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Fe,N 共掺杂核桃壳生物炭活化过一硫酸盐降解磺胺甲恶唑:性能与机制。

Activation of peroxymonosulfate by Fe,N co-doped walnut shell biochar for the degradation of sulfamethoxazole: Performance and mechanisms.

机构信息

KU Leuven, Department of Chemical Engineering, Process and Environmental Technology Lab, J. De Nayarita 5, 2860 Sint-Katelijne-Waver, Belgium.

University of Aveiro, Department of Materials and Ceramics Engineering, Aveiro Institute of Materials, CICECO, 3810-193, Aveiro, Portugal.

出版信息

Environ Pollut. 2024 Aug 15;355:124018. doi: 10.1016/j.envpol.2024.124018. Epub 2024 Apr 30.

Abstract

Fe and N co-doped walnut shell biochar (Fe,N-BC) was prepared through a one-pot pyrolysis procedure by using walnut shells as feedstocks, melamine as the N source, and iron (III) chloride as the Fe source. Moreover, pristine biochar (BC), nitrogen-doped biochar (N-BC), and α-FeO-BC were synthesized as controls. All the prepared materials were characterized by different techniques and were used for the activation of peroxymonosulfate (PMS) for the degradation of sulfamethoxazole (SMX). A very high degradation rate for SMX (10 mg/L) was achieved with Fe,N-BC/PMS (0.5 min), which was higher than those for BC/PMS (0.026 min), N-BC/PMS (0.038 min), and α-FeO-BC/PMS (0.33 min) under the same conditions. This is mainly due to the formation of FeC and iron oxides, which are very reactive for the activation of PMS. In the next step, Fe,N-BC was employed for the formation of a composite membrane structure by a liquid-induced phase inversion process. The synthesized ultrafiltration membrane not only exhibited high separation performance for humic acid sodium salt (HA, 98%) but also exhibited improved self-cleaning properties when applied for rhodamine B (RhB) filtration combined with a PMS solution cleaning procedure. Scavenging experiments revealed that O was the predominant species responsible for the degradation of SMX. The transformation products of SMX and possible degradation pathways were also identified. Furthermore, the toxicity assessment revealed that the overall toxicity of the intermediate was lower than that of SMX.

摘要

Fe 和 N 共掺杂的核桃壳生物炭(Fe,N-BC)通过一步热解法制备,以核桃壳为原料,三聚氰胺为 N 源,三氯化铁为 Fe 源。此外,还合成了原始生物炭(BC)、氮掺杂生物炭(N-BC)和α-FeO-BC 作为对照。所有制备的材料均通过不同的技术进行了表征,并用于活化过一硫酸盐(PMS)以降解磺胺甲恶唑(SMX)。在相同条件下,Fe,N-BC/PMS(0.5 min)对 SMX(10 mg/L)的降解率非常高,为 0.026 min,高于 BC/PMS(0.026 min)、N-BC/PMS(0.038 min)和α-FeO-BC/PMS(0.33 min)。这主要是由于 FeC 和铁氧化物的形成,它们对 PMS 的活化非常有反应性。在下一步中,通过液致相转化过程将 Fe,N-BC 用于形成复合膜结构。合成的超滤膜不仅对腐殖酸钠(HA,98%)表现出高分离性能,而且在与 PMS 溶液清洗程序结合使用时还表现出改善的自清洁性能。清除实验表明,O 是降解 SMX 的主要物质。还鉴定了 SMX 的转化产物和可能的降解途径。此外,毒性评估表明,中间产物的整体毒性低于 SMX。

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