical, mechanical, and capacity percolation leads to high-performance MoS2/nanotube composite lithium ion battery electrodes. ACS Nano 10:5980–5990

    Article  CAS  Google Scholar 

  45. Fang Y, Lv Y, Gong F, Elzatahry AA, Zheng G, Zhao D (2016) Synthesis of 2D-mesoporous-carbon/MoS2 heterostructures with well-defined interfaces for high-performance lithium-ion batteries. Adv Mater 28:9385–9390

    Article  CAS  Google Scholar 

  46. Wang Y, Yu L, Lou XWD (2016) Inside back cover: synthesis of highly uniform molybdenum–glycerate spheres and their conversion into hierarchical MoS2 hollow nanospheres for lithium-ion batteries (Angew. Chem. Int. Ed. 26/2016). Angew Chem Int Ed 55:7549–7549

    Article  Google Scholar 

  47. Jiang L, Lin B, Li X, Song X, Xia H, Li L, Zeng H (2016) Monolayer MoS2–graphene hybrid aerogels with controllable porosity for lithium-ion batteries with high reversible capacity. ACS Appl Mater Interfaces 8:2680–2687

    Article  CAS  Google Scholar 

  48. Deng Z, Jiang H, Hu Y, Liu Y, Zhang L, Liu H, Li C (2017) 3D ordered macroporous MoS2@ C nanostructure for flexible Li-ion batteries. Adv Mater 29(10):1603020.

  49. Chao Y, Jalili R, Ge Y, Wang C, Zheng T, Shu K, Wallace GG (2017) Self-assembly of flexible free-standing 3D porous MoS2-reduced graphene oxide structure for high-performance Lithium-ion batteries. Adv Funct Mater 27(22):1700234.

  50. Wang R, Wang S, Peng X, Zhang Y, Jin D, Chu PK, Zhang L (2017) Elucidating the intercalation pseudocapacitance mechanism of MoS2–carbon monolayer interoverlapped superstructure: toward high-performance sodium-ion-based hybrid supercapacitor. ACS Appl Mater Interfaces 9:32745–32755

    Article  CAS  Google Scholar 

  51. Chang K, Chen W (2011) L-cysteine-assisted synthesis of layered MoS2/graphene composites with excellent electrochemical performances for lithium ion batteries. ACS Nano 5:4720–4728

    Article  CAS  Google Scholar 

  52. Zuo X, Chang K, Zhao J, Xie Z, Tang H, Li B, Chang Z (2016) Bubble-template-assisted synthesis of hollow fullerene-like MoS 2 nanocages as a lithium ion battery anode material. J Mater Chem A 4:51–58

    Article  CAS  Google Scholar 

  53. Zhou J, Qin J, Zhao N, Shi C, Liu E-Z, He F, Li J, He C (2016) Salt-template-assisted synthesis of robust 3D honeycomb-like structured MoS 2 and its application as a lithium-ion battery anode. J Mater Chem A 4:8734–8741

    Article  CAS  Google Scholar 

  54. Cao X, Shi Y, Shi W, Rui X, Yan Q, Kong J, Zhang H (2013) Preparation of MoS2-coated three-dimensional graphene networks for high-performance anode material in Lithium-ion batteries. Small 9:3433–3438

    Article  CAS  Google Scholar 

  55. Huang G, Chen T, Chen W, Wang Z, Chang K, Ma L, Huang F, Chen D, Lee JY (2013) Graphene-like MoS2/graphene composites: cationic surfactant-assisted hydrothermal synthesis and electrochemical reversible storage of lithium. Small 9:3693–3703

    Article  CAS  Google Scholar 

  56. Zhou J, Qin J, Zhang X, Shi C, Liu E, Li J, Zhao N, He C (2015) 2D space-confined synthesis of few-layer MoS2 anchored on carbon nanosheet for lithium-ion battery anode. ACS Nano 9:3837–3848

    Article  CAS  Google Scholar 

  57. Li H, Yu K, Fu H, Guo B, Lei X, Zhu Z (2015) MoS2/graphene hybrid nanoflowers with enhanced electrochemical performances as anode for lithium-ion batteries. J Phys Chem C 119:7959–7968

