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研究论文

曹华莉,马志飞,吴山,吴代赦,杨天学,徐宇,曹侃,熊卿.氮掺杂石墨碳包埋Fe⁰复合材料的制备及活化过硫酸盐性能研究[J].环境科学学报,2020,40(3):930-939

Preparation and properties of nitrogen-doped-graphite-carbon-zero-valent iron composite for persulfate activation

摘要：采用"水热+热解"两步法制备介孔碳复合零价铁材料（Fe@HC）作为过硫酸盐（PS）活化剂，生成强氧化的活性物质，进而降解偶氮类染料活性黑5（RB5）.同时，采用X射线衍射仪（XRD）、透射电子显微镜（TEM）、比表面测试仪（BET）和X射线光电子能谱仪（XPS）对制备的复合材料进行表征，并考察了Fe@HC投加量、PS投加量、pH值及阴离子对活化PS去除RB5的影响.结果表明，采用"水热+热解"两步法成功制备了Fe@HC，其比表面积为280.7 m²·g^-1，平均孔径约为5.1 nm，BJH吸附累积总孔体积为0.284 cm³·g^-1.相对于单独的Fe@HC和PS，Fe@HC和PS共同存在可高效地去除RB5，脱色率为99.24%，且萘环破坏效率也达到了61.76%.RB5整体去除效果随Fe@HC、PS投加量的增大而提升，Fe@HC/PS体系在pH=3~11范围内对RB5的萘环破坏效率及脱色效率始终高于62%及86%，Cl^-和SO₄^2-对去除效率的影响较小，Fe@HC展示出良好的环境抗干扰能力.Fe@HC活化PS去除RB5的机理主要是体系中¹O₂的氧化降解作用.Fe@HC循环再生性能好.

Abstract：A mesoporous carbon-zero-valent iron composite material(denoted as Fe@HC), which is synthesized by using the "hydrothermal + pyrolysis" two-step method, has been adopted as a persulfate(PS) activator to form strong oxidizing active substances for the degradation of azo dye reactive black 5(RB5). The instruments of XRD, TEM, BET, and XPS have been applied to characterize the synthesized material, and to investigate the effects of Fe@HC dosage, PS dosage, pH, and anion on RB5 removal. The results show that Fe@HC is successfully synthesized. The specific surface area, average pore diameter, and total adsorption accumulation pore volume of BJH are 280.7 m²·g^-1, 5.1 nm, and 0.284 cm³·g^-1, respectively; compared with Fe@HC or PS alone, RB5 can be removed more efficiently with the combination of Fe@HC and PS, whose decolorization and naphthalene ring destruction efficiency are up to 99.24% and 61.76%. The overall removal effect of RB5 improves with Fe@HC and PS dosage. The Fe@HC/PS system has a naphthalene ring destruction and decolorization efficiency of RB5 that always higher than 62% and 86% in the range of pH 3~11. While Cl^- and SO₄^2- have little effect on removal efficiency, demonstrating the good stability and recycle of Fe@HC. The mechanism of Fe@HC activating PS to remove RB5 is mainly attributed to the oxidant ¹O₂ produced in the system.

Key words：carbon-zero-valent iron composite persulfate reactive black 5 degradation active substances