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<p>Although layered double hydroxides (LDHs) have been substantially applied as catalysts for the elimination of dye pollutants, the mechanism of the process still needs to be fully understood. Herein, NiCo-LDH[X] catalysts with different Ni: Co ratios (X = 1:1, 1:2, and 1:3) were prepared via the coprecipitation method, and we explored their effectiveness in the activation of peroxymonosulfate (PMS) to achieve efficient degradation of methylene blue (MB). The effect of several parameters on the catalytic performance of NiCo-LDH[X] was systematically evaluated. Following thorough experimental investigations, the activation mechanism and MB degradation pathways were proposed. Among the different NiCo-LDH[X] catalysts, NiCo-LDH[1:2] showed methylene blue degradation performance. Experimental results showed that this catalyst achieved MB degradation efficiency of 97.2% within 12&#xa0;min, and a total organic carbon removal rate of 67.1% within 60 min, while exhibiting remarkable adaptability, reusability, and stability, as confirmed by post-catalytic characterization. Radical scavenging studies identified superoxide radicals (O<sub>2</sub><sup>·−</sup>), sulfate radicals (SO<sub>4</sub><sup>·−</sup>), and singlet oxygen (<sup>1</sup>O<sub>2</sub>) as the primary reactive oxygen species generated in the NiCo-LDH[1:2]/PMS system. The results of X-ray photoelectron spectroscopy (XPS) analysis clarified the roles of oxygen vacancies and Co sites as active sites, demonstrating the reversible redox behavior of NiCo-LDH[1:2] through Ni<sup>2+</sup>/Ni<sup>3+</sup> and Co<sup>2+</sup>/Co<sup>3+</sup> cycles. This study highlights the enhanced efficacy of PMS by NiCo-LDH catalysis and elucidates the activation mechanism of these catalysts in the removal of organic contaminants.</p> Graphical Abstract <p></p>

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Efficient Methylene Blue Degradation by NiCo-LDH-Activated Peroxymonosulfate: Efficiency, Mechanism, and Degradation Route

  • 期刊论文

  • 发表日期：

    2026年4月29日

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  • Suya Zhao,
  • Yuexiang Zhang,
  • Yaling Lu,
  • Xifeng Lv,
  • Jianbo Zhao,
  • Weiliang Tian,
  • Libing Hu

摘要

Although layered double hydroxides (LDHs) have been substantially applied as catalysts for the elimination of dye pollutants, the mechanism of the process still needs to be fully understood. Herein, NiCo-LDH[X] catalysts with different Ni: Co ratios (X = 1:1, 1:2, and 1:3) were prepared via the coprecipitation method, and we explored their effectiveness in the activation of peroxymonosulfate (PMS) to achieve efficient degradation of methylene blue (MB). The effect of several parameters on the catalytic performance of NiCo-LDH[X] was systematically evaluated. Following thorough experimental investigations, the activation mechanism and MB degradation pathways were proposed. Among the different NiCo-LDH[X] catalysts, NiCo-LDH[1:2] showed methylene blue degradation performance. Experimental results showed that this catalyst achieved MB degradation efficiency of 97.2% within 12 min, and a total organic carbon removal rate of 67.1% within 60 min, while exhibiting remarkable adaptability, reusability, and stability, as confirmed by post-catalytic characterization. Radical scavenging studies identified superoxide radicals (O2·−), sulfate radicals (SO4·−), and singlet oxygen (1O2) as the primary reactive oxygen species generated in the NiCo-LDH[1:2]/PMS system. The results of X-ray photoelectron spectroscopy (XPS) analysis clarified the roles of oxygen vacancies and Co sites as active sites, demonstrating the reversible redox behavior of NiCo-LDH[1:2] through Ni2+/Ni3+ and Co2+/Co3+ cycles. This study highlights the enhanced efficacy of PMS by NiCo-LDH catalysis and elucidates the activation mechanism of these catalysts in the removal of organic contaminants.

Graphical Abstract