Bioinspired Homonuclear Diatomic Iron Active Site Regulation for Efficient Antifouling Osmotic Energy Conversion.

Abstract

Membrane-based reverse electrodialysis is globally recognized as a promising technology for harnessing osmotic energy. However, its practical application is greatly restricted by the poor anti-fouling ability of existing membrane materials. Inspired by the structural and functional models of natural cytochrome c oxidases (CcO), the first use of atomically precise homonuclear diatomic iron composites as high-performance osmotic energy conversion membranes with excellent anti-fouling ability is demonstrated. Through rational tuning of the atomic configuration of the diatomic iron sites, the oxidase-like activity can be precisely tailored, leading to the augmentation of ion throughput and anti-fouling capacity. Composite membranes featuring direct Fe-Fe motif configurations embedded within cellulose nanofibers (CNF/Fe-DACs-P) surpass state-of-the-art CNF-based membranes with power densities of ca. 6.7 W m^-2 and a 44.5-fold enhancement in antimicrobial performance. Combined, experimental characterization and density functional theory simulations reveal that homonuclear diatomic iron sites with metal-metal interactions can achieve ideally balanced adsorption and desorption of intermediates, thus realizing superior oxidase-like activity, enhanced ionic flux, and excellent antibacterial activity.