Details

Autor(en) / Beteiligte

• Chen, Weirui
• Li, Xukai
• Wei, Xipeng
• Liao, Gaozu
• Wang, Jing
• Li, Laisheng

Titel

Activation of peroxymonosulfate for degrading ibuprofen via single atom Cu anchored by carbon skeleton and chlorine atom: The radical and non-radical pathways

Ist Teil von

• The Science of the total environment, 2023-02, Vol.858 (Pt 3), p.160097, Article 160097

Ort / Verlag

Netherlands: Elsevier B.V

Erscheinungsjahr

2023

Quelle

Alma/SFX Local Collection

Beschreibungen/Notizen

• Single atomic Cu catalysts (SACs Cu@C) anchored by carbon skeleton and chlorine atom was synthesized by hydrolyzing Cu-MOFs and then pickled by aqua-regia to remove Cu nanoparticles (NPs Cu). Comparative characterizations revealed that SACs Cu@C was a hierarchically porous nanostructure and Cu dispersed uniformly throughout the carbon skeletons. With less active components, SACs Cu@C behaved better in activating PMS over NPs Cu@C on ibuprofen removal (91.3 % versus 30.2 % in 30 min). Two Cu coordination environments were found by EXAF and DFT calculation, including four-coordinated Cu with 4C atoms and six-coordinated Cu with 4Cu and 2Cl atoms. The obvious interfacial electron delivery between PMS and SACs Cu@C was found, which was enhanced by Cl atom. Cu(I)/Cu(II) redox cycle would donate electron to peroxy bond of PMS for generating OH, SO4− and O2−. But electron transferred in opposite direction when PMS bonded to Cu atom through its terminal oxygen atom in sulfate, which formed 1O2. IBP degradation proceeded through both radical and non-radical route. IBP degradation was inhibited with the presence of TBA, methanol and furfuryl alcohol but accelerated by p-BQ, which could accelerate OH generation. Two degradation pathways were deducted. This study provided a new insight into catalysts designed for PMS activation. [Display omitted] •SACs Cu@C was prepared by Cu-MOFs hydrolyzing and aqua regia pickling.•Atomic Cu existed in CuC4 and CuC4Cl2 configurations within SACs Cu@C.•SACs Cu@C had the greater atomic utilization rate in activating PMS than NPs Cu@C.•The satisfied IBP removal was obtained by the radical and non-radical routes.•IBP degradation pathway was deducted and toxicity of by-products were assessed.