Morphology-controlled MoS2 nanosheets were successfully synthesized with the aid of graphene/acid coexistence by a one-pot hydrothermal method. The ultrathin MoS2 nanosheets were self-assembled into a cockscomb-like structure with an exposed (100) facet on graphene sheets, which is in strong contrast to large aggregate MoS2 plates grown freely on graphene sheets without acetic acid. The ultrathin MoS2 nanosheets displayed excellent rate performance for Li storage (709 mAh·g(-1) capacity at 8320 mA·g(-1) discharging rate) and superior charge/discharge cyclability.
A 2H-MoS2 (H=hexagonal) ultrathin nanomesh with high defect generation and large porosity is demonstrated to improving electrochemical performance, including in lithium-ion batteries (LIBs) and the hydrogen evolution reaction (HER), with the aid of a 3D reduced graphene oxide (RGO) scaffold as fast electron and ion channels. The 3D defect-rich MoS2 nanomesh/RGO foam (Dr-MoS2 Nm/RGO) can be easily obtained through a one-pot cobalt acetate/graphene oxide (GO) co-assisted hydrothermal reaction, in which GO, cobalt and acetate ions are co-morphology-controlling agents and defect inducers. As an anode material for LIBs, Dr-MoS2 Nm/RGO has only a 9% capacity decay at a 10 C discharge rate versus 0.2 C with stable cyclability at the optimized composition (5 wt% RGO to MoS2 and 2 mol% Co to Mo), and significantly achieves 810 mA h g(-1) at a high current density of 9.46 A g(-1) over at least 150 cycles. Moreover, Dr-MoS2 Nm/RGO exhibits superior activity for the HER with an overpotential as low as 80 mV and a Tafel slope of about 36 mV per decade. In contrast to the MoS2 nanosheet/RGO (MoS2 Ns/RGO), which is synthesized in the absence of cobalt ions, Dr-MoS2 Nm/RGO provides high interconnectivity for efficient lithium-ion transport, and rich defects as electrochemically active sites. DFT is used to prove the existence of rich defects due to anion replacement to become a Co-Mo-S atomic structure, releasing inert basal planes to active sites.
Surface carbon coating to improve the inherent poor electrical conductivity of lithium iron phosphate (LiFePO4, LFP) has been considered as most efficient strategy. Here, we also report one of the conventional methods for LFP but exhibiting a specific capacity beyond the theoretical value, ultrahigh rate performance, and excellent long-term cyclability: the specific capacity is 171.9 mAh/g (70 μm-thick electrode with ∼10 mg/cm(2) loading mass) at 0.1 C (17 mA/g) and retains 143.7 mAh/g at 10 C (1.7 A/g) and 95.8% of initial capacity at 10 C after 1000 cycles. It was found that the interior conformal N-C coating enhances the intrinsic conductivity of LFP nanorods (LFP NR) and the exterior reduced graphene oxide coating acts as an electrically conducting secondary network to electrically connect the entire electrode. The great electron transport mutually promoted with shorten Li diffusion length on (010) facet exposed LFP NR represents the highest specific capacity value recorded to date at 10 C and ultralong-term cyclability. This conformal carbon coating approach can be a promising strategy for the commercialization of LFP cathode in lithium ion batteries.
The electrodes in lithium-ion batteries (LIBs) are typically films that are arranged on metal foil current collectors with a thickness of several tens of μm. Here, we report on the preparation of a thick free-standing graphene film synthesized by CVD as an alternative to Cu foil as an anode current collector. As a model system, MoS2 anodes with a flower-like morphology were anchored onto the surface of the thick graphene film. A hybrid and binder free anode without a conventional metal current collector exhibited an excellent capacity value of around 580 mAh/g (@50 mA/g) and reasonable charge/discharge cyclability. The work presented here may stimulate the use of graphene films as replacements for conventional current collectors and additive free electrode in LIBs.
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