Activation of peroxymonosulfate by boron nitride loaded with Co mixed oxides and boron vacancy for ultrafast removal of drugs in surface water

IF 7.4 2区 工程技术 Q1 ENGINEERING, CHEMICAL Journal of Environmental Chemical Engineering Pub Date : 2024-09-24 DOI:10.1016/j.jece.2024.114241
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Abstract

The mediation of vacancy in catalysts is crucial for the enhancement of oxidant activation. Here the boron nitride loaded with Co mixed oxides (Co2O3-CoO) and boron vacancy (Bv) catalyst (Co/BN-X) was prepared to degrade sulfamethoxazole (SMX) by activating peroxymonosulfate (PMS). Under dark condition, Co/BN-3+PMS system can completely remove SMX in surface water within 15 min, and its removal efficiency constant (0.5154 min−1) was 4.0 and 6.7 times greater than those of Co/BN-2+PMS (0.1284 min−1) and Co/BN-1+PMS (0.0771 min−1), respectively. The system showed excellent performance in different influencing factors and cyclic experiments, and exhibited good practical application potential in secondary effluent. Electron paramagnetic resonance, radical quenching and electrochemical tests certified that singlet oxygen (1O2) was the major active species, followed by •O2, and SO4•–, further elaborating the activation pathway of PMS in Co/BN-3+PMS system. The density functional theory (DFT) calculations confirmed that CoO and PMS-O2 sites were the main reaction sites, and the existence of Bv reduced the adsorption energy of Co/BN-3 for PMS. This work reveals the synergistic effect between Co oxide sites and Bv on the catalyst surface and offers a potential modification method to accelerate Fenton-like reaction.
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氮化硼负载钴混合氧化物和硼空位活化过一硫酸盐,超快去除地表水中的药物
催化剂中空位的调解对于提高氧化剂活化至关重要。本文制备了负载钴混合氧化物(Co2O3-CoO)和硼空位(Bv)的氮化硼催化剂(Co/BN-X),通过活化过一硫酸盐(PMS)来降解磺胺甲噁唑(SMX)。在黑暗条件下,Co/BN-3+PMS 系统能在 15 分钟内完全去除地表水中的 SMX,其去除效率常数(0.5154 min-1)分别是 Co/BN-2+PMS (0.1284 min-1)和 Co/BN-1+PMS (0.0771 min-1)的 4.0 倍和 6.7 倍。该系统在不同影响因素和循环实验中均表现出优异的性能,在二级污水中具有良好的实际应用潜力。电子顺磁共振、自由基淬灭和电化学测试证明,单线态氧(1O2)是主要的活性物种,其次是-O2-和SO4--,进一步阐明了Co/BN-3+PMS体系中PMS的活化途径。密度泛函理论(DFT)计算证实,CoO 和 PMS-O2 位点是主要的反应位点,Bv 的存在降低了 Co/BN-3 对 PMS 的吸附能。这项研究揭示了催化剂表面 Co 氧化位点和 Bv 之间的协同效应,为加速 Fenton 类反应提供了一种潜在的改性方法。
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来源期刊
Journal of Environmental Chemical Engineering
Journal of Environmental Chemical Engineering Environmental Science-Pollution
CiteScore
11.40
自引率
6.50%
发文量
2017
审稿时长
27 days
期刊介绍: The Journal of Environmental Chemical Engineering (JECE) serves as a platform for the dissemination of original and innovative research focusing on the advancement of environmentally-friendly, sustainable technologies. JECE emphasizes the transition towards a carbon-neutral circular economy and a self-sufficient bio-based economy. Topics covered include soil, water, wastewater, and air decontamination; pollution monitoring, prevention, and control; advanced analytics, sensors, impact and risk assessment methodologies in environmental chemical engineering; resource recovery (water, nutrients, materials, energy); industrial ecology; valorization of waste streams; waste management (including e-waste); climate-water-energy-food nexus; novel materials for environmental, chemical, and energy applications; sustainability and environmental safety; water digitalization, water data science, and machine learning; process integration and intensification; recent developments in green chemistry for synthesis, catalysis, and energy; and original research on contaminants of emerging concern, persistent chemicals, and priority substances, including microplastics, nanoplastics, nanomaterials, micropollutants, antimicrobial resistance genes, and emerging pathogens (viruses, bacteria, parasites) of environmental significance.
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