Magnetic nitrogen-doped sludge-derived biochar catalysts for persulfate activation: Internal electron transfer mechanism
Magnetic nitrogen-doped sludge-derived biochar catalysts for persulfate activation: Internal electron transfer mechanism
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用于过硫酸盐活化的磁性氮掺杂污泥衍生生物炭催化剂：内部电子转移机制
DOI：
10.1016/j.cej.2019.01.163
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发表时间：
2019-05
影响因子：
15.1
通讯作者：
Ren X
中科院分区：
文献类型：
--
作者：
Yu J;Tang L;Pang Y;Zeng G;Wang J;Deng Y;Liu Y;Feng H;Chen S;Ren X
过硫酸盐为基础的深度氧化工艺是一种强有力的水修复对策，目前还需要高效、低成本的催化剂。本文提出了一种一锅法合成磁性掺氮污泥生物炭（ms -生物炭）的方法，该方法对四环素的催化降解性能优于典型的石墨碳（石墨粉、氧化石墨烯和多壁碳纳米管）和其他两种类型的生物炭。EDAX表现出元素在ms -生物炭中的均匀分散。与“自上而下”类似，提出了从整体到部分的ms -生物炭贡献测量思路，其中酸溶性物质（ASS）对MS-400/600贡献最大，而碳基质（CM）对MS-800贡献最大。猝灭和EPR在ms -生物炭/PDS中显示出自由基途径，其中ASS主要被认为对so4自由基dot -有效，而CM主要致力于自由基dotOH的生成。EDAX， XPS和Raman研究证实了三种催化位点，即铁化合物，掺杂氮和石墨碳。讨论了它们的活化机理，并首次提出了从sp3到纳米晶esp2碳的内部电子迁移路径。可重复利用性、金属浸出检测和制药废水应用表明了质谱生物炭的潜力。本研究不仅为污泥资源化处理提供了一种可能，为材料性能测量提供了一种从整体到局部的新颖研究思路，而且为过硫酸盐活化碳材料，特别是sp2和sp3共杂化碳材料的设计提供了指导。
Persulfate-based advanced oxidation process is a powerful countermeasure for water remediation, where effective and low-cost catalysts are still needed. Herein, a one-pot synthetic method for magnetic nitrogen-doped sludge biochar (MS-biochar) was presented, which exhibited better catalytic property with PDS for tetracycline degradation than typical graphitic carbon (graphite powder, graphene oxide and multiwalled carbon nanotubes) and two other types biochars. EDAX manifested the uniform dispersion of elements in MS-biochar. Similar to “top-down”, a research thought from whole to part of MS-biochar for contribution measurement was presented, where acid-soluble substance (ASS) was the most important contributor for MS-400/600 while carbon matrix (CM) was dominant for MS-800. Quenching and EPR demonstrated a free-radicals pathway in MS-biochar/PDS, where ASS mainly assumed to be effective for SO4radical dot−and CM was primarily committed to radical dotOH generation. EDAX, XPS and Raman studies proved three kinds of catalytic sites, namely the iron compounds, doped nitrogen and graphitic carbon. And their activating mechanism were discussed where one internal electron migration path (fromsp3to nanocrystallinesp2carbon) has been first proposed. Reusability, metal leaching detection and pharmaceutical wastewater application indicated the potential of MS-biochar. This work not only presents a potential resource-based disposal of sewage sludge, a novel research thought from whole to part for materials performance measurement, but also provides guidance for carbon materials’ design for persulfate activation, especially forsp2andsp3co-hybridized carbons.
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