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1.  Polymer-Derived Ceramic Functionalized MoS2 Composite Paper as a Stable Lithium-Ion Battery Electrode 
Scientific Reports  2015;5:9792.
A facile process is demonstrated for the synthesis of layered SiCN-MoS2 structure via pyrolysis of polysilazane functionalized MoS2 flakes. The layered morphology and polymer to ceramic transformation on MoS2 surfaces was confirmed by use of electron microscopy and spectroscopic techniques. Tested as thick film electrode in a Li-ion battery half-cell, SiCN-MoS2 showed the classical three-stage reaction with improved cycling stability and capacity retention than neat MoS2. Contribution of conversion reaction of Li/MoS2 system on overall capacity was marginally affected by the presence of SiCN while Li-irreversibility arising from electrolyte decomposition was greatly suppressed. This is understood as one of the reasons for decreased first cycle loss and increased capacity retention. SiCN-MoS2 in the form of self-supporting paper electrode (at 6 mg·cm−2) exhibited even better performance, regaining initial charge capacity of approximately 530 mAh·g−1 when the current density returned to 100 mA·g−1 after continuous cycling at 2400 mA·g−1 (192 mAh·g−1). MoS2 cycled electrode showed mud-cracks and film delamination whereas SiCN-MoS2 electrodes were intact and covered with a uniform solid electrolyte interphase coating. Taken together, our results suggest that molecular level interfacing with precursor–derived SiCN is an effective strategy for suppressing the metal-sulfide/electrolyte degradation reaction at low discharge potentials.
doi:10.1038/srep09792
PMCID: PMC4389211  PMID: 25851595
2.  Exfoliated MoS2 Sheets and Reduced Graphene Oxide-An Excellent and Fast Anode for Sodium-ion Battery 
Scientific Reports  2015;5:12571.
Three dimensional (3D) MoS2 nanoflowers are successfully synthesized by hydrothermal method. Further, a composite of as prepared MoS2 nanoflowers and rGO is constructed by simple ultrasonic exfoliation technique. The crystallography and morphological studies have been carried out by XRD, FE-SEM, TEM, HR-TEM and EDS etc. Here, XRD study revealed, a composite of exfoliated MoS2 with expanded spacing of (002) crystal plane and rGO can be prepared by simple 40 minute of ultrasonic treatment. While, FE-SEM and TEM studies depict, individual MoS2 nanoflowers with an average diameter of 200 nm are uniformly distributed throughout the rGO surface. When tested as sodium-ion batteries anode material by applying two different potential windows, the composite demonstrates a high reversible specific capacity of 575 mAhg−1 at 100 mAg−1 in between 0.01 V–2.6 V and 218 mAhg−1 at 50 mAg−1 when discharged in a potential range of 0.4 V–2.6 V. As per our concern, the results are one of the best obtained as compared to the earlier published one on MoS2 based SIB anode material and more importantly this material shows such an excellent reversible Na-storage capacity and good cycling stability without addition of any expensive additive stabilizer, like fluoroethylene carbonate (FEC), in comparison to those in current literature.
doi:10.1038/srep12571
PMCID: PMC4517166  PMID: 26215284
3.  A new cathode material for super-valent battery based on aluminium ion intercalation and deintercalation 
Scientific Reports  2013;3:3383.
Due to their small footprint and flexible siting, rechargeable batteries are attractive for energy storage systems. A super-valent battery based on aluminium ion intercalation and deintercalation is proposed in this work with VO2 as cathode and high-purity Al foil as anode. First-principles calculations are also employed to theoretically investigate the crystal structure change and the insertion-extraction mechanism of Al ions in the super-valent battery. Long cycle life, low cost and good capacity are achieved in this battery system. At the current density of 50 mAg−1, the discharge capacity remains 116 mAhg−1 after 100 cycles. Comparing to monovalent Li-ion battery, the super-valent battery has the potential to deliver more charges and gain higher specific capacity.
doi:10.1038/srep03383
PMCID: PMC3843166  PMID: 24287676
4.  Fe2O3 Nanoparticles Wrapped in Multi-walled Carbon Nanotubes With Enhanced Lithium Storage Capability 
Scientific Reports  2013;3:3392.
