2D metal–organic frameworks (2D MOFs) are promising templates for the fabrication of carbon supported 2D metal/metal sulfide nanocomposites. Herein, controllable synthesis of a newly developed 2D Ni‐based MOF nanoplates in well‐defined rectangle morphology is first realized via a pyridine‐assisted bottom‐up solvothermal treatment of NiSO4 and 4,4′‐bipyridine. The thickness of the MOF nanoplates can be controlled to below 20 nm, while the lateral size can be tuned in a wide range with different amounts of pyridine. Subsequent pyrolysis treatment converts the MOF nanoplates into 2D free‐standing nitrogen‐doped Ni‐Ni3S2@carbon nanoplates. The obtained Ni‐Ni3S2 nanoparticles encapsulated in the N‐doped carbon matrix exhibits high electrocatalytic activity in oxygen evolution reaction. A low overpotential of 284.7 mV at a current density of 10 mA cm−2 is achieved in alkaline solution, which is among the best reported performance of substrate‐free nickel sulfides based nanomaterials.

Single-layer LDH nanosheets serve as a free hydroxide ion donor and 2D hopping lane for superionic conduction.

Silicon (Si) has attracted intensive academic and commercial attention due to its extremely high theoretical capacity. However, it is still far away from practical application because of its fast capacity fading, which is caused by the huge volume change. Here, a novel network polymer binder is synthesized through in situ thermal crosslinking of water‐soluble carboxymethyl cellulose (CMC) and maleic anhydride (MAH). The as‐obtained polymer binder network can effectively restrict the huge volume change of Si anodes upon lithiation. Because of the significantly enhanced structural stability, the Si anodes with network polymer binder deliver enhanced electrochemical performance, with a capacity of 996 mAh g−1 at a high current density of 1 A g−1 after 120 cycles under high mass loading. Most importantly, a high average Coulomb efficiency (CE) of 99.4% is obtained, which is superior over the average CE (98.7%) of Si only using CMC as binder. It is considered that this novel 3D network cross‐linking binder can be used for high‐capacity anode materials in next‐generation Li‐ion batteries.

In this work, MoS2 nanosheets were obtained successfully using the liquid phase exfoliation method assisted by formamide solvothermal treatment. The exfoliation efficiency in N-methyl-2-pyrrolidone (NMP) was enhanced by the synergetic effect of easier intercalation of polar solvent and higher repulsive force of the treated bulk MoS2. The exfoliated MoS2 nanosheets were assembled alternately with H3Mo12O40P (PMo12) into a multilayer heterostructure by the layer-by-layer (LBL) method, in which PMo12 with high electron mobility bridges the adjacent catalytically active MoS2 layers. Based on the heterostructure, the electrocatalytic performance for hydrogen evolution was substantially enhanced over multilayer MoS2 nanosheets alone. Moreover, it was found that the electrocatalytic performance was influenced by the layer number, indicating that an optimum balance between the mass transfer (MoS2 layer) and electron conductivity (PMo12 layer) was needed for the construction of efficient electrocatalysts. In addition, the electrocatalytic performance of the multilayers (MoS2)n and (PMo12/MoS2)n could be improved by oxygen plasma treatment, which might be ascribed to the increased number of edges and defects in MoS2 nanosheets. This work not only provides a facile method to exfoliate MoS2 with higher efficiency, but also offers a feasible strategy to build up high-performance electrocatalysts by rationally assembling nanosheets and polyoxometalate species at the nanoscale level.