Wang Gen, Zhang Yue, Ge Lei, Liu Zhuoyue, Zhu Xiurong, Yang Shengjiong, Jin Pengkang, Zeng Xiangkang, Zhang Xiwang
Shaanxi Key Laboratory of Environmental Engineering, School of Environmental and Municipal Engineering, Xi'an University of Architecture and Technology, Xi'an, Shaanxi 710055, PR China.
Shaanxi Key Laboratory of Environmental Engineering, School of Environmental and Municipal Engineering, Xi'an University of Architecture and Technology, Xi'an, Shaanxi 710055, PR China.
J Hazard Mater. 2022 May 5;429:128282. doi: 10.1016/j.jhazmat.2022.128282. Epub 2022 Jan 15.
Nonradical oxidation based on singlet oxygen (O) has attracted great interest in groundwater remediation due to the selective oxidation property and good resistance to background constituents. Herein, recoverable CuO nanoparticles (NPs) supported on mineral substrates (SiO) were prepared by calcination of surface-coated metal-plant phenolic networks and explored for peroxymonosulfate (PMS) activation to generate O for degrading organic pollutants in groundwater. CuO NPs with a close particle size (40 nm) were spatially monodispersed on SiO substrates, allowing highly exposure of active sites and consequently leading to outstanding catalytic performance. Efficient removal of various organic pollutants was obtained by the supported CuO NPs/PMS system under wide operation conditions, e.g., working pH, background anions and natural organic matters. Chemical scavenging experiments, electron paramagnetic resonance tests, furfuryl alcohol decay and solvent dependency experiments confirmed the formation of O and its dominant role in pollutants removal. In situ characterization with ATR-FTIR and Raman spectroscopy and computational calculation revealed that a redox cycle of surface Cu(II)-Cu(III)-Cu(II) was responsible for the generation of O. The feasibility of the supported CuO NPs/PMS for actual groundwater remediation was evaluated via a flow-through test in a fixed-bed column, which manifested long-term durability, high mineralization ratio and low metal ion leaching.
基于单线态氧（O）的非自由基氧化因其选择性氧化特性和对背景成分的良好耐受性，在地下水修复领域引起了广泛关注。在此，通过对表面包覆的金属-植物酚类网络进行煅烧，制备了负载在矿物基底（SiO）上的可回收氧化铜纳米颗粒（NPs），并探索了其用于活化过一硫酸盐（PMS）以生成O来降解地下水中有机污染物的性能。粒径相近（40nm）的氧化铜纳米颗粒在SiO基底上呈空间单分散状态，使得活性位点高度暴露，从而具有出色的催化性能。负载型氧化铜纳米颗粒/过一硫酸盐体系在较宽的操作条件下，如工作pH值、背景阴离子和天然有机物存在的情况下，都能有效去除各种有机污染物。化学清除实验、电子顺磁共振测试、糠醇衰减实验和溶剂依赖性实验证实了O的形成及其在污染物去除中的主导作用。采用衰减全反射傅里叶变换红外光谱（ATR-FTIR）和拉曼光谱进行原位表征以及计算计算表明，表面Cu（II）-Cu（III）-Cu（II）的氧化还原循环是产生O的原因。通过固定床柱中的流通试验评估了负载型氧化铜纳米颗粒/过一硫酸盐体系用于实际地下水修复的可行性，结果表明该体系具有长期耐久性、高矿化率和低金属离子浸出率。