We have designed a novel hybrid nanostructure by coating Fe2O3 nanoparticles with multi-walled carbon nanotubes to enhance the lithium storage capability of Fe2O3. The strategy to prepare Fe2O3@MWCNTs involves the synthesis of Fe nanoparticles wrapped in MWCNTs, followed by the oxidation of Fe nanoparticles under carbon dioxide. When used as the anode in a Li-ion battery, this hybrid material (70.32 wt% carbon nanotubes, 29.68 wt% Fe2O3) showed a reversible discharge capacity of 515 mAhg−1 after 50 cycles at a density of 100 mAg−1 and the capacity based on Fe2O3 nanoparticles was calculated as 1147 mAhg−1, Three factors are responsibile for the superior performance: (1) The hollow interiors of MWCNTs provide enough spaces for the accommodation of large volume expansion of inner Fe2O3 nanoparticles, which can improving the stability of electrode; (2) The MWCNTs increase the overall conductivity of the anode; (3) A stable solid electrolyte interface film formed on the surface of MWCNTs may reduce capacity fading.
doi:10.1038/srep03392
PMCID: PMC3844968  PMID: 24292097
5.  Scalable Functionalized Graphene Nano-platelets as Tunable Cathodes for High-performance Lithium Rechargeable Batteries 
Scientific Reports  2013;3:1506.
High-performance and cost-effective rechargeable batteries are key to the success of electric vehicles and large-scale energy storage systems. Extensive research has focused on the development of (i) new high-energy electrodes that can store more lithium or (ii) high-power nano-structured electrodes hybridized with carbonaceous materials. However, the current status of lithium batteries based on redox reactions of heavy transition metals still remains far below the demands required for the proposed applications. Herein, we present a novel approach using tunable functional groups on graphene nano-platelets as redox centers. The electrode can deliver high capacity of ~250 mAh g−1, power of ~20 kW kg−1 in an acceptable cathode voltage range, and provide excellent cyclability up to thousands of repeated charge/discharge cycles. The simple, mass-scalable synthetic route for the functionalized graphene nano-platelets proposed in this work suggests that the graphene cathode can be a promising new class of electrode.
doi:10.1038/srep01506
PMCID: PMC3604708  PMID: 23514953
6.  Superior cycle performance and high reversible capacity of SnO2/graphene composite as an anode material for lithium-ion batteries 
Scientific Reports  2015;5:9055.
SnO2/graphene composite with superior cycle performance and high reversible capacity was prepared by a one-step microwave-hydrothermal method using a microwave reaction system. The SnO2/graphene composite was characterized by X-ray diffraction, thermogravimetric analysis, Fourier-transform infrared spectroscopy, Raman spectroscopy, scanning electron microscope, X-ray photoelectron spectroscopy, transmission electron microscopy and high resolution transmission electron microscopy. The size of SnO2 grains deposited on graphene sheets is less than 3.5 nm. The SnO2/graphene composite exhibits high capacity and excellent electrochemical performance in lithium-ion batteries. The first discharge and charge capacities at a current density of 100 mA g−1 are 2213 and 1402 mA h g−1 with coulomb efficiencies of 63.35%. The discharge specific capacities remains 1359, 1228, 1090 and 1005 mA h g−1 after 100 cycles at current densities of 100, 300, 500 and 700 mA g−1, respectively. Even at a high current density of 1000 mA g−1, the first discharge and charge capacities are 1502 and 876 mA h g−1, and the discharge specific capacities remains 1057 and 677 mA h g−1 after 420 and 1000 cycles, respectively. The SnO2/graphene composite demonstrates a stable cycle performance and high reversible capacity for lithium storage.
doi:10.1038/srep09055
PMCID: PMC4357011  PMID: 25761938
7.  Fabrication of Nb2O5 Nanosheets for High-rate Lithium Ion Storage Applications 
Scientific Reports  2015;5:8326.
