Hubei Key Laboratory of Mineral Resources Processing and Environment, School of Resources and Environmental Engineering, State Key Laboratory of Silicate Materials for Architectures, Wuhan University of Technology, Wuhan 430070, China.
Hubei Key Laboratory of Mineral Resources Processing and Environment, School of Resources and Environmental Engineering, State Key Laboratory of Silicate Materials for Architectures, Wuhan University of Technology, Wuhan 430070, China; The James Hutton Institute, Craigiebuckler, Aberdeen AB15 8QH, UK.
J Hazard Mater. 2023 Feb 15;444(Pt A):130336. doi: 10.1016/j.jhazmat.2022.130336. Epub 2022 Nov 6.
Neonicotinoids pose potential serious risks to human health even at environmental concentration and their removal from water is considered as a great challenge. A novel ball milling and acetic acid co-modified sludge biochar (BASBC) was the first time synthesized, which performed superior physicochemical characteristics including larger surface area, more defect structures and functional groups (e.g., CO and -OH). Electrochemistry was introduced to enhance BASBC for peroxymonosulfate (PMS) activation (E/BASBC/PMS) to degrade environmental concentration neonicotinoids (e.g., imidacloprid (IMI)). The degradation efficiency of IMI was 95.2% within 60 min (C (PMS)= 1 mM, E= 25 V, m (BASBC)= 10 mg). Solution pH and anionic species/concentrations were critical affecting factors. The scavenging and electron paramagnetic resonance experiments suggested that OH and O were the dominant reactive oxygen species contributing to IMI degradation. Three degradation pathways were proposed and pathway Ⅲ was the main one. 86.1% of IMI were mineralized into non-toxic CO and HO, and others were converted into less toxic intermediates. Also, E/BASBC/PMS system achieved the sustainable degradation of IMI in the cycle experiments. Additionally, it exhibited excellent degradation performance for other three typical neonicotinoids (96.6% of thiacloprid (THI), 96.5% of thiamethoxam (THX) and 82.6% of clothianidin (CLO)) with high mineralization efficiencies (87.8% of THI, 90.5% of THX and 75.4% of CLO).
新烟碱类杀虫剂即使在环境浓度下也对人类健康构成潜在的严重风险,因此将其从水中去除被认为是一项巨大的挑战。本研究首次合成了一种新型球磨和乙酸共改性污泥生物炭(BASBC),其具有优异的物理化学特性,包括更大的比表面积、更多的缺陷结构和官能团(如 CO 和-OH)。电化学被引入到 BASBC 中以增强其对过一硫酸盐(PMS)的活化(E/BASBC/PMS)以降解环境浓度的新烟碱类杀虫剂(如吡虫啉(IMI))。在 60 分钟内,IMI 的降解效率达到 95.2%(C(PMS)=1mM,E=25V,m(BASBC)=10mg)。溶液 pH 值和阴离子种类/浓度是关键的影响因素。清除和电子顺磁共振实验表明,OH 和 O 是导致 IMI 降解的主要活性氧物质。提出了三种降解途径,其中途径Ⅲ是主要途径。86.1%的 IMI 矿化为无毒的 CO 和 HO,其余的转化为毒性较低的中间产物。此外,E/BASBC/PMS 体系在循环实验中实现了 IMI 的可持续降解。此外,该体系对其他三种典型的新烟碱类杀虫剂(噻虫啉(THI)96.6%、噻虫嗪(THX)96.5%和噻虫胺(CLO)82.6%)也表现出优异的降解性能,具有较高的矿化效率(THI 为 87.8%,THX 为 90.5%,CLO 为 75.4%)。