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内源性 Fe 和外源性 N 掺杂制药污泥生物炭中产生的 FeN 用于增强过一硫酸盐活化以降解左氧氟沙星。

FeN produced in pharmaceutical sludge biochar by endogenous Fe and exogenous N doping to enhance peroxymonosulfate activation for levofloxacin degradation.

机构信息

Jiangsu Key Laboratory of Anaerobic Biotechnology, School of Environment and Civil Engineering, Jiangnan University, Wuxi 214122, China.

Jiangsu Key Laboratory of Anaerobic Biotechnology, School of Environment and Civil Engineering, Jiangnan University, Wuxi 214122, China; Jiangsu Collaborative Innovation Center of Water Treatment Technology and Material, Suzhou 215011, China.

出版信息

Water Res. 2022 Oct 1;224:119022. doi: 10.1016/j.watres.2022.119022. Epub 2022 Aug 28.

Abstract

For preparing high performance biochar to be applicated in persulfate-based oxidation treatment of wastewater, the feasibility of deriving Fe-N biochar from pharmaceutical sludge by endogenous Fe and exogenous N doping was investigated. With exogenous urea doping, FeN contained biochar (PZBC800U) was successfully derived from endogenous Fe(OH) contained pharmaceutical sludge. PZBC800U effectively activated peroxymonosulfate (PMS) to remove 80 mg·L levofloxacin (LEV) within 90 min. The main mechanism of PMS activation by PZBC800U for LEV degradation was revealed as non-radical pathways dominated by O generation and direct electron transfer. The formation of FeN combined with the increase of pyridinic-N in the biochar changed the electronic structure, improved the electron transfer ability, and thus achieved the excellent PMS activation capacity of the biochar. The vital function of endogenous Fe(OH) was verified by comparing PZBC800U to Fe leached and extra Fe added controls. A total of 18 intermediates in the degradation of LEV were identified, and degradation pathways were proposed. Combined with the average local ionization energy calculation, the priority of piperazine breakage during LEV degradation was experimentally proved and mechanistically elucidated. This study provides a new insight into FeN biochar preparation from pharmaceutical sludge and the mechanisms of its excellent PMS activation performance for LEV degradation.

摘要

为了制备可应用于过硫酸盐氧化处理废水的高性能生物炭,研究了通过内源性 Fe 和外源性 N 掺杂从制药污泥中衍生出 Fe-N 生物炭的可行性。通过外加尿素掺杂,成功地从含有内源性 Fe(OH)的制药污泥中衍生出含 FeN 的生物炭(PZBC800U)。PZBC800U 可有效激活过一硫酸盐(PMS),在 90 min 内去除 80 mg·L 的左氧氟沙星(LEV)。通过 PZBC800U 活化 PMS 降解 LEV 的主要机制为以 O 生成和直接电子转移为主的非自由基途径。FeN 的形成和生物炭中吡啶-N 的增加改变了电子结构,提高了电子传递能力,从而使生物炭具有优异的 PMS 活化能力。通过与浸出的 Fe 和外加的 Fe 进行对比,验证了内源性 Fe(OH)的重要作用。共鉴定出 LEV 降解过程中的 18 种中间产物,并提出了降解途径。结合平均局部电离能计算,实验证明并从机理上证实了 LEV 降解过程中哌嗪断裂的优先性。本研究为从制药污泥中制备 Fe-N 生物炭以及其对 LEV 降解具有优异的 PMS 激活性能的机制提供了新的见解。

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