Nb2O5 nanosheets are successfully synthesized through a facile hydrothermal reaction and followed heating treatment in air. The structural characterization reveals that the thickness of these sheets is around 50 nm and the length of sheets is 500 ~ 800 nm. Such a unique two dimensional structure enables the nanosheet electrode with superior performance during the charge-discharge process, such as high specific capacity (~184 mAh·g−1) and rate capability. Even at a current density of 1 A·g−1, the nanosheet electrode still exhibits a specific capacity of ~90 mAh·g−1. These results suggest the Nb2O5 nanosheet is a promising candidate for high-rate lithium ion storage applications.
doi:10.1038/srep08326
PMCID: PMC4321166  PMID: 25659574
8.  In-situ One-step Hydrothermal Synthesis of a Lead Germanate-Graphene Composite as a Novel Anode Material for Lithium-Ion Batteries 
Scientific Reports  2014;4:7030.
Lead germanate-graphene nanosheets (PbGeO3-GNS) composites have been prepared by an efficient one-step, in-situ hydrothermal method and were used as anode materials for Li-ion batteries (LIBs). The PbGeO3 nanowires, around 100–200 nm in diameter, are highly encapsulated in a graphene matrix. The lithiation and de-lithiation reaction mechanisms of the PbGeO3 anode during the charge-discharge processes have been investigated by X-ray diffraction and electrochemical characterization. Compared with pure PbGeO3 anode, dramatic improvements in the electrochemical performance of the composite anodes have been obtained. In the voltage window of 0.01–1.50 V, the composite anode with 20 wt.% GNS delivers a discharge capacity of 607 mAh g−1 at 100 mA g−1 after 50 cycles. Even at a high current density of 1600 mA g−1, a capacity of 406 mAh g−1 can be achieved. Therefore, the PbGeO3-GNS composite can be considered as a potential anode material for lithium ion batteries.
doi:10.1038/srep07030
PMCID: PMC4229670  PMID: 25391220
9.  Silicon carbide-free graphene growth on silicon for lithium-ion battery with high volumetric energy density 
Nature Communications  2015;6:7393.
Silicon is receiving discernable attention as an active material for next generation lithium-ion battery anodes because of its unparalleled gravimetric capacity. However, the large volume change of silicon over charge–discharge cycles weakens its competitiveness in the volumetric energy density and cycle life. Here we report direct graphene growth over silicon nanoparticles without silicon carbide formation. The graphene layers anchored onto the silicon surface accommodate the volume expansion of silicon via a sliding process between adjacent graphene layers. When paired with a commercial lithium cobalt oxide cathode, the silicon carbide-free graphene coating allows the full cell to reach volumetric energy densities of 972 and 700 Wh l−1 at first and 200th cycle, respectively, 1.8 and 1.5 times higher than those of current commercial lithium-ion batteries. This observation suggests that two-dimensional layered structure of graphene and its silicon carbide-free integration with silicon can serve as a prototype in advancing silicon anodes to commercially viable technology.
The volume expansion of silicon is a big problem in lithium-ion batteries with silicon anodes. Here, the authors report direct graphene growth on silicon nanoparticles, which effectively mitigates the problem, leading to excellent electrochemical performance.
doi:10.1038/ncomms8393
PMCID: PMC4491181  PMID: 26109057
10.  Excellent Temperature Performance of Spherical LiFePO4/C Composites Modified with Composite Carbon and Metal Oxides 
The Scientific World Journal  2014;2014:364327.
Nanosized spherical LiFePO4/C composite was synthesized from nanosized spherical FePO4·2H2O, Li2C2O4, aluminum oxide, titanium oxide, oxalic acid, and sucrose by binary sintering process. The phases and morphologies of LiFePO4/C were characterized using SEM, TEM, CV, EIS, EDS, and EDX as well as charging and discharging measurements. The results showed that the as-prepared LiFePO4/C composite with good conductive webs from nanosized spherical FePO4·2H2O exhibits excellent electrochemical performances, delivering an initial discharge capacity of 161.7 mAh·g−1 at a 0.1 C rate, 152.4 mAh·g−1 at a 1 C rate and 131.7 mAh·g−1 at a 5 C rate, and the capacity retention of 99.1%, 98.7%, and 95.8%, respectively, after 50 cycles. Meanwhile, the high and low temperature performance is excellent for 18650 battery, maintaining capacity retention of 101.7%, 95.0%, 88.3%, and 79.3% at 55°C, 0°C, −10°C, and −20°C by comparison withthat of room temperature (25°C) at the 0.5 C rate over a voltage range of 2.2 V to 3.6 V, respectively.
doi:10.1155/2014/364327
PMCID: PMC3913080  PMID: 24526888
11.  Dynamics of Electrochemical Lithiation/Delithiation of Graphene-Encapsulated Silicon Nanoparticles Studied by In-situ TEM 
Scientific Reports  2014;4:3863.
