Self‐Supporting Metal‐Organic Framework Electrocatalysts for High‐Current‐Density Alkaline Water Splitting ^†

Comprehensive Summary Electrochemical water splitting is vital to green and sustainable hydrogen production. Electrocatalysts with high efficiency and robust stability under high‐current‐densities play an essential role in industrial implementation of this technology. Self‐supporting metal‐organic framework materials have attracted intensive attention as promising electrocatalysts under high‐current‐densities due to their large surface area, adjustable compositions, accessible active sites, effective mass and electron transport. This review summarizes the recent advances in developing self‐supporting pristine MOF‐based electrocatalysts for high‐current‐densities water electrolysis. First, the fundamentals of water electrolysis and the key aspects for producing electrocatalysts under high‐current‐density are introduced. Then, the architectural advantages and preparation strategies of self‐supporting MOFs are highlighted. Finally, methods dedicated to enhancing high‐current‐densities activity are discussed, which involve key strategies such as electronic structure tuning, ligand engineering, interface engineering, defect construction, and single atom design. The challenges and development prospects associated with the future industrial water electrolysis are also discussed. Key Scientists