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过一硫酸盐活化水稻秸秆生物炭负载血红素制备新型 Fe/N-C 催化剂强化降解西玛津。

Enhanced simazine degradation via peroxymonosulfate activation using hemin-doped rice husk biochar as a novel Fe/N-C catalyst.

机构信息

Department of Chemistry, College of Basic and Applied Sciences, University of Ghana, Legon, Ghana; School of Architecture, Civil, Environmental and Energy Engineering, Kyungpook National University, Daegu, 41566, Republic of Korea.

Department of Civil, Construction, and Environmental Engineering, University of Alabama, Tuscaloosa, Alabama, 35487, United States; School of Architecture, Civil, Environmental and Energy Engineering, Kyungpook National University, Daegu, 41566, Republic of Korea.

出版信息

Chemosphere. 2024 Oct;366:143549. doi: 10.1016/j.chemosphere.2024.143549. Epub 2024 Oct 16.

Abstract

The presence of herbicides, including simazine (SIM), in aquatic environments pose significant threats to these ecosystems, necessitating a method for their removal. In this study, a hemin-doped rice husk-derived biochar (RBC@Hemin) was synthesized using a simple, one-step pyrolysis, and its degradation efficiency towards SIM via peroxymonosulfate (PMS) was assessed. Under optimized conditions (hemin loading = 20 wt%, SIM = 0.5 ppm, RBC@Hemin catalyst = 0.2 g L, PMS = 2.0 mM, and pH = 5.84 [unadjusted]), RBC@Hemin, as an Fe/N-C catalyst, could activate PMS to achieve >99% degradation of SIM. Based on radical scavenger and electron spin resonance spectroscopy (ESR) experiments, both radical (OH and SO) and non-radical (such as singlet oxygen, O) mechanisms and electron transfer were involved in the degradation system. Significant mineralization (97.3%) and reusability efficiency (∼74.1% SIM degradation after 4 applications) were exhibited by the RBC@Hemin/PMS system, which also maintained a remarkable degradation efficiency in tap-, river-, and ground-water. Additionally, the RBC@Hemin/PMS system exhibited rapid degradation of tetracycline (TC) and diclofenac (DCF), indicating its prospects in the degradation of other organic pollutants of aquatic environments. The plausible degradation mechanism pathways of SIM are proposed based on identified intermediates. Finally, the toxicity of these intermediate products is analysed using the Ecological Structure Activity Relationship (ECOSAR) software. It is expected that this study will expand the current knowledge on the synthesis of efficient biomass-based Fe/N-C composites for the removal of organic pollutants in water.

摘要

水体中存在莠去津(SIM)等除草剂,对这些生态系统构成了重大威胁,因此需要一种去除它们的方法。在这项研究中,使用简单的一步热解法合成了一种血红素掺杂稻壳衍生生物炭(RBC@Hemin),并评估了其过一硫酸盐(PMS)对 SIM 的降解效率。在优化条件下(血红素负载量为 20wt%,SIM 为 0.5ppm,RBC@Hemin 催化剂用量为 0.2gL,PMS 为 2.0mM,pH 值为 5.84[未调节]),作为 Fe/N-C 催化剂的 RBC@Hemin 可以激活 PMS 以实现 SIM 的>99%降解。基于自由基清除剂和电子自旋共振光谱(ESR)实验,降解体系涉及自由基(OH 和 SO)和非自由基(如单线态氧,O)机制和电子转移。RBC@Hemin/PMS 体系表现出显著的矿化(97.3%)和可重复使用效率(4 次应用后 SIM 降解率约为 74.1%),并且在自来水、河水和地下水等水中也保持了显著的降解效率。此外,RBC@Hemin/PMS 体系还表现出对四环素(TC)和双氯芬酸(DCF)的快速降解,表明其在降解其他水环境有机污染物方面具有广阔的应用前景。根据鉴定的中间产物,提出了 SIM 的可能降解机制途径。最后,使用生态结构活性关系(ECOSAR)软件分析这些中间产物的毒性。预计这项研究将扩展关于高效生物量基 Fe/N-C 复合材料去除水中有机污染物的合成的现有知识。

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