College of Chemistry and Materials Science, Sichuan Normal University, Chengdu 610068, China.
College of Chemistry and Materials Science, Sichuan Normal University, Chengdu 610068, China.
J Hazard Mater. 2022 May 15;430:128433. doi: 10.1016/j.jhazmat.2022.128433. Epub 2022 Feb 7.
Developing efficient modulation strategies to boost the degradation efficiencies of non-noble metal catalysts for toxic phenolic compounds involving peroxymonosulfate (PMS)-based oxidation processes is essential but remains an arduous challenge. This study reports the one-pot construction of in-situ surface vulcanized CoFeO @carbon (S-CF@C) to boost the PMS activation for 4-nitrophenol (4-NP) destruction. The direct pyrolysis of an aerogel precursor consisted of cobalt nitrate, ferric nitrate, melamine, and thiourea enables the as-formed S-CF@C with hierarchical structure, rich oxygen vacancies, and electron/mass transfer, thereby considerably promoting PMS activation performance of S-CF@C toward 4-NP degradation. Specifically, the optimal S-CF@C can achieve a removal efficiency of 99% for 4-NP destruction (20 mg/L) through PMS activation. Meanwhile, the catalyst also has generality to degrade a variety of antibiotic and dye organic pollutants. The radical quenching and electron paramagnetic resonance tests reveal the radical and non-radical activation mechanism in the S-CF@C/PMS system. The degradation pathway for 4-NP destruction over the S-CF@C/PMS system is proposed. This study provides an efficient approach to modulate the PMS activation performance of ferrite spinel materials toward the degradation of acute phenolic compounds.
开发高效的调制策略来提高非贵金属催化剂在涉及过一硫酸盐(PMS)的氧化过程中对有毒酚类化合物的降解效率至关重要,但仍然是一个艰巨的挑战。本研究报道了一种原位表面硫化 CoFeO@碳(S-CF@C)的一锅法构建,以增强 PMS 对 4-硝基苯酚(4-NP)的破坏作用。由硝酸钴、硝酸铁、三聚氰胺和硫脲组成的气凝胶前体制备的直接热解使得所形成的 S-CF@C 具有分级结构、丰富的氧空位和电子/质量转移,从而大大提高了 S-CF@C 对 PMS 激活性能,有利于 4-NP 的降解。具体而言,最佳的 S-CF@C 通过 PMS 激活可以实现 99%的 4-NP 去除效率(20mg/L)。同时,该催化剂还具有普遍性,可以降解各种抗生素和染料有机污染物。自由基猝灭和电子顺磁共振测试揭示了 S-CF@C/PMS 体系中的自由基和非自由基激活机制。提出了 S-CF@C/PMS 体系中 4-NP 破坏的降解途径。本研究为调制尖晶石铁氧体材料对急性酚类化合物降解的 PMS 激活性能提供了一种有效的方法。