4.7 Article

Ultra-adsorption enhancing peroxymonosulfate activation by ultrathin NiAl-layered double hydroxides for efficient degradation of sulfonamide antibiotics

期刊

JOURNAL OF CLEANER PRODUCTION
卷 369, 期 -, 页码 -

出版社

ELSEVIER SCI LTD
DOI: 10.1016/j.jclepro.2022.133277

关键词

Sulfonamide antibiotics; Ultrathin NiAl-Layered double hydroxides; Ultra-adsorption effect; Enhancing peroxymonosulfate activation; Dual reaction sites

资金

  1. Zhejiang Province Public Welfare Technology Application Research Project of China [LGG22E080023]
  2. Ningbo S&T Innovation 2025 Major Special Program [2020Z059, 2020Z107]
  3. Hundred Talents Programs in Chinese Academy of Science
  4. Ningbo Yongjiang Talent Introduction Program [2021A-036-B]

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The use of ultrathin nickel aluminium layered double hydroxide as an efficient peroxymonosulfate activator greatly accelerates the degradation of sulfonamide antibiotics in water. The super-adsorption phenomenon of U-NiAl-LDH and the activation of Ni(II) on its surface enhance the production of reactive oxygen species, leading to the fast elimination of target contaminants.
Sulfonamides have attracted special attention due to their widespread use and refractory nature in the aquatic environment. Heterogeneous catalytic peroxymonosulfate (PMS) activation for sulfonamide degradation has been demonstrated to be an encouraging strategy. Herein, ultrathin nickel aluminium layered double hydroxide (U-NiAl-LDH) was employed as an efficient peroxymonosulfate activator. The adsorption kinetics experiment showed that U-NiAl-LDH exhibited a super-adsorption phenomenon for sulfonamide antibiotics, such as sulfamethoxazole (SMX) and sulfachloropyridazine (SCP). U-NiAl-LDH was composed of 6 layers of a NiAl bimetallic layer structure. The degradation performance of organic contaminants via PMS activation was greatly accelerated by decreasing the number of LDH layers. Ni(II) on the surface of U-NiAl-LDH activated PMS to produce surface-bound hydroxyl radicals and sulfate radicals by donating electrons to cleave the O-O bond of PMS. These in-situ generated reactive oxygen species (ROS) on the surface of U-NiAl-LDH could directly attack adjacent adsorbed SMX or SCP molecules, where the migration distance between the ROS and target contaminants was reduced. Consequently, super-adsorption synergistically promoted the degradation efficiency of SMX and SCP, which decreased the demand for PMS. The newly found ultra-adsorption enhancing peroxymonosulfate activation effect was pioneered for the ultrafast elimination of sulfonamide antibiotics in real water. This proposed mechanism provides preliminary guiding significance to design PMS catalysts with dual reaction sites for the treatment of targeted refractory organic contaminant wastewater.

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