UV-driven trace Cu(II)/peroxymonosulfate for efficient degradation of phosphonate: Mechanism and broad pH adaptability

作者：Tianhong Wang, Jiahui Xu, Anhong Cai, Jibo Xiao, Peng Wang, Min Zhao, Xianfeng Huang · 发表于：Chemical Engineering Journal Advances · 年份：2025 · DOI：10.1016/j.ceja.2025.100866 · 被引用次数：6 · 研究领域：Advanced oxidation water treatment、Advanced Photocatalysis Techniques、Chemical Synthesis and Characterization

Organic phosphonates detected frequently in water bodies pose severely environmental risks, and the cleavage of their C-P bonds to converse orthophosphate (PO 4 3- ) serves as a prerequisite step for achieving deep phosphorus elimination. Although the in situ generation of Cu(III) via Cu(II)/oxidant system for selective phosphonates degradation has been studied, the oxidation efficiency is constrained by sluggish Cu(II)/Cu(I) reduction, especially under acidic conditions. In this study, the introduction of UV irradiation accelerated the Cu(I)/Cu(II)/Cu(III) cycle in Cu(II)/peroxymonosulfate (PMS) process, enabling efficient and selective oxidation of 1,1-diphosphonic acid (HEDP, a typical phosphonate) into PO 4 3- across a wide pH range. UV-driven trace Cu(II)/PMS system can convert 90% of HEDP into PO 4 3- within 10 min at the pH range of 4-10, which was significantly higher than the conversion efficiency of HEDP by UV/PMS, Cu(II)/PMS and UV/Cu(II)/H 2 O 2 processes. The decomposition of HEDP was enhanced with increasing Cu(II) and PMS concentrations. Notably, mechanistic investigation revealed that Cu(III)-induced intramolecular electron transfer was the key contributor during the UV/Cu(II)/PMS-driven decomposition of HEDP into PO 4 3- . The experimental results of competitive ligands clearly suggested that the high selectivity of HEDP oxidation by UV/Cu(II)/PMS was closely related to the complexation of Cu(II) with HEDP. Additionally, although natural organic matter and in...