We study the synthesis, electrochemical and mechanical performance of layered freestanding papers composed of acid exfoliated few layer molybdenum disulfide (MoS 2 ) and reduced graphene oxide (rGO) flakes for use as a self-standing flexible electrode in sodium ion batteries. Synthesis was achieved through vacuum filtration of homogenous dispersions consisting of varying wt. % of acid treated MoS 2 flakes in GO in DI water, followed by thermal reduction at elevated temperatures. The electrochemical performance of the crumpled composite paper (at 4 mg.cm -2 ) was evaluated as counter electrode against pure Na foil in a half-cell configuration. The electrode showed good Na cycling ability with a stable charge capacity of approx.230 mAh.g -1 with respect to total weight of the electrode with coulombic efficiency reaching approx. 99 %. In addition, static uniaxial tensile tests performed on crumpled composite papers showed high average strain to failure reaching approx. %.KEYWORDS: TMDC, sodium battery, freestanding electrode, graphene, MoS 2 2 Lithium ion batteries (LIBs) have been extensively studied for energy-storage applications like portable electronic devices and electric vehicles. [1][2][3] However, concerns over the cost, safety and availability of Li reserves 4 for large-scale applications involving renewable energy integration and the electrical grid have to be answered. In this regard, sodium ion batteries (SIBs) have drawn increasing attention because in contrast to lithium, 5-7 sodium resources are practically inexhaustible and evenly distributed around the world while the ion insertion chemistry is largely identical to that of lithium. Also, from electrochemical point of view, sodium has a very negative redox potential (-2.71 V, vs. SHE) and a small electrochemical equivalent (0.86 gAh -1 ), which make it the most advantageous element for battery applications after lithium. However, many challenges remain before SIBs can become commercially competitive with LIBs. For instance, Na ions are about 55% larger in radius than Li-ions, which makes it difficult to find a suitable host material to allow reversible and rapid ion insertion and extraction. 8 To this end, researchers have proposed a number of high-capacity sodium host materials (negative electrode) involving either carbon or group IVA and VA elements that form intermetallic compounds with Na. [9][10][11][12][13] The alloying compounds demonstrate high first cycle Na-storage capacities, such as Na 15 Sn 4 (847 mAhg -1 ), Na 15 Pb 4 (485 mAhg -1 ), Na 3 Sb (600 mAhg -1 ) and Na 3 P (2560 mAhg -1 ), respectively. However, this comes at the cost of very high volume change upon Na-insertion (as much as 500 % in some cases), resulting in formation of internal cracks, loss of electrical contact, and eventual failure of the electrode (particularly for thick electrodes). 14 Novel nanostructured designs that can accommodate large volumetric strains need further exploration. [15][16][17][18] For carbon-based electrode materials, much of the emphasis ...

Separation of bulk tungsten disulfide (or WS2) into few-layer two-dimensional (2-D) crystals is of interest because of their high surface area for certain chemical processes and size-dependent optical and electronic characteristics. Herein, we demonstrate a process that involves the physical separation of weakly bonded WS2 layers by use of a strong acid treatment (chlorosulfonic acid) at 2 mg/mL, followed by quenching in deionized (DI) water. X-ray photoelectron spectroscopy of the superacid-treated WS2 suggests the formation of W-O type bonds, signifying oxidation of tungsten and reduction of the sulfur phase. Thermogravimetric analysis showed a three-phase weight-loss pattern, suggesting acid functionalization of WS2 surfaces. We also studied the electrochemical behavior of an acid-treated WS2 anode in a lithium half-cell configuration that showed a three-step charge-discharge behavior, characteristic of a conversion reaction. The electrochemical capacity was 118 mAh/g after 50 cycles.

Silicon and graphene are promising anode materials for lithium-ion batteries because of their high theoretical capacity; however, low volumetric energy density, poor efficiency and instability in high loading electrodes limit their practical application. Here we report a large area (approximately 15 cm × 2.5 cm) self-standing anode material consisting of molecular precursor-derived silicon oxycarbide glass particles embedded in a chemically-modified reduced graphene oxide matrix. The porous reduced graphene oxide matrix serves as an effective electron conductor and current collector with a stable mechanical structure, and the amorphous silicon oxycarbide particles cycle lithium-ions with high Coulombic efficiency. The paper electrode (mass loading of 2 mg cm−2) delivers a charge capacity of ∼588 mAh g−1electrode (∼393 mAh cm−3electrode) at 1,020th cycle and shows no evidence of mechanical failure. Elimination of inactive ingredients such as metal current collector and polymeric binder reduces the total electrode weight and may provide the means to produce efficient lightweight batteries.

We demonstrate the synthesis and electrochemical performance of polymer-derived silicon oxycarbide−carbon nanotube (SiOC−CNT) composites as a stable lithium intercalation material for secondary battery applications. Composite synthesis was achieved through controlled thermal decomposition of 1,3,5,7-tetramethyl 1,3,5,7-tetravinyl cyclotetrasiloxane (TTCS) precursor on carbon nanotubes surfaces that resulted in formation of shell/core type ceramic SiOC−CNT architecture. Li-ion battery anode (prepared at a loading of ∼1.0 mg cm −2 ) showed stable charge capacity of 686 mA h g −1 even after 40 cycles. The average Coulombic efficiency (excluding the first cycle loss) was 99.6%. Further, the post electrochemical imaging of the dissembled cells showed no apparent damage to the anode surface, highlighting improved chemical and mechanical stability of these composites. A similar trend was observed in the rate capability tests, where the SiOC−CNT anode (with 5 wt % loading in TTCS) again showed stable performance, completely recovering the first cycle capacity of ∼750 mA h g −1 when the current density was brought back to 50 mA g −1 after cycling at higher current densities.

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.