Blocking Effect Retards Electron Release from Asymmetric Active Units for Selective Seawater Oxidation
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摘要：During seawater electrolysis, chloride ion (Cl-) adsorption at the anode leads to an inevitable competitive chloride oxidation reaction (ClOR) with the oxygen evolution reaction (OER), compromising the long-term stability of the electrolysis process. Furthermore, Ni-based OER electrocatalysts are challenged by activity degradation due to the overoxidation of Ni3+. In response, we present a design of oxygen-vacancy-regulated asymmetric Nb-O-Ni bonds aimed at selective seawater oxidation. The experimental and in situ characterization results indicate that the blocking effect of oxygen vacancies effectively alleviates the electron release of Ni3+ and the electron enrichment of Nb5+ on asymmetric Nb-O-Ni bonds, achieving a stable and selective OER in alkaline seawater. Density functional theory (DFT) calculations reveal that oxygen vacancies in Nb-O-Ni bonds optimize the adsorption strength of reaction intermediates and break up the scaling relationship between *OH and *OOH intermediates. The constructed anion exchange membrane electrolysis cell achieves a cost efficiency of $1.07 per GGE (gasoline gallon equivalent) for H2 production at a current density of 1000 mA cm-2, maintaining operational stability for 100 h at 500 mA cm-2.
卷号：19
期号：9
是否译文：否