The incorporation of nanostructured carbon has been recently reported as an effective approach to improve the cycling stability when Si is used as high-capacity anodes for the next generation Li-ion battery. However, the mechanism of such notable improvement remains unclear. Herein, we report in-situ transmission electron microscopy (TEM) studies to directly observe the dynamic electrochemical lithiation/delithiation processes of crumpled graphene-encapsulated Si nanoparticles to understand their physical and chemical transformations. Unexpectedly, in the first lithiation process, crystalline Si nanoparticles undergo an isotropic to anisotropic transition, which is not observed in pure crystalline and amorphous Si nanoparticles. Such a surprising phenomenon arises from the uniformly distributed localized voltage around the Si nanoparticles due to the highly conductive graphene sheets. It is observed that the intimate contact between graphene and Si is maintained during volume expansion/contraction. Electrochemical sintering process where small Si nanoparticles react and merge together to form large agglomerates following spikes in localized electric current is another problem for batteries. In-situ TEM shows that graphene sheets help maintain the capacity even in the course of electrochemical sintering. Such in-situ TEM observations provide valuable phenomenological insights into electrochemical phenomena, which may help optimize the configuration for further improved performance.
doi:10.1038/srep03863
PMCID: PMC3900994  PMID: 24457519
12.  High energy density rechargeable magnesium battery using earth-abundant and non-toxic elements 
Scientific Reports  2014;4:5622.
Rechargeable magnesium batteries are poised to be viable candidates for large-scale energy storage devices in smart grid communities and electric vehicles. However, the energy density of previously proposed rechargeable magnesium batteries is low, limited mainly by the cathode materials. Here, we present new design approaches for the cathode in order to realize a high-energy-density rechargeable magnesium battery system. Ion-exchanged MgFeSiO4 demonstrates a high reversible capacity exceeding 300 mAh·g−1 at a voltage of approximately 2.4 V vs. Mg. Further, the electronic and crystal structure of ion-exchanged MgFeSiO4 changes during the charging and discharging processes, which demonstrates the (de)insertion of magnesium in the host structure. The combination of ion-exchanged MgFeSiO4 with a magnesium bis(trifluoromethylsulfonyl)imide–triglyme electrolyte system proposed in this work provides a low-cost and practical rechargeable magnesium battery with high energy density, free from corrosion and safety problems.
doi:10.1038/srep05622
PMCID: PMC4092329  PMID: 25011939
13.  Rapid continuous synthesis of spherical reduced graphene ball-nickel oxide composite for lithium ion batteries 
Scientific Reports  2014;4:5786.
In this study, we synthesized a powder consisting of core-shell-structured Ni/NiO nanocluster-decorated graphene (Ni/NiO-graphene) by a simple process for use as an anodic material for lithium-ion batteries. First, a crumpled graphene powder consisting of uniformly distributed Ni nanoclusters was prepared by one-pot spray pyrolysis. This powder was subsequently transformed into the Ni/NiO-graphene composite by annealing at 300°C in air. The Ni/NiO-graphene composite powder exhibited better electrochemical properties than those of the hollow-structured NiO-Ni composite and pure NiO powders. The initial discharge and charge capacities of the Ni/NiO-graphene composite powder were 1156 and 845 mA h g−1, respectively, and the corresponding initial coulombic efficiency was 73%. The discharge capacities of the Ni/NiO-graphene, NiO-Ni, and pure NiO powders after 300 cycles were 863, 647, and 439 mA h g−1, respectively. The high stability of the Ni/NiO-graphene composite powder, attributable to the unique structure of its particles, resulted in it exhibiting long-term cycling stability even at a current density of 1500 mA g−1, as well as good rate performance. The structural stability of the Ni/NiO-graphene composite powder particles during cycling lowered the charge transfer resistance and improved the Li-ion diffusion rate.
doi:10.1038/srep05786
PMCID: PMC4148662  PMID: 25167932
14.  Lithium ion storage between graphenes 
Nanoscale Research Letters  2011;6(1):203.
