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Cobalt-doped boosted the peroxymonosulfate activation performance of LaFeO3 perovskite for atrazine degradation
Chemical Engineering Journal ( IF 13.3 ) Pub Date : 2022-09-26 , DOI: 10.1016/j.cej.2022.139427
Heng Zhang , Renjing Zhang , Zechao Wu , Fashan Yang , Mengfan Luo , Gang Yao , Zhimin Ao , Bo Lai

In this work, cobalt (Co) doped perovskite with a molecular formula of LaFe0.9Co0.1O3 (LFCO) was synthesized, and was successfully employed for peroxymonosulfate (PMS) activation to eliminate atrazine (ATZ) from water. In contrast with alone perovskite without doped Co (LFO), the PMS activation performance was significantly improved. The influences of experimental parameters including LFCO dosage, PMS content, and reaction pH on the elimination of ATZ were discussed. Based on the consequences of quenching experiments and electron paramagnetic resonance test, radical dotOH and SO4radical dot were confirmed to be the primary active species in the LFCO/PMS system. LFCO surface chemistry analysis combined with density functional theory (DFT) calculations were utilized to systematically reveal the underlying activation pathway of LFCO and suggested that there is a synergetic function between Co and Fe in PMS activation via accelerating redox cycle of surface metal ions. Additionally, the application potential of the LFCO/PMS system was discussed by demonstrating its resistance to common water matrix. The possible transformation pathway of ATZ in the LFCO/PMS system was proposed according to the findings of UPLC-QTOF-MS/MS. This research sheds light on the role of bimetallic oxides in PMS activation for degrading organic contaminants.



中文翻译:

钴掺杂提高了 LaFeO3 钙钛矿对阿特拉津降解的过氧单硫酸盐活化性能

在这项工作中,合成了分子式为 LaFe 0.9 Co 0.1 O 3 (LFCO) 的钴 (Co) 掺杂钙钛矿,并成功用于过氧单硫酸盐 (PMS) 活化以消除水中的阿特拉津 (ATZ)。与没有掺杂Co的单独钙钛矿(LFO)相比,PMS活化性能显着提高。讨论了LFCO用量、PMS含量、反应pH等实验参数对ATZ消除的影响。基于淬灭实验和电子顺磁共振测试的结果,激进点OH 和 SO 4 激进点-被证实是 LFCO/PMS 系统中的主要活性物质。LFCO 表面化学分析结合密度泛函理论 (DFT) 计算系统地揭示了 LFCO 的潜在活化途径,并表明 Co 和 Fe 通过加速表面金属离子的氧化还原循环在 PMS 活化中具有协同作用。此外,通过展示其对普通水基质的耐受性,讨论了 LFCO/PMS 系统的应用潜力。根据UPLC-QTOF-MS/MS的发现,提出了ATZ在LFCO/PMS系统中可能的转化途径。这项研究揭示了双金属氧化物在 PMS 活化以降解有机污染物中的作用。

更新日期:2022-09-28
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