Orbital coupling effect enables low-chloride concentration electrolyte for four-electron redox in aqueous zinc | |iodine batteries - Nature
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AbstractThe I-/I0/I+ redox chemistry is hindered by the inherent instability of the electrophilic I+, which undergoes hydrolysis in aqueous media or is rapidly consumed by comproportionation with triiodide ions. Here, we design a copper single-atom embedded nitrogen-doped carbon host that synergistically combines d-p orbital hybridization and local low-concentration chloride ions to stabilize the I+. The atomic Cu-Nx sites interact moderately with iodine species through Cu d- and I p-orbital hybridization, which enhances iodine species adsorption, accelerates redox kinetics, and increases the hydrolysis energy barrier of I+. Simultaneously, the Cu-Nx sites promote a localized I-Cl microenvironment through electrostatic interaction, enabling efficient I0/I+ conversion even in a low-concentration Cl- ion electrolyte.
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