In this article, we investigate the storage of lithium ions between two parallel graphene sheets using the continuous approximation and the 6-12 Lennard-Jones potential. The continuous approximation assumes that the carbon atoms can be replaced by a uniform distribution across the surface of the graphene sheets so that the total interaction potential can be approximated by performing surface integrations. The number of ion layers determines the major storage characteristics of the battery, and our results show three distinct ionic configurations, namely single, double, and triple ion forming layers between graphenes. The number densities of lithium ions between the two graphenes are estimated from existing semi-empirical molecular orbital calculations, and the graphene sheets giving rise to the triple ion layers admit the largest storage capacity at all temperatures, followed by a marginal decrease of storage capacity for the case of double ion layers. These two configurations exceed the maximum theoretical storage capacity of graphite. Further, on taking into account the charge-discharge property, the double ion layers are the most preferable choice for enhanced lithium storage. Although the single ion layer provides the least charge storage, it turns out to be the most stable configuration at all temperatures. One application of the present study is for the design of future high energy density alkali batteries using graphene sheets as anodes for which an analytical formulation might greatly facilitate rapid computational results.
doi:10.1186/1556-276X-6-203
PMCID: PMC3211259  PMID: 21711713
15.  Graphene wrapped ordered LiNi0.5Mn1.5O4 nanorods as promising cathode material for lithium-ion batteries 
Scientific Reports  2015;5:11958.
LiNi0.5Mn1.5O4 nanorods wrapped with graphene nanosheets have been prepared and investigated as high energy and high power cathode material for lithium-ion batteries. The structural characterization by X-ray diffraction, Raman spectroscopy, and Fourier transform infrared spectroscopy indicates the LiNi0.5Mn1.5O4 nanorods prepared from β-MnO2 nanowires have ordered spinel structure with P4332 space group. The morphological characterization by scanning electron microscopy and transmission electron microscopy reveals that the LiNi0.5Mn1.5O4 nanorods of 100–200 nm in diameter are well dispersed and wrapped in the graphene nanosheets for the composite. Benefiting from the highly conductive matrix provided by graphene nanosheets and one-dimensional nanostructure of the ordered spinel, the composite electrode exhibits superior rate capability and cycling stability. As a result, the LiNi0.5Mn1.5O4-graphene composite electrode delivers reversible capacities of 127.6 and 80.8 mAh g−1 at 0.1 and 10 C, respectively, and shows 94% capacity retention after 200 cycles at 1 C, greatly outperforming the bare LiNi0.5Mn1.5O4 nanorod cathode. The outstanding performance of the LiNi0.5Mn1.5O4-graphene composite makes it promising as cathode material for developing high energy and high power lithium-ion batteries.
doi:10.1038/srep11958
PMCID: PMC4493710  PMID: 26148558
16.  Facile synthesis and electrochemical performances of hollow graphene spheres as anode material for lithium-ion batteries 
Nanoscale Research Letters  2014;9(1):368.
The hollow graphene oxide spheres have been successfully fabricated from graphene oxide nanosheets utilizing a water-in-oil emulsion technique, which were prepared from natural flake graphite by oxidation and ultrasonic treatment. The hollow graphene oxide spheres were reduced to hollow graphene spheres at 500°C for 3 h under an atmosphere of Ar(95%)/H2(5%). The first reversible specific capacity of the hollow graphene spheres was as high as 903 mAh g-1 at a current density of 50 mAh g-1. Even at a high current density of 500 mAh g-1, the reversible specific capacity remained at 502 mAh g-1. After 60 cycles, the reversible capacity was still kept at 652 mAh g-1 at the current density of 50 mAh g-1. These results indicate that the prepared hollow graphene spheres possess excellent electrochemical performances for lithium storage. The high rate performance of hollow graphene spheres thanks to the hollow structure, thin and porous shells consisting of graphene sheets.
