College of Environmental Science and Engineering and Key Laboratory of Environmental Biology and Pollution Control (Ministry of Education), Hunan University, Changsha 410082, PR China.
College of Environmental Science and Engineering and Key Laboratory of Environmental Biology and Pollution Control (Ministry of Education), Hunan University, Changsha 410082, PR China.
Water Res. 2023 Jun 15;237:119979. doi: 10.1016/j.watres.2023.119979. Epub 2023 Apr 13.
The conventional oxidation-adsorption methods are effective for the removal of roxarsone (ROX) but are limited by complicated operation, toxic residual oxidant and leaching of toxic metal ions. Herein, we proposed a new approach to improve ROX removal, i.e., using the FeS/sulfite system. Experimental results showed that approximately 100% of ROX (20 mg/L) was removed and more than 90% of the released inorganic arsenic (As(V) dominated) was adsorbed on FeS within 40 min. This FeS/sulfite system was a non-homogeneous activation process, and SO, ·OH and O were identified as reactive oxidizing species with their contributions to ROX degradation being 48.36%, 27.97% and 2.64%, respectively. Based on density functional theory calculations and HPLC-MS results, the degradation of ROX was achieved by C-As breaking, electrophilic addition, hydroxylation and denitrification. It was also found that the released inorganic arsenic was adsorbed through a combination of outer-sphere complexation and surface co-precipitation, and the generated arsenopyrite (FeAsS), a precursor to ecologically secure scorodite (FeAsO·2HO), was served as the foundation for further inorganic arsenic mineralization. This is the first attempt to use the FeS/sulfite system for organic heavy metal removal, which proposes a prospective technique for the removal of ROX.
传统的氧化-吸附方法对于去除罗硝唑(ROX)是有效的,但操作复杂,存在有毒残留氧化剂和有毒金属离子浸出等问题。本文提出了一种新的去除 ROX 的方法,即使用 FeS/亚硫酸盐系统。实验结果表明,在 40 分钟内,约 100%的 ROX(20mg/L)被去除,超过 90%的释放无机砷(以 As(V)为主)被 FeS 吸附。该 FeS/亚硫酸盐系统是非均相活化过程,SO、·OH 和 O 被确定为活性氧化物种,其对 ROX 降解的贡献分别为 48.36%、27.97%和 2.64%。基于密度泛函理论计算和 HPLC-MS 结果,ROX 的降解是通过 C-As 键断裂、亲电加成、羟化和脱硝实现的。还发现,释放的无机砷通过外球络合和表面共沉淀结合被吸附,生成砷铁矿(FeAsS),作为进一步无机砷矿化的基础。这是首次尝试使用 FeS/亚硫酸盐系统去除有机重金属,为去除 ROX 提供了一种有前景的技术。