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FeO/N共掺杂污泥生物炭催化下过一硫酸盐氧化降解环丙沙星的效率及机理

Efficiency and mechanism of the degradation of ciprofloxacin by the oxidation of peroxymonosulfate under the catalysis of a FeO/N co-doped sludge biochar.

作者信息

Zheng Dayang, Zou Jiali, Xu Hao, Wu Min, Wang Yayi, Feng Cang, Zheng Eryang, Wang Teng, Shi Yuxiang, Chen Yongjian, Li Binyang

机构信息

State Key Laboratory of Pollution Control and Resources Reuse, College of Environmental Science and Engineering, Tongji University, Siping Road, Shanghai, 200092, China.

Department of Natural Resources of Gansu Province, Hongxinggang Road, Lanzhou, 730099, China.

出版信息

Chemosphere. 2023 Jun;325:138387. doi: 10.1016/j.chemosphere.2023.138387. Epub 2023 Mar 11.

Abstract

A novel and recyclable composite material, FeO/N co-doped sludge biochar (FNBC), was developed from original sludge biochar (BC) and found to have excellent stability and superior catalytic capacity during the ciprofloxacin (CIP) degradation under the action of peroxymonosulfate (PMS). In the FNBC/PMS system, an approximately complete removal of CIP was achieved within 60 min under the condition of 1.0 g/L FNBC, 3.0 mM PMS, and 20 mg/L CIP, which was about 2.08 times of that in BC/PMS system (48.01%). Besides, FNBC/PMS system could effectively remove CIP under the influence of wide pH (2.0-10.0) or inorganic ions compared with BC/PMS system. Moreover, it was found that there were radical produced under the effect of Fe element, defects, functional groups, pyridinic N and pyrrolic N and non-radical caused by graphitic N, carbon atoms next to the iron atoms and better adsorption capacity in the FNBC/PMS system. It was observed that the contribution of hydroxyl radical (•OH), sulfate radical (SO) and singlet oxygen (O), which were the main reactive oxygen species, during the CIP degradation, were 75.80%, 11.49% and 10.26%, respectively. Furthermore, total organic carbon (TOC) variation was analyzed and the degradation pathway of CIP was speculated. The application of this material could combine the recycling of sludge with the effective degradation of refractory organic pollutant, providing an environmentally friendly and economic method.

摘要

一种新型可回收复合材料——FeO/N共掺杂污泥生物炭(FNBC),由原始污泥生物炭(BC)制备而成,发现其在过一硫酸盐(PMS)作用下对环丙沙星(CIP)降解过程中具有出色的稳定性和卓越的催化能力。在FNBC/PMS体系中,在1.0 g/L FNBC、3.0 mM PMS和20 mg/L CIP条件下,60分钟内可实现CIP的近乎完全去除,约为BC/PMS体系(48.01%)去除率的2.08倍。此外,与BC/PMS体系相比,FNBC/PMS体系在较宽pH范围(2.0 - 10.0)或存在无机离子影响下能有效去除CIP。而且,发现FNBC/PMS体系中,Fe元素、缺陷、官能团、吡啶氮和吡咯氮作用产生自由基,石墨氮、铁原子旁碳原子产生非自由基且具有更好的吸附能力。观察到,作为主要活性氧物种的羟基自由基(•OH)、硫酸根自由基(SO)和单线态氧(O)在CIP降解过程中的贡献分别为75.80%、11.49%和10.26%。此外,分析了总有机碳(TOC)变化并推测了CIP的降解途径。该材料的应用可将污泥回收与难降解有机污染物的有效降解相结合,提供一种环境友好且经济的方法。

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