PACS
81.05.ue; 61.48.Gh; 72.80.Vp
doi:10.1186/1556-276X-9-368
PMCID: PMC4119061  PMID: 25114657
Lithium-ion batteries; Hollow graphene spheres; Electrochemical performance; Cycle performance
17.  Large and fast reversible Li-ion storages in Fe2O3-graphene sheet-on-sheet sandwich-like nanocomposites 
Scientific Reports  2013;3:3502.
Fe2O3 nanosheets and nanoparticles are grown on graphene by simply varying reaction solvents in a facile solvothermal/hydrothermal preparation. Fe2O3 nanosheets are uniformly dispersed among graphene nanosheets, forming a unique sheet-on-sheet nanostructure. Due to the structure affinity between two types of two dimensional nanostructures, graphene nanosheets are separated better by Fe2O3 nanosheets compared to nanoparticles and their agglomeration is largely prevented. A large surface area of 173.9 m2 g−1 is observed for Fe2O3-graphene sheet-on-sheet composite, which is more than two times as large as that of Fe2O3-graphene particle-on-sheet composite (81.5 m2 g−1). The sheet-on-sheet composite is found to be better suitable as an anode for Li-ion battery. A high reversible capacity of 662.4 mAh g−1 can be observed after 100 cycles at 1000 mA g−1. The substantially improved cycling performance is ascribed to the unique structure affinity between Fe2O3 nanosheets and graphene nanosheets, thus offering complementary property improvement.
doi:10.1038/srep03502
PMCID: PMC3863982  PMID: 24336301
18.  In situ catalytic growth of large-area multilayered graphene/MoS2 heterostructures 
Scientific Reports  2014;4:4673.
Stacking various two-dimensional atomic crystals on top of each other is a feasible approach to create unique multilayered heterostructures with desired properties. Herein for the first time, we present a controlled preparation of large-area graphene/MoS2 heterostructures via a simple heating procedure on Mo-oleate complex coated sodium sulfate under N2 atmosphere. Through a direct in situ catalytic reaction, graphene layer has been uniformly grown on the MoS2 film formed by the reaction of Mo species with S pecies, which is from the carbothermal reduction of sodium sulfate. Due to the excellent graphene “painting” on MoS2 atomic layers, the significantly shortened lithium ion diffusion distance and the markedly enhanced electronic conductivity, these multilayered graphene/MoS2 heterostructures exhibit high specific capacity, unprecedented rate performance and outstanding cycling stability, especially at a high current density, when used as an anode material for lithium batteries. This work provides a simple but efficient route for the controlled fabrication of large-area multilayered graphene/metal sulfide heterostructures with promising applications in battery manufacture, electronics or catalysis.
doi:10.1038/srep04673
PMCID: PMC3985074  PMID: 24728289
19.  Fabrication of high-quality graphene oxide nanoscrolls and application in supercapacitor 
We reported a simple and effective way of fabricating one-dimensional (1D) graphene oxide nanoscrolls (GONS) from graphene oxide (GO) sheets through shock cooling by liquid nitrogen. The corresponding mechanism of rolling was proposed. One possibility is the formation of ice crystals during the shock cooling process in liquid nitrogen to be the driving force. The other might be due to the uneven stress of the sheets inside or outside ice during the lyophilization. After reducing, graphene nanoscrolls (GNS) exhibited good structural stability, high specific surface area, and high specific capacitance. The capacitance properties were investigated by cyclic voltammetry, galvanostatic charge-discharge, and electrical impedance spectroscopy. A specific capacity of 156 F/g for the GNS at the current density of 1.0 A/g was obtained comparing with the specific capacity of 108 F/g for graphene sheets. Those results indicated that GNS-based rolling structure could be a kind of promising electrode material for supercapacitors and batteries.
