4.8 Article

Photocatalysis-activated SR-AOP over PDINH/MIL-88A(Fe) composites for boosted chloroquine phosphate degradation: Performance, mechanism, pathway and DFT calculations

Journal

APPLIED CATALYSIS B-ENVIRONMENTAL
Volume 293, Issue -, Pages -

Publisher

ELSEVIER
DOI: 10.1016/j.apcatb.2021.120229

Keywords

Metal-organic framework; Chloroquine phosphate; Sulfate radical-advanced oxidation process; DFT calculation; Degradation pathways

Funding

  1. Beijing Natural Science Foundation [8202016]
  2. National Natural Science Foundation of China [51878023]
  3. National Key Research and Development Program of China [2016YFC0402505]
  4. Great Wall Scholars Training Program Project of Beijing Municipality Universities [CITTCD20180323]
  5. Beijing Talent Project [2020A27]
  6. Fundamental Research Funds for Beijing University of Civil Engineering and Architecture [X20147, X20141, X20135, X20146]
  7. BUCEA Post Graduate Innovation Project [PG2020038]

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PDINH/MIL-88A(Fe) composites were fabricated using a facile ball-milling strategy, showing outstanding degradation performance towards CQ under low power LED visible light. The activation of PDS over P25M175 and pristine MIL-88A contributed to boosted CQ degradation efficiency through direct and indirect electron transfer. Active radicals and singlet oxygen were found to participate in the CQ decomposition, with proposed degradation pathways and toxicity evaluations of intermediates.
PDINH/MIL-88A(Fe) composites (PxMy) were fabricated from MIL-88A(Fe) and perylene-34,910-tetracarboxylic diimide (PDINH) via facile ball-milling strategy. The optimum P25M175 exhibited outstanding degradation performance toward chloroquine phosphate (CQ) by activating peroxydisulfate (PDS) under low power LED visible light. The synergistic effects of photocatalytic activations of PDS via the direct electron transfer PDS activation over P25M175 and indirect electron transfer PDS activation over pristine MIL-88A contributed to the boosted CQ degradation efficiency. The active species capture experimental data and electron spin resonance (ESR) determinations revealed that both active radicals (like (SO4-)-S-center dot, (OH-)-O-center dot, O-center dot(2)-, h(+)) and nonradical singlet oxygen (O-1(2)) participated in the CQ decomposition. The CQ degradation pathways and the toxicity evaluation of the intermediates were proposed based on LC-MS determination and DFT calculation. Also, P25M175 demonstrated good reusability and stability. The findings within this work offered deep insights into the mechanisms of organic pollutants degradation via photocatalysis-activated SR-AOP over Fe-MOF photocatalyst.

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