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具有表面氧缺陷的氧化铜上超快短程催化途径修饰过一硫酸氢盐活化用于降解盐酸四环素

Ultrafast short-range catalytic pathway modified peroxymonosulfate activation over CuO with surface oxygen defects for tetracycline hydrochloride degradation.

作者信息

Zhu Yi, Guan Zeyu, Li Xiaohu, Xia Dongsheng, Li Dongya

机构信息

School of Environmental Engineering, Wuhan Textile University, Wuhan, 430073, PR China.

School of Space and Environment, Beihang University, Beijing, 100191, PR China.

出版信息

Environ Res. 2023 Apr 1;222:115322. doi: 10.1016/j.envres.2023.115322. Epub 2023 Jan 21.

DOI:10.1016/j.envres.2023.115322
PMID:36693467
Abstract

The presence of antibiotics in water bodies seriously threatens the ecosystem and human health. Advanced oxidation processes (AOPs) based on peroxymonosulfate (PMS), an effective method to remove antibiotics, have a bottleneck problem that the low oxidant utilization is attributed to the hindered electron transfer between metal oxides and peroxides. Here, CuO with rich oxygen vacancies (OVs), MSCuO-300, was synthesized to efficiently degrade tetracycline hydrochloride (TTCH) (k = 0.095 min). The dominant role of direct adsorption and activation of OVs and its regulated Cu-O, rather than surface hydroxyl adsorption, mediated a short-range catalytic pathway. The shortened catalytic pathway between active sites and PMS accelerated the charge transfer at the interface, which promoted PMS activation. Compared with CuO-500 and Commercial CuO, the activation rate of PMS was increased by 11.97, and 12.64 times, respectively. OVs contributed to the production of O and O, the main active species. In addition, MSCuO-300/PMS showed excellent adaptability to real water parameters, such as pH (3-11), anions, and continuous reactor maintained for 168 h. This study provides a successful case for the purification of antibiotic-containing wastewater in the design of efficient catalysts by oxygen defect strategies.

摘要

水体中抗生素的存在严重威胁生态系统和人类健康。基于过一硫酸盐(PMS)的高级氧化工艺(AOPs)是一种去除抗生素的有效方法,但存在一个瓶颈问题,即低氧化剂利用率归因于金属氧化物和过氧化物之间电子转移受阻。在此,合成了具有丰富氧空位(OVs)的CuO,即MSCuO-300,以有效降解盐酸四环素(TTCH)(k = 0.095 min⁻¹)。OVs的直接吸附和活化及其调控的Cu-O而非表面羟基吸附起主导作用,介导了一条短程催化途径。活性位点与PMS之间缩短的催化途径加速了界面处的电荷转移,从而促进了PMS的活化。与CuO-500和商业CuO相比,PMS的活化率分别提高了11.97倍和12.64倍。OVs有助于产生主要活性物种O₂⁻和·OH。此外,MSCuO-300/PMS对实际水参数如pH(3 - 11)、阴离子以及连续运行168 h的反应器表现出优异的适应性。本研究为通过氧缺陷策略设计高效催化剂净化含抗生素废水提供了一个成功案例。

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