doi:10.1186/s11671-015-0894-3
PMCID: PMC4420763  PMID: 25977663
81.07.De (Nanotubes); 81.16.Be (Chemical synthesis methods); 62.23.Hj (Nanowires); 72.80.Vp (Graphene electronic transport); Graphene nanoscrolls; Shock cooling; Supercapacitors
20.  Electrodeposition of porous graphene networks on nickel foams as supercapacitor electrodes with high capacitance and remarkable cyclic stability 
Abstract
We describe a facile, low-cost, and green method to fabricate porous graphene networks/nickel foam (PG/NF) electrodes by electrochemical deposition of graphene sheets on nickel foams (NFs) for the application of supercapacitor electrodes. The electrodeposition process was accomplished by electrochemical reduction of graphene oxide (GO) in its aqueous suspension. The resultant binder-free PG/NF electrodes exhibited excellent double-layer capacitive performance with a high rate capability and a high specific capacitance of 183.2 mF cm-2 at the current density of 1 mA cm-2. Moreover, the specific capacitance maintains nearly 100% over 10,000 charge-discharge cycles, demonstrating a remarkable cyclic stability of these porous supercapacitor electrodes.
PACS
82.47.Uv (Electrochemical capacitors); 82.45.Fk (Electrodes electrochemistry); 81.05.Rm (Fabrication of porous materials)
Electronic supplementary material
The online version of this article (doi:10.1186/1556-276X-9-672) contains supplementary material, which is available to authorized users.
doi:10.1186/1556-276X-9-672
PMCID: PMC4493843  PMID: 26089003
Graphene; Porous; Electrodeposition; Nickel foam; Crumpled morphology; Supercapacitor; Electrode
21.  Hollow Porous SiO2 Nanocubes Towards High-performance Anodes for Lithium-ion Batteries 
Scientific Reports  2013;3:1568.
The high theoretical capacity and low discharge potential of silicon have attracted much attention on Si-based anodes. Herein, hollow porous SiO2 nanocubes have been prepared via a two-step hard-template process and evaluated as electrode materials for lithium-ion batteries. The hollow porous SiO2 nanocubes exhibited a reversible capacity of 919 mAhg−1 over 30 cycles. The reasonable property could be attributed to the unique hollow nanostructure with large volume interior and numerous crevices in the shell, which could accommodate the volume change and alleviate the structural strain during Li ions' insertion and extraction, as well as allow rapid access of Li ions during charge/discharge cycling. It is found that the formation of irreversible or reversible lithium silicates in the anodes determines the capacity of a deep-cycle battery, fast transportation of Li ions in hollow porous SiO2 nanocubes is beneficial to the formation of Li2O and Si, contributing to the high reversible capacity.
doi:10.1038/srep01568
PMCID: PMC3610094  PMID: 23535780
22.  Low-cost carbon-silicon nanocomposite anodes for lithium ion batteries 
Nanoscale Research Letters  2014;9(1):360.
The specific energy of the existing lithium ion battery cells is limited because intercalation electrodes made of activated carbon (AC) materials have limited lithium ion storage capacities. Carbon nanotubes, graphene, and carbon nanofibers are the most sought alternatives to replace AC materials but their synthesis cost makes them highly prohibitive. Silicon has recently emerged as a strong candidate to replace existing graphite anodes due to its inherently large specific capacity and low working potential. However, pure silicon electrodes have shown poor mechanical integrity due to the dramatic expansion of the material during battery operation. This results in high irreversible capacity and short cycle life. We report on the synthesis and use of carbon and hybrid carbon-silicon nanostructures made by a simplified thermo-mechanical milling process to produce low-cost high-energy lithium ion battery anodes. Our work is based on an abundant, cost-effective, and easy-to-launch source of carbon soot having amorphous nature in combination with scrap silicon with crystalline nature. The carbon soot is transformed in situ into graphene and graphitic carbon during mechanical milling leading to superior elastic properties. Micro-Raman mapping shows a well-dispersed microstructure for both carbon and silicon. The fabricated composites are used for battery anodes, and the results are compared with commercial anodes from MTI Corporation. The anodes are integrated in batteries and tested; the results are compared to those seen in commercial batteries. For quick laboratory assessment, all electrochemical cells were fabricated under available environment conditions and they were tested at room temperature. Initial electrochemical analysis results on specific capacity, efficiency, and cyclability in comparison to currently available AC counterpart are promising to advance cost-effective commercial lithium ion battery technology. The electrochemical performance observed for carbon soot material is very interesting given the fact that its production cost is away cheaper than activated carbon. The cost of activated carbon is about $15/kg whereas the cost to manufacture carbon soot as a by-product from large-scale milling of abundant graphite is about $1/kg. Additionally, here, we propose a method that is environmentally friendly with strong potential for industrialization.
