Cation leaching and congenetic oxyanion adsorption of amorphous high-entropy LDH for promoting water/seawater oxidation

doi:10.1016/j.jmst.2025.03.047

Abstract

Abstract: Water/seawater oxidation determines the hydrogen production efficiency of water/seawater splitting. Developing high-efficiency, conductive, stable, and erosion-resisting transition metal-based layered double hydroxide (TM-LDH) is crucial to water/seawater oxidation. Hence, amorphous high-entropy FeCoNiCr-LDH is fabricated by one-step electrodeposition to promote water/seawater oxidation. Coupling of high entropy, Cr cation leaching, congenetic CrO₄^2- adsorption, and amorphization to facilitate electrochemical reconstruction. The advanced strategy enhances active sites, reaction kinetics, reaction selectivity, conductivity, stability, and corrosion resistance with the electrostatic chlorine-repellent layer. The in-situ Cr leaching and congenetic CrO₄^2- adsorption-induced electrochemical reconstruction are identified by cyclic voltammetry (CV) activation, in-situ Bode plots, and electrochemical impedance spectroscopy (EIS) plots, ex-situ Raman and ultraviolet-visible spectrophotometry (UV-Vis). The OER active species of oxyhydroxides are also formed during electrochemical reconstruction. Moreover, control tests of soaking and extra CrO₄^2- additive verify the superiorities of electrochemical reconstruction with in-situ Cr leaching and congenetic CrO₄^2- adsorption. Accordingly, FeCoNiCr-LDH exhibits excellent electrochemical performances with low overpotentials of 193/225 mV at 10 mA cm^-2, high Faradaic efficiencies of 99.3 %/97.4 % and strong stability for alkaline water/simulated seawater oxidation, respectively. This study provides one innovative strategy to construct efficient water/seawater oxidation electrocatalysts, showing the great theoretical significance and practical values in industrial water/seawater splitting for hydrogen production.

Key words: Amorphous high-entropy LDH, Water/seawater oxidation, Cation leaching, Congenetic oxyanion adsorption, Electrochemical reconstruction

Han-Ming Zhang, Min Yao, Zhengyu Yong, Yali Li, Junxia Guo, Jinfeng Sun. Cation leaching and congenetic oxyanion adsorption of amorphous high-entropy LDH for promoting water/seawater oxidation[J]. J. Mater. Sci. Technol., 2025, 238: 199-208.

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