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N、S 共掺杂多孔碳活化过硫酸盐去除四环素:非自由基机制。

N, S-Doped porous carbons for persulfate activation to remove tetracycline: Nonradical mechanism.

机构信息

College of Architecture & Environment, Sichuan University, Chengdu 610065, PR China.

College of Architecture & Environment, Sichuan University, Chengdu 610065, PR China.

出版信息

J Hazard Mater. 2020 Jun 5;391:122055. doi: 10.1016/j.jhazmat.2020.122055. Epub 2020 Jan 28.

DOI:10.1016/j.jhazmat.2020.122055
PMID:32045799
Abstract

Nitrogen and sulfur-codoped porous carbons (SNCs) with porous structures and high surface areas were successfully synthesized employing coffee grounds, sodium bicarbonate and L-cysteine monohydrochloride as precursors. The SNCs were highly efficient for adsorption and exhibited outstanding catalytic performance for the oxidative degradation of tetracycline hydrochloride (TeC) solutions, especially at a calcined temperature of 700 °C (SNCs-700). The radical quenching, advanced in situ electron paramagnetic resonance (EPR) technology, PS decomposition rates and Linear Sweep Voltammetry (LSV) indicated that the excellent oxidative effectiveness of the PS/SNCs-700 system originated from the nonradical pathways (singlet oxygen (O) and electron transfer). It's supposed that N and S doping can effectively create point defects, which could generate O, while carbonyl groups were determined to be the main active sites contributing to the electron transfer. TeC degradation intermediates were also identified, three degradation pathways, revealing that the pre-adsorption significantly accelerated the nonradical oxidation pathways. This approach provides an innovative method for the large-scale production and application of high-quality catalysts in water treatment.

摘要

氮硫共掺杂多孔碳(SNCs)具有多孔结构和高比表面积,采用咖啡渣、碳酸氢钠和 L-半胱氨酸盐酸盐为前驱体制备成功。SNCs 对吸附具有很高的效率,并表现出对盐酸四环素(TeC)溶液的出色催化氧化降解性能,特别是在煅烧温度为 700°C(SNCs-700)时。自由基淬灭、先进的原位电子顺磁共振(EPR)技术、PS 分解率和线性扫描伏安法(LSV)表明,PS/SNCs-700 体系的优异氧化效果源于非自由基途径(单线态氧(O)和电子转移)。据推测,N 和 S 的掺杂可以有效地产生点缺陷,从而产生 O,而羰基被确定为促进电子转移的主要活性位点。还鉴定了 TeC 降解中间体,揭示了三条降解途径,表明预吸附显著加速了非自由基氧化途径。该方法为在水处理中大规模生产和应用高质量催化剂提供了一种创新方法。

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