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ZIF-8衍生的氮掺杂多孔碳作为过一硫酸盐活化的无金属催化剂。

ZIF-8 derived nitrogen-doped porous carbon as metal-free catalyst of peroxymonosulfate activation.

作者信息

Ma Wenjie, Du Yunchen, Wang Na, Miao Peng

机构信息

MIIT Key Laboratory of Critical Materials Technology for New Energy Conversion and Storage, School of Chemistry and Chemical Engineering, Harbin Institute of Technology, Harbin, 150001, China.

出版信息

Environ Sci Pollut Res Int. 2017 Jul;24(19):16276-16288. doi: 10.1007/s11356-017-9191-2. Epub 2017 May 24.

Abstract

Nitrogen-doped porous carbon (NPC) is synthesized through a direct pyrolysis of zeolitic imidazolate framework (ZIF)-8 under N flow followed by acid washing process. It is found that NPC-800 pyrolyzed at 800 °C can inherit the perfect rhombic dodecahedron morphology of ZIF-8 crystals and achieve the considerable nitrogen-doping content of 15.20%. When NPC-800 is applied as the heterogeneous catalyst in peroxymonosulfate (PMS) activation for the degradation of Rhodamine B (RhB) and phenol, NPC-800 will exhibit its better performance than some conventional transition metal-based oxides and common carbon materials. The active sites can be primarily ascribed to nitrogen modification and sp -hybridized carbon frameworks. Besides, the influence of several parameters such as the dosage of catalyst, the concentration of oxidant, and reaction temperature is conducted systematically. More importantly, NPC-800 can maintain its considerable degradation in the presence of some anions and natural organic matters, even under some actual water background conditions. Although NPC-800 displays mild deactivation in repeated experiments, its catalytic performance can be easily recovered through heat treatment at 350 °C in air. Radical quenching tests reveal that both sulfate and hydroxyl radicals are responsible for the removal of organic pollutants. This research may provide a new way for the application of novel metal-free carbocatalysts in terms of PMS activation.

摘要

通过在氮气流下对沸石咪唑酯骨架(ZIF)-8进行直接热解,随后进行酸洗过程,合成了氮掺杂多孔碳(NPC)。研究发现,在800℃下热解的NPC-800可以继承ZIF-8晶体完美的菱形十二面体形态,并实现15.20%的可观氮掺杂量。当将NPC-800用作过一硫酸盐(PMS)活化降解罗丹明B(RhB)和苯酚的非均相催化剂时,NPC-800将表现出比一些传统过渡金属基氧化物和普通碳材料更好的性能。活性位点主要归因于氮修饰和sp 杂化碳骨架。此外,系统地研究了催化剂用量、氧化剂浓度和反应温度等几个参数的影响。更重要的是,即使在一些实际水背景条件下,NPC-800在存在一些阴离子和天然有机物的情况下仍能保持其可观的降解效果。尽管NPC-800在重复实验中表现出轻微失活,但其催化性能可通过在空气中350℃热处理轻松恢复。自由基猝灭试验表明,硫酸根和羟基自由基均对有机污染物的去除起作用。该研究可能为新型无金属碳催化剂在PMS活化方面的应用提供一种新途径。

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