Nickel in hierarchically structured nitrogen-doped graphene for robust and promoted degradation of antibiotics
Nickel in hierarchically structured nitrogen-doped graphene for robust and promoted degradation of antibiotics
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DOI：
10.1016/j.jclepro.2019.01.323
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发表时间：
2019-05
影响因子：
11.1
通讯作者：
Jian Kang;Huayang Zhang;Xiaoguang Duan;Hongqi Sun;X. Tan;Shaobin Wang
中科院分区：
文献类型：
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作者：
Jian Kang;Huayang Zhang;Xiaoguang Duan;Hongqi Sun;X. Tan;Shaobin Wang
通过一锅法合成了包裹在氮掺杂多孔石墨烯中的镍纳米颗粒（Ni@NPG），作为催化活化过硫酸盐（PS）的新型材料。评价了Ni@NPG催化剂对作为新兴污染物的抗生素磺胺氯哒嗪（SCP）的吸附和催化去除，发现其表现出优异的吸附和催化，仅在30 min内从水中去除100% SCP。同时，在连续运行4次后，具有良好的稳定性和可重复使用性，并具有令人满意的有机物降解。此外，由于碳壁的保护，金属浸出被禁止从金属@碳催化剂。进一步研究了不同浓度的湿酸和无机阴离子（HCO3-、Cl-、Br-和H2PO4-）对SCP降解的影响，结果表明，这些阴离子在低浓度时均能促进SCP降解，而在高浓度时由于自由基猝灭作用，对SCP降解有抑制作用。电子顺磁共振（EPR）和淬灭实验揭示了PS的活化机制，包括在没有单线态氧的情况下产生SO4·−、·OH和·O2 −。自由基和非自由基途径的协同作用在SCP氧化过程中起着至关重要的作用。
Nickel nanoparticles encapsulated in nitrogen-doped porous graphene (Ni@NPG) were synthesized through a one-pot method as a novel material for catalytic activation of persulfate (PS). The Ni@NPG catalysts were evaluated for adsorptive and catalytic removals of antibiotic sulfachloropyridazine (SCP) as an emerging pollutant and were found to exhibit excellent adsorption and catalysis with 100% SCP removal from water in only 30 min. Meanwhile, great stability and reusability can be achieved with satisfactory organic degradation after 4 successive runs. In addition, metal leaching was prohibited from the metal@carbon catalysts due to the protection of carbon walls. The influences of humid acid and inorganic anions (HCO3−, Cl−, Br−and H2PO4−) on SCP degradation at various concentrations were further investigated and the present study shows that all these species promoted the SCP degradation at a low concentration whereas an inhibition effect occurred at higher concentrations due to radical quenching. Electron paramagnetic resonance (EPR) and quenching experiments reveal the PS activation mechanism involving generation of SO4•−,•OH and•O2−without singlet oxygen. The synergistic effect of radical and nonradical pathways played crucial roles during the SCP oxidation process.