Boosted Aluminum Storage Performance by d-p Orbital Modulation in Zinc Selenide with Manganese Element Dopants

Abstract

Transition metal chalcogenides (TMCs) are extensively employed as cathode materials for rechargeable aluminum batteries (RABs) due to their high theoretical specific capacity and voltage plateau. Although promising, practical applications are hindered by challenges such as inferior structure stability, slow reaction kinetics, and inadequate electronic conductivity. Herein, Mn-ion doping engineering and g-C3N4 etched porous carbon frameworks (Mn-ZnSe@CNPC) were integrated to synergistically enhance the electrochemical properties of ZnSe. Through modulating the center of the d- and p-band and regulating electronic interaction, Mn-ion doping enhances the adsorption for solvent groups and reduces electron transfer energy barriers, resulting in Mn-ZnSe@CNPC cathodes with high redox activity and fast reaction kinetics. In addition, the porous carbon nanocages act as support frameworks, preventing the agglomeration of ZnSe nanoparticles and providing ample ion transport channels, thus addressing issues related to poor cyclability and slow electrochemical kinetics in RABs. Benefiting from the d-p orbital modulation strategy and structural advantages, the tailored Mn-ZnSe@CNPC cathode exhibits boosted electrochemical performance and excellent stability.