Denitrification mechanism in oxygen-rich aquatic environments through long-distance electron transfer

Abstract The lack of electron donors in oxygen-rich aquatic environments limits the ability of natural denitrification to remove excess nitrate, leading to eutrophication of aquatic ecosystems. Herein, we demonstrate that electron-rich substances in river or lake sediments could participate in long-distance electron rebalancing to reduce nitrate in the overlying water. A microstructure containing Dechloromonas and consisting of an inner layer of green rust and an outer layer of lepidocrocite forms in the sediment-water system through synergetic evolution and self-assembly. The microstructure enables long-distance electron transfer from the sediment to dilute nitrate in the overlying water. Specifically, the inner green rust adsorbs nitrate and reduces the kinetic barrier for denitrification via an Fe(II)/Fe(III) redox mediator. Our study reveals the mechanism of spontaneous electron transfer between distant and dilute electron donors and acceptors to achieve denitrification in electron-deficient aquatic systems.