Abstract
The growing challenge of water scarcity has spurred extensive research into the development of advanced freestanding pseudocapacitive electrode materials. These electrodes, characterized by their controlled morphology, mechanical complexity, and enhanced desalination capabilities, are advancing water treatment technologies. Additionally, electrodes with interfacially influenced heterostructures demonstrate substantial potential to enhance electrochemical kinetics. However, their widespread adoption is hindered by intricate synthesis procedures and the necessity for multiple discrete components. Herein, the report introduces a cohesive approach that utilizes electrospinning and carbonization to create a freestanding, hierarchically porous nitrogen-doped carbon nanofiber network encapsulating FeNi3 alloy (FeNi3@CNFs) for desalination applications. The method enhances the interfacial effect, mitigates volume changes during sodium ion adsorption and desorption, and improves interfacial stability. By capitalizing on structural and compositional advantages, the novel FeNi3@CNFs electrode delivers outstanding electrochemical properties, including a high desalination capacity (46.47 mg g−1 at 1.2 V), rapid desalination rate (0.77 mg g−1 min−1), and enhanced cyclic durability. Computational analysis via Density Functional Theory shows that the work function prompts a surface charge redistribution at the FeNi3@CNFs heterojunction, optimizing the surface electronic structure and reducing the energy barrier for adsorption. The modification significantly boosts the diffusion kinetics of sodium adsorption. The study delineates a comprehensive methodology for fabricating high-performance heterostructured electrode materials that are effective for capacitive deionization.
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