Ma Shuangnian, Gan Yu, Song Weifeng, Dai Wencan, Yang Zuoyi, Yang Rengao, Huang Xiangwu, Li Jinfu, Wu Zhixin, Chen Liyao
School of Environmental Science and Engineering, Guangdong University of Technology, Guangzhou, 510006, China.
School of Environmental Science and Engineering, Guangdong University of Technology, Guangzhou, 510006, China.
Chemosphere. 2023 Apr;320:138034. doi: 10.1016/j.chemosphere.2023.138034. Epub 2023 Feb 2.
Efficient degradation technologies are urgent to be developed to avoid the ecological and healthy hazards brought from atrazine (ATZ). LaCoO/peroxymonosulfate (PMS) system was proved to have strong degradation capabilities to contaminants. In this work, we intended to investigate the effect of the synthesis method on LaCoO. However, the hydrothermal method yielded a new material (H-Co) with better catalytic performance than LaCoO, which showed stable catalytic ability at pH 3.0-9.0 and 5 consecutive cycles. The coexistence of inorganic Cl, SO, NO, HPO, HCO and organic humic acids exerted little influences on the H-Co/PMS system. In addition, the actual livestock and poultry breeding wastewater could be well degraded and mineralized by the H-Co/PMS system. Free radical burst experiments and EPR characterization were performed to verify the synergistic effects of free radicals and non-free radicals during ATZ degradation. Based on SEM, XRD, O-TPD, FTIR, XPS, and electrochemistry characterizations, the efficient catalytic ability of H-Co could be attributed to the abundant oxygen vacancies, surface hydroxyl groups, zero-valent cobalt sites and high electronic conductivity. The degradation pathways were proposed based on the detection of degradation intermediates of ATZ by UPLC-MS. Moreover, the toxic of ATZ during the oxidation was evaluated by TEXT and E. coli inhibition assay. This work comprehensively analyzed the catalytic reaction mechanism of the H-Co/PMS system and provided a feasible pathway for the treatment of the actual livestock and poultry breeding wastewater.
迫切需要开发高效的降解技术，以避免莠去津（ATZ）带来的生态和健康危害。事实证明，LaCoO/过一硫酸盐（PMS）体系对污染物具有很强的降解能力。在本研究中，我们旨在研究合成方法对LaCoO的影响。然而，水热法产生了一种新材料（H-Co），其催化性能优于LaCoO，在pH 3.0-9.0和连续5个循环中表现出稳定的催化能力。无机Cl、SO、NO、HPO、HCO的共存以及有机腐殖酸对H-Co/PMS体系的影响很小。此外，H-Co/PMS体系能够很好地降解和矿化实际的畜禽养殖废水。进行了自由基猝灭实验和电子顺磁共振（EPR）表征，以验证ATZ降解过程中自由基和非自由基的协同作用。基于扫描电子显微镜（SEM）、X射线衍射（XRD）、氧程序升温脱附（O-TPD）、傅里叶变换红外光谱（FTIR）、X射线光电子能谱（XPS）和电化学表征，H-Co的高效催化能力可归因于丰富的氧空位、表面羟基、零价钴位点和高电子导电性。基于超高效液相色谱-质谱联用（UPLC-MS）对ATZ降解中间体的检测，提出了降解途径。此外，通过发光细菌毒性测试（TEXT）和大肠杆菌抑制试验评估了ATZ氧化过程中的毒性。本研究全面分析了H-Co/PMS体系的催化反应机理，为实际畜禽养殖废水的处理提供了一条可行的途径。
