Metal–Organic Frameworks‐Derived Self‐Supported Carbon‐Based Composites for Electrocatalytic Water Splitting

Abstract Electrocatalytic water splitting has been considered as a promising strategy for the sustainable evolution of hydrogen energy and storage of intermittent electric energy. Efficient catalysts for electrocatalytic water splitting are urgently demanded to decrease the overpotentials and promote the sluggish reaction kinetics. Carbon‐based composites, including heteroatom‐doped carbon materials, metals/alloys@carbon composites, metal compounds@carbon composites, and atomically dispersed metal sites@carbon composites have been widely used as the catalysts due to their fascinating properties. However, these electrocatalysts are almost powdery form, and should be cast on the current collector by using the polymeric binder, which would result in the unsatisfied electrocatalytic performance. In comparison, a self‐supported electrode architecture is highly attractive. Recently, self‐supported metal–organic frameworks (MOFs) constructed by coordination of metal centers and organic ligands have been considered as suitable templates/precursors to construct free‐standing carbon‐based composites grown on conductive substrate. MOFs‐derived carbon‐based composites have various merits, such as the well‐aligned array architecture and evenly distributed active sites, and easy functionalization with other species, which make them suitable alternatives to non‐noble metal‐included electrocatalysts. In this review, we intend to show the research progresses by employment of MOFs as precursors to prepare self‐supported carbon‐based composites. Focusing on these MOFs‐derived carbon‐based nanomaterials, the latest advances in their controllable synthesis, composition regulation, electrocatalytic performances in hydrogen evolution reaction (HER), oxygen evolution reaction (OER), and overall water splitting (OWS) are presented. Finally, the challenges and perspectives are showed for the further developments of MOFs‐derived self‐supported carbon‐based nanomaterials in electrocatalytic reactions.