Microwave synthesis of SnO2 nanocrystals decorated on the layer-by-layer reduced graphene oxide for an application into lithium ion battery anode
Graphical abstract
Introduction
Rechargeable lithium ion batteries (LIBs) are a promising energy source for electrical vehicles, electrical devices and energy storage system (ESS) because of the high energy density, high operation voltage and long life cycle [1]. Although graphite has been mostly used as a commercial anode in LIBs, it has not been satisfied in the demand of high energy density because of the its intrinsically limited specific capacity of 372 mAh g−1 and sluggish ion and electron transport kinetics through the van der Waals gaps of interlayers [2], [3]. In order to resolve the afore-mentioned bottlenecks, various kinds of anode materials have been developed for the design of the high performance LIBs.
Graphene-derived materials are also considered as the promising energy storage materials because there are several advantages such as high theoretical specific capacity (744 mAh g−1), superior electrical conductivities, large specific surface area (∼2600 m2 g−1) and good mechanical properties [4], [5], [6], [7]. To apply those advantages for LIBs, researchers have tried to make layer-by-layer structure by using chemical vapor deposition [8], [9], vacuum filtration [10], [11] and so on [12], [13], but the restacking of graphene sheets such as face-to-face aggregation could hamper fast electrolyte diffusion into the storage sites. Moreover, it results in diminishing available surface area. In order to prevent the restacking problem, researchers have investigated to use carbon nanotubes [14], [15], [16], [17], [18], carbon nanofibers [19], conducting polymer [20], [21], [22] and metal oxides [23], [24] as a role of pillars to hold spaces between the graphene sheets that allows to maximize the intrinsically good properties of graphene for the improved electrochemical performances [25]. Among the various kinds of pillars, metal oxides could be a better solution for LIBs because the rGO could be in a form of composites with metal oxide on a nanoscale and the synergizing effects of integrating high capacity metal oxide with high conductivity and large specific surface area of rGO on the battery performances. The representative metal oxides to incorporate with graphene are tungsten oxide [26], iron oxides [27], [28], [29], copper oxides [30], [31], cobalt oxides [32], [33], [34], manganese oxides [35], [36], nickel oxides [37], [38] and tin oxides [39], [40]. Especially, SnO2 is an attractive anode material because of high theoretical reversible capacity (781 mAh g−1 for SnO2), less toxicity and excellent processability for LIBs [41], [42], [43], [44], [45], [46], [47], [48]. If SnO2 nanoparticles are randomly decorated on the rGO sheets, it is possible to solve the restacking problem and to enhance the rate and cyclic capabilities along with the high specific capacity.
The SnO2 nanoparticles decorated onto the graphene sheets have been investigated by various synthesis methods such as microwave, hydrothermal, gas-liquid interfacial reaction, laser irradiation, co-precipitation and ultrasonication synthesis [39], [49], [50], [51], [52], [53], [54], [55]. Particularly, the microwave synthesis is a representative method to fabricate the nanocomposites efficiently because of ultra-fast reaction time, high energy efficiency and simple process. In addition, it is eco-friendly, economical and has better reproducibility, compared to the conventional methods [56], [57], [58].
Herein, we demonstrate the method to make layer-by-layer yet restacking inhibited structured G-SnO2 with the well-defined uniform SnO2 nanoparticles by utilizing a vacuum filtration and microwave method. The precursors of SnO2 are inserted into the interlayers of rGO sheets and directly transformed to the metal oxide nanoparticles through the nucleation and growth induced by the microwave irradiation. Thus, the SnO2 nanoparticles are randomly decorated onto the surfaces of rGO interlayer, while acting as pillars to provide both mechanical exfoliation and high capacity.
Section snippets
Synthesis of rGO
The GO was prepared by Hummers method [59]. GO (40 mg) were uniformly dispersed into the deionized water (7.6 mL) by sonication. Hypophorous acid (H3PO2, SAMCHUN Chemical, 50 wt%) and iodine (I2, DAEJUNG, 99.0%) was blended with the dispersed mixture into a vial. Then, the mixture was placed into the 80 °C oven for 12 h. After the gel was formed, the gel was washed by deionized water. When it became pH 7, the gel was put into the freeze-dryer for 72 h, and the rGO was obtained.
Microwave synthesis of SnO2 on rGO sheets
The rGO (5 wt%)
Results and discussion
As shown in Fig. 2(a), the SnO2 nanoparticles were randomly decorated on the rGO sheets because the microwave was uniformly irradiated to the reactor bottles and nucleation was very fast. Such randomly deposited SnO2 nanoparticles were well distributed onto the mesoporous surface of rGO without significant local aggregation. Moreover, the surface of G-SnO2 became rough and crumpled after the microwave irradiation. From Fig. 2(b), the layer-by-layer structure which was formed by vacuum
Conclusion
In summary, G-SnO2 was simply synthesized by vacuum filtration and microwave irradiation. G-SnO2 created a layer-by-layer structure in the course of the vacuum filtration, while the exfoliation of rGO sheets was preserved with the synthesis and decoration of SnO2 nanoparticles during the microwave irradiation. Through those processes, SnO2 nanoparticles were randomly inserted into the rGO sheets, playing important roles of pillars to prevent the restacking problem and of active material to
Acknowledgment
This research was supported by a grant from R&D Program of the Korea Railroad Research Institute, Republic of Korea.
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2019, Journal of Power SourcesCitation Excerpt :Despite these advantages, vanadium oxides have the limitation of low electronic conductivity [17,18], large volume expansion [19,20], and dissolution of active species resulting in low rate capability and capacity fading during cycles [21]. High capacity transition metal oxides are hybridized with or deposited onto a large surface area of carbon nanomaterials in order to release localized stress and increase electronic conductivity [22–27]. Inspired by these chemical modifications, vanadium pentoxide (V2O5)/graphene composites have been synthesized through hydrothermal [15,28], sol-gel [29], solvothermal [30,31], and self-assembly methods [32].