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N 掺杂石墨化生物炭由螺旋藻提取藻蓝蛋白后的残余物制备,用于催化过硫酸盐实现非自由基消毒和有机氧化。

N-doped graphitic biochars from C-phycocyanin extracted Spirulina residue for catalytic persulfate activation toward nonradical disinfection and organic oxidation.

机构信息

State Key Laboratory of Urban Water Resource and Environment, School of Environment, Harbin Institute of Technology, Harbin, 150090, PR China.

State Key Laboratory of Urban Water Resource and Environment, School of Environment, Harbin Institute of Technology, Harbin, 150090, PR China.

出版信息

Water Res. 2019 Aug 1;159:77-86. doi: 10.1016/j.watres.2019.05.008. Epub 2019 May 4.

DOI:10.1016/j.watres.2019.05.008
PMID:31078754
Abstract

Biochars are low-cost and environmental-friendly materials, which are promising in wastewater treatment. In this study, biochars were manufactured from C-phycocyanin extracted (C-CP) Spirulina residue (SDBC) via thermal pyrolysis. Simultaneously, N-doping was also achieved from the protein in the algae for obtaining a high-performance carbocatalyst for peroxydisulfate (PDS) activation. The SDBC yielded large specific surface areas, nitrogen loading, and good conductivity, which demonstrated excellent oxidation efficiencies toward a wide array of aqueous microcontaminants. An in-depth mechanistic study was performed by integrating selective radical scavenging, solvent exchange (HO to DO), diverse organic probes, and electrochemical measurement, unveiling that SDBC/PDS did not rely on free radicals or singlet oxygen but a nonradical pathway. PDS intimately was bonded with a biochar (SDBC 900-acid, pyrolysis at 900 °C) to form a surface reactive complex that subsequently attacked an organic sulfamethoxazole (SMX) adsorbed on the biochar via an electron-transfer regime. During this process, the SDBC 900-acid played versatile roles in PDS activation, organic accumulation and mediating the electron shuttle from SMX to PDS. This nonradical system can maintain a superior oxidation efficiency in complicated water matrix and long-term stable operation. More importantly, the nonradical species in SDBC 900-acid/PDS system were capable of inactivating the bacteria (Escherichia coli) in wastewater. Therefore, the biochar based nonradical system can provide a mild and high-efficiency strategy for disinfection in waste and drinking water by green carbocatalysis. This study provides not only a value-added biochar catalyst for wastewater purification but also the first insight into the bacteria inactivation via nonradical oxidation.

摘要

生物炭是一种低成本、环保的材料,在废水处理中具有广阔的应用前景。在本研究中,通过热解从提取的 C-藻蓝蛋白(C-CP)螺旋藻残渣(SDBC)中制造生物炭。同时,藻类中的蛋白质也进行了氮掺杂,以获得用于过一硫酸盐(PDS)活化的高性能碳催化剂。SDBC 具有较大的比表面积、氮负载量和良好的导电性,对多种水相微污染物表现出优异的氧化效率。通过选择性自由基清除、溶剂交换(HO 到 DO)、不同的有机探针和电化学测量等综合手段进行了深入的机理研究,揭示了 SDBC/PDS 不是依赖于自由基或单线态氧,而是一种非自由基途径。PDS 与生物炭(SDBC900-酸,在 900°C 下热解)紧密结合形成表面反应性络合物,然后通过电子转移机制攻击吸附在生物炭上的有机磺胺甲恶唑(SMX)。在此过程中,SDBC900-酸在 PDS 活化、有机累积和介导 SMX 到 PDS 的电子穿梭中发挥了多种作用。这种非自由基体系可以在复杂的水基质中保持优异的氧化效率和长期稳定的运行。更重要的是,SDBC900-酸/PDS 体系中的非自由基物质能够使废水中的细菌(大肠杆菌)失活。因此,基于生物炭的非自由基体系为通过绿色碳催化处理废水和饮用水中的消毒提供了一种温和高效的策略。本研究不仅为废水净化提供了一种增值生物炭催化剂,而且首次揭示了非自由基氧化对细菌失活的作用。

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