Regulating the Charge and Spin Ordering of Two-Dimensional Ultrathin Solids for Electrocatalytic Water Splitting

Electrocatalytic water splitting, which underpins a series of sustainable energy conversion technologies, has become even more relevant as our energy needs have increased. Exploring efficient non-precious-metal electrocatalysts is necessary for the widespread application of this energy storage model. Two-dimensional (2D) ultrathin solids with a special atomic and electronic structure are full of unlimited potential in the pursuit of high-efficiency electrocatalysts and have been identified as a perfect platform for establishing clear structure-property relationships. Hence, in this review, we first clear up the fundamental relationship between intrinsic charge and spin ordering and electrocatalytic properties. Then, on this basis, we summarize recent attempts to regulate electrical behavior and spin ordering in 2D ultrathin solids to optimize electrocatalytic water-splitting performance. In addition, we highlight the coupling relationship among lattice, charge, and spin ordering in ultrathin electrocatalysts. Finally, we also present some personal perspectives on the challenges and future research directions in this promising area.