doi:10.1186/1556-276X-9-360
PMCID: PMC4112838  PMID: 25114651
Nanostructured carbon; Carbon-silicon nanocomposite; Anode materials; Lithium ion batteries; Electrochemical energy storage; Ball milling technique
23.  Stable Cycling of SiO2 Nanotubes as High-Performance Anodes for Lithium-Ion Batteries 
Scientific Reports  2014;4:4605.
Herein, SiO2 nanotubes have been fabricated via a facile two step hard-template growth method and evaluated as an anode for Li-ion batteries. SiO2 nanotubes exhibit a highly stable reversible capacity of 1266 mAhg−1 after 100 cycles with negligible capacity fading. SiO2 NT anodes experience a capacity increase throughout the first 80 cycles through Si phase growth via SiO2 reduction. The hollow morphology of the SiO2 nanotubes accommodates the large volume expansion experienced by Si-based anodes during lithiation and promotes preservation of the solid electrolyte interphase layer. The thin walls of the SiO2 nanotubes allow for effective reduction in Li-ion diffusion path distance and, thus, afford a favorable rate cyclability. The high aspect ratio character of these nanotubes allow for a relatively scalable fabrication method of nanoscale SiO2-based anodes.
doi:10.1038/srep04605
PMCID: PMC3986728  PMID: 24732245
24.  High Energy Density Asymmetric Supercapacitor Based on NiOOH/Ni3S2/3D Graphene and Fe3O4/Graphene Composite Electrodes 
Scientific Reports  2014;4:7274.
The application of the composite of Ni3S2 nanoparticles and 3D graphene as a novel cathode material for supercapacitors is systematically investigated in this study. It is found that the electrode capacitance increases by up to 111% after the composite electrode is activated by the consecutive cyclic voltammetry scanning in 1 M KOH. Due to the synergistic effect, the capacitance and the diffusion coefficient of electrolyte ions of the activated composite electrode are ca. 3.7 and 6.5 times higher than those of the Ni3S2 electrode, respectively. Furthermore, the activated composite electrode exhibits an ultrahigh specific capacitance of 3296 F/g and great cycling stability at a current density of 16 A/g. To obtain the reasonable matching of cathode/anode electrodes, the composite of Fe3O4 nanoparticles and chemically reduced graphene oxide (Fe3O4/rGO) is synthesized as the anode material. The Fe3O4/rGO electrode exhibits the specific capacitance of 661 F/g at 1 A/g and excellent rate capability. More importantly, an asymmetric supercapacitor fabricated by two different composite electrodes can be operated reversibly between 0 and 1.6 V and obtain a high specific capacitance of 233 F/g at 5 mV/s, which delivers a maximum energy density of 82.5 Wh/kg at a power density of 930 W/kg.
doi:10.1038/srep07274
PMCID: PMC4250917  PMID: 25449978
25.  Ultrasmall SnO2 Nanocrystals: Hot-bubbling Synthesis, Encapsulation in Carbon Layers and Applications in High Capacity Li-Ion Storage 
Scientific Reports  2014;4:4647.
Ultrasmall SnO2 nanocrystals as anode materials for lithium-ion batteries (LIBs) have been synthesized by bubbling an oxidizing gas into hot surfactant solutions containing Sn-oleate complexes. Annealing of the particles in N2 carbonifies the densely packed surface capping ligands resulting in carbon encapsulated SnO2 nanoparticles (SnO2/C). Carbon encapsulation can effectively buffer the volume changes during the lithiation/delithiation process. The assembled SnO2/C thus deliver extraordinarily high reversible capacity of 908 mA·h·g−1 at 0.5 C as well as excellent cycling performance in the LIBs. This method demonstrates the great potential of SnO2/C nanoparticles for the design of high power LIBs.
doi:10.1038/srep04647
PMCID: PMC3986698  PMID: 24732294

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