Tailoring Materials Design for Aqueous Energy Storage and Conversion through Electrochemical Reconstruction

The growing demand for renewable energy has spurred the development of efficient electrochemical systems. Transition metal-based materials serve as key electrode materials due to their tunable structures and redox activity, with electrochemical reconstruction playing a critical role in modulation of their properties. A deep understanding of the evolution of active sites and local environments is essential for the rational design of energy materials. Focusing on aqueous energy storage and water splitting, this review discusses the behaviors, mechanisms, and thermodynamics of electrochemical reconstruction. It systematically summarizes recent advances in material design through electrochemical reconstruction across six aspects: doping, defects, active centers, high-valence sites, heterostructures, and electrode/electrolyte interfaces. A connection is established among the reconstruction techniques, the nature of active species, and the corresponding electrochemical behaviors. We also highlight milestone discoveries in reconstruction guided by external fields and the starting topology, alongside <i>in situ</i>/<i>operando</i> techniques for probing dynamic processes. Furthermore, we outline the growing role of artificial intelligence (AI)-driven methods in facilitating material discovery and process optimization, emphasizing the underlying principles of scientific synthesis and analysis. Besides, we discuss the remaining challenges and offer new insights, aiming to inspire future research in machine-learning-assisted design and fabrication of advanced materials for energy storage and conversion.