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Efficiency and mechanism of high surface area mesoporous nanocast NC-LaCoO3 for activating peroxymonosulfate to degrade atrazine in water
Separation and Purification Technology ( IF 8.1 ) Pub Date : 2024-07-15 , DOI: 10.1016/j.seppur.2024.128823
Shahzad Afzal , Andleeb Mehmood , Lingyue Jin , Ke Pan , Munir Ahmad , Muhammad Javid , Muhammad Ikram , Ming Zhang , LiangKai Liu

A highly active perovskite is needed to activate peroxymonosulfate (PMS) into reactive oxygen species (ROS) to degrade organic pollutants in wastewater. High surface area LaCoO was fabricated via nano-casting employing mesoporous silica KIT-6 (a 3D material, first fabricated in Korea Advanced Institute of Science and Technology number 6) as the hard template. The NC-LaCoO showed a higher surface area (81.33 m·g), pore volume (0.21 cm·g) and pore diameter (7.78 nm), abundant acidic/basic sites, rich oxygen vacancies (OVs), and easily accessible active sites, as well as higher catalytic efficiency to degrade atrazine than uncast/citric acid-assisted perovskite (CA-LaCoO), CA-LaO and CoO. Under the specific experimental condition (PMS concentration: 4.30 mM; catalyst dosage: 0.60 g·L; pH: 8.20; atrazine concentration: 10 mg·L; and room temperature), in 6.0 min, approximately 19.02 %, 56 %, 29.38 %, and 39.21 % of atrazine were degraded by sole PMS, CA-LaCoO/PMS, CA-LaO/PMS and CoO/PMS respectively, while it was completely degraded in 4.0 min in NC-LaCoO/PMS. Moreover, 0.06 mg/L leaching of cobalt was detected during oxidation in the NC-LaCoO /PMS process. The NC-LaCoO depicted stable catalytic efficiency after six recycling terms. Radical scavengers depicted that SO and OH were produced as the main reactive species at the initial phase of the catalytic reaction, and subsequently, O and O were generated as the secondary oxidative species. A comparatively dominant inhibitory effect of methanol compared to TBA suggested that SO was mainly involved in atrazine degradation. XPS, EPR, in-situ ATR-FTIR, EIS, LSV, and chronoamperometric measurements were employed to explore the catalytic reaction mechanism. High catalytic efficiency was ascribed to better textural properties, diffusion-friendly structure, rich oxygen vacancies, and radical species. This research suggests that perovskites with a range of A and B metals can be synthesized by nanocasting using high surface area templates for advanced oxidation processes, especially PMS activation, to remediate organic wastewater.

中文翻译:


高比表面积介孔纳米铸NC-LaCoO3活化过一硫酸盐降解水中莠去津的效率及机理



需要一种高活性钙钛矿来将过一硫酸盐(PMS)活化成活性氧(ROS),以降解废水中的有机污染物。高表面积 LaCoO 是通过纳米铸造制造的,采用介孔二氧化硅 KIT-6(一种 3D 材料,首次在韩国高级科学技术研究所第 6 号制造)作为硬模板。 NC-LaCoO表现出较高的表面积(81.33 m·g)、孔体积(0.21 cm·g)和孔径(7.78 nm)、丰富的酸性/碱性位点、丰富的氧空位(OV)和易于接近的活性位点与未铸造/柠檬酸辅助钙钛矿 (CA-LaCoO)、CA-LaO 和 CoO 相比,降解莠去津的催化效率更高。在特定实验条件下(PMS浓度:4.30 mM;催化剂用量:0.60 g·L;pH:8.20;莠去津浓度:10 mg·L;室温),6.0 min内,分别约为19.02%、56%、29.38%和 39.21% 的莠去津分别被单独的 PMS、CA-LaCoO/PMS、CA-LaO/PMS 和 CoO/PMS 降解,而在 NC-LaCoO/PMS 中则在 4.0 分钟内完全降解。此外,在 NC-LaCoO /PMS 工艺的氧化过程中检测到 0.06 mg/L 的钴浸出量。 NC-LaCoO 在六个回收期后表现出稳定的催化效率。自由基清除剂描述了在催化反应的初始阶段产生的SO和OH作为主要反应物种,随后产生O和O作为次要氧化物种。与TBA相比,甲醇的抑制作用相对显着,表明SO主要参与莠去津的降解。采用 XPS、EPR、原位 ATR-FTIR、EIS、LSV 和计时电流测量来探索催化反应机理。 高催化效率归因于更好的结构特性、扩散友好的结构、丰富的氧空位和自由基物种。这项研究表明,具有一系列 A 和 B 金属的钙钛矿可以通过使用高表面积模板进行纳米铸造来合成,用于高级氧化过程,特别是 PMS 活化,以修复有机废水。
更新日期:2024-07-15
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