    Article  CAS  Google Scholar 

  58. Liu H, Chen X, Deng L, Su X, Guo K, Zhu Z (2016) Preparation of ultrathin 2D MoS 2/graphene heterostructure assembled foam-like structure with enhanced electrochemical performance for lithium-ion batteries. Electrochim Acta 206:184–191

    Article  CAS  Google Scholar 

  59. Youn DH, Jo C, Kim JY, Lee J, Lee JS (2015) Ultrafast synthesis of MoS2 or WS2-reduced graphene oxide composites via hybrid microwave annealing for anode materials of lithium ion batteries. J Power Sources 295:228–234

    Article  CAS  Google Scholar 

  60. Choi M, Koppala SK, Yoon D, Hwang J, Kim SM, Kim J (2016) A route to synthesis molybdenum disulfide-reduced graphene oxide (MoS2-RGO) composites using supercritical methanol and their enhanced electrochemical performance for Li-ion batteries. J Power Sources 309:202–211

    Article  CAS  Google Scholar 

  61. Jing Y, Ortiz-Quiles EO, Cabrera CR, Chen Z, Zhou Z (2014) Layer-by-layer hybrids of MoS 2 and reduced graphene oxide for lithium ion batteries. Electrochim Acta 147:392–400

    Article  CAS  Google Scholar 

  62. Srivastava S, Kartick B, Choudhury S, Stamm M (2016) Thermally fabricated MoS2-graphene hybrids as high performance anode in lithium ion battery. Mater Chem Phys 183:383–391

    Article  CAS  Google Scholar 

  63. Zhang X, Zhang Q, Sun Y, Zhang P, Gao X, Zhang W, Guo J (2016) MoS2-graphene hybrid nanosheets constructed 3D architectures with improved electrochemical performance for lithium-ion batteries and hydrogen evolution. Electrochim Acta 189:224–230

    Article  CAS  Google Scholar 

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We thank the Analytical and Testing Center of Huazhong University of Science and Technology (HUST) for the field emission scanning electron microscopy (FESEM) testing, as well as Flexible Electronics Research Center of HUST.


This work is supported by the National Science Foundation of China (No. 51275195 and No.51775218), the National Basic Research Program of China (No. 2015CB057205), the Program for Changjiang Scholars.

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Authors and Affiliations



YZ and ZT conceived the idea of experiments. YZ carried out the experiments. YH, SC, CC, and LS participated in the discussion and analysis of the experimental result. YZ wrote the manuscript. LS, GL and ZT improved the manuscript. All authors read and approved the final manuscript.

Corresponding author

Correspondence to Zirong Tang.

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Additional files

Additional file 1:

Figure S1. Mechanical performance of the MoS2/RGO aerogel under the finger compression. (JPG 70 kb)

Additional file 2:

Figure S2. Mechanical performance of the MoS2/RGO aerogel before compression (a), under compression (b), and after compression (c). (PNG 2203 kb)

Additional file 3:

Figure S3. (a) TEM picture of the MoS2/RGO sample. (b) TEM-EDS mapping of Mo, S, C elements. (c) EDX spectra of the MoS2/RGO sample. (JPG 304 kb)

Additional file 4:

Figure S4. (a) Rate performances of RGO aerogel electrodes at different current densities. (b) Cycling performance of RGO electrodes at a constant current density of 100 mA g−1. (JPG 114 kb)

Additional file 5:

Figure S5. FESEM images of (a, b) MoS2/RGO electrode, (c, d) cross-sectional images of MoS2/RGO and SEM images of (e, f) bare MoS2 electrode after 100 cycles performed with a current density of 100 mA g−1. (JPG 1649 kb)

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Zhong, Y., Shi, T., Huang, Y. et al. Three-dimensional MoS2/Graphene Aerogel as Binder-free Electrode for Li-ion Battery. Nanoscale Res Lett 14, 85 (2019).

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  • MoS2
  • Graphene aerogel
  • Binder-free
  • Li-ion battery