Graphene or chemically modified graphene, because of its high specific surface area and abundant functional groups, provides an ideal template for the controllable growth of metal-organic framework (MOF) particles. The nanocomposite assembled from graphene and MOFs can effectively overcome the limitations of low stability and poor conductivity of MOFs, greatly widening their application in the field of electrochemistry. Furthermore, it can also be utilized as a versatile precursor due to the tunable structure and composition for various derivatives with sophisticated structures, showing their unique advantages and great potential in many applications, especially energy storage and conversion. Therefore, the related studies have been becoming a hot research topic and have achieved great progress. This review summarizes comprehensively the latest methods of synthesizing MOFs/graphene and their derivatives, and their application in energy storage and conversion with a detailed analysis of the structure-property relationship. Additionally, the current challenges and opportunities in this field will be discussed with an outlook also provided.

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Recent progress in metal-organic framework/graphene-derived materials for energy storage and conversion: design, preparation, and application.

Advances and perspectives of ZIFs-based materials for electrochemical energy storage: Design of synthesis and crystal structure, evolution of mechanisms and electrochemical performance

There is an urgent need to develop improved anode materials for lithium-ion batteries (LIBs). Herein, we report the synthesis of a graphene quantum dots (GQDs)-coated hierarchical nanoflake-based CuO microspheres (H–CuO) composite on Cu foam via a one-pot hydrothermal technique for use as a binder-free anode for LIBs. The carboxyl-functionalized GQD coating on H–CuO not only results in lower charge-transfer resistance and enhanced electrical conductivity but also prevents the dissolution and agglomeration of the electrode. The GQDs/H–CuO composite anode exhibits a reversible capacity as high as 609 mAh g−1 (pristine H–CuO: 61 mAh g−1) after 200 cycles at 0.2 A g−1. It also shows long-term cycling stability, exhibiting a capacity retention rate of 79.4% after 1000 cycles (pristine H–CuO: 0.7%) at a high current density (2 A g−1) and improved initial coulombic efficiency at 88.2% (pristine H–CuO: 75.2%). The superior electrochemical properties of the GQDs/H–CuO composite anode are attributable to the graphene networks, which help maintain a high specific surface area and effectively protect the anodic active material from forming an unstable solid electrolyte interface layer. The proposed strategy for fabricating the GQD-coated metal oxide microsphere-based anode should contribute to the development of next-generation LIBs with improved electrochemical performance.

Synthesis of graphene quantum dots-coated hierarchical CuO microspheres composite for use as binder-free anode for lithium-ion batteries

Metal oxides have been regarded as promising next-generation anode materials for rechargeable lithium ion batteries; however, their poor stability, which is caused by large volume changes during repeated lithiation/delithiation, remains a challenge. Here, conformally encapsulated low-oxidation state oxide cubes with reduced graphene oxide (RGO) obtained via a new pressurized reduction consisting of external mechanical compression and internal thermokinetic reduction from highly porous metal oxides/RGO aerogel (RGOA) are reported. Using single crystalline (SC) cobalt oxides and iron oxide cubes as model systems, the SC-Co3O4 or Fe2O3 cube/RGOA are pressurized into compacted xerogel along with a uniform thermokinetic reduction, which result in topotactic transformation to core-shelled CoO/RGO or Fe3O4@RGO cubes. The SC-CoO and SC-Fe3O4 cubes isolated perfectly in the RGO shells have dramatically improved their cycling stabilities for lithium ion storage to hundreds of times.

Core-Shelled Low-Oxidation State Oxides@Reduced Graphene Oxides Cubes Via Pressurized Reduction for Highly Stable Lithium Ion Storage

Two-dimensional carbon-based composite nanosheets (2D-CCNSs) are expected to be promising electrodes for fast charging lithium-ion batteries. Even though synthesis procedures exist for these materials, current approaches often require rigid reaction conditions and complicated synthetic steps. Herein, we develop a facile and general approach to fabricate a new type of 2D-CCNSs and demonstrate its superiority as a high-rate anode for lithium-ion batteries. It is found that the introduction of a nanocellulose as building unit can guide itself to self-assemble with polydopamine and metal ions to form a 2D inorganic–organic hybrid, which can be directly transformed into 2D-CCNSs after a carbonization treatment without structural deterioration. Unlike common 2D-CCNSs with a pure graphitic or amorphous carbon framework, the as-constructed materials possess a distinctively heterogeneous carbonaceous skeleton comprising graphitic nanorods with a crystalline framework and amorphous carbon with a microporous structure. The synthetic strategy is also demonstrated to be general for embedding numerous metal oxides, such as Fe2O3, CoO, NiO nanoparticles, into the carbon framework just by adjusting the types of metal ions. Profiting from the well-orchestrated structure, the as-prepared 2D-CCNSs exhibit impressive high-rate lithium ion storage performance. For instance, after being fully charged within 40.8 s, a long discharge time as high as 342 min can be achieved accompanied with a high and stable reversible capacity of 560 mA h g−1.

A general strategy for metal oxide nanoparticles embedded into heterogeneous carbon nanosheets as high-rate lithium-ion battery anodes

Multi-component hierarchical hollow Co–Mo–O nanocages anchored on reduced graphene oxide with strong interfacial interaction for lithium-ion batteries

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Multi-component hierarchical hollow Co–Mo–O nanocages anchored on reduced graphene oxide with strong interfacial interaction for lithium-ion batteries