增强过氧单硫酸盐活化环丙沙星降解由去木素化木材衍生的碳。

IF 7.7 2区 环境科学与生态学 Q1 ENVIRONMENTAL SCIENCES
Xiangyu Wang, Yuwei Li, Hongjiao Chen, Luyao Zhang, Chengfeng Zhou, Jiaqi Cong, Cunzhen Geng, Bin Hui
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引用次数: 0

摘要

开发高性能和可持续的碳催化剂来促进有机抗生素的降解仍然是一个巨大的挑战。本文设计了一种脱木质素的含氮木源碳(DLWC@N),以增强过氧单硫酸盐(PMS)的活化,以降解环丙沙星(CIP)。研究发现,杨木中木质素和半纤维素的去除有助于形成更多孔的结构,并减少碳通道的渗透性。通过简单的热解策略对该亲水性纤维素骨架上的N种类和N含量进行调控。所得DLWC@N-700在60 min内达到97.49%的CIP去除率,连续4个循环后的去除率达到79.64%。衍生碳中独特的三维网络结构促进了溶液的扩散并暴露出更多的活性位点。石墨N键和N- o键是PMS活化过程中的主要活性位点。猝灭实验结合电子顺磁共振和电化学分析表明,降解过程以单重态氧和电子转移的非自由基途径为主。液相色谱-质谱分析结果表明,CIP的主要降解途径包括羟基化、哌嗪环裂解和环丙烷脱落,形成17个反应中间体。本工作提出了一种先进的游离金属木源碳催化剂,以增强PMS对抗生素降解的活化,促进废水处理技术的发展。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
Enhanced peroxymonosulfate activation for ciprofloxacin degradation enabled by a delignified wood-derived carbon.

Developing high-performance and sustainable carbon catalysts for enhancing the degradation of organic antibiotics remains a great challenge. Herein, a delignified wood-derived carbon embedded with nitrogen (DLWC@N) was designed to enhance peroxymonosulfate (PMS) activation for the degradation of aqueous ciprofloxacin (CIP). The removal of lignin and hemicellulose in poplar wood was found to facilitate the formation of a more porous architecture and tailed the permeability of channels in the carbon. N species and N content were regulated on this hydrophilic cellulose skeleton through a simple pyrolysis strategy. The resulting DLWC@N-700 achieved 97.49% CIP removal within 60 min and exhibited 79.64 % removal efficiency after four consecutive cycles. The unique three-dimensional network structure in the derived carbon promoted the diffusion of the solution and exposed much more active sites. Graphitic N and N-O bonds as main active sites during PMS activation were revealed. The quenching experiments combined with electron paramagnetic resonance and electrochemical analysis unveiled that the degradation process was dominated by a non-radical pathway of singlet oxygen and electron transfer. Liquid chromatography-mass spectrometer results demonstrated that the main degradation pathway of CIP included hydroxylation, cleavage of the piperazine ring, and cyclopropane shedding, resulting in the formation of seventeen reaction intermediates. This work proposes an advanced free-metal wood-derived carbon catalyst to enhance PMS activation for antibiotics degradation, facilitating the development of wastewater treatment technology.

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来源期刊
Environmental Research
Environmental Research 环境科学-公共卫生、环境卫生与职业卫生
CiteScore
12.60
自引率
8.40%
发文量
2480
审稿时长
4.7 months
期刊介绍: The Environmental Research journal presents a broad range of interdisciplinary research, focused on addressing worldwide environmental concerns and featuring innovative findings. Our publication strives to explore relevant anthropogenic issues across various environmental sectors, showcasing practical applications in real-life settings.
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