Song Yang, Feng Sha, Qin Wen, Ma Jun
School of Civil and Transportation Engineering, Guangdong University of Technology, Guangzhou, Guangdong, People's Republic of China.
State Key Laboratory of Urban Water Resource and Environment, School of Environment, Harbin Institute of Technology, Harbin, People's Republic of China.
Environ Technol. 2023 Feb;44(6):739-750. doi: 10.1080/09593330.2021.1983024. Epub 2021 Oct 3.
In this study, expanded graphite (EG) was prepared by the oxidation and intercalation of the natural flake graphite using perchloric acid and potassium permanganate at different expansion temperatures (300, 400, 500, and 600°C), and were characterized by scanning electron microscope (SEM) and X-ray photoelectron spectroscopy (XPS). EG prepared at 500°C was found to be highly effective for the mineralization of oxalic acid aqueous solution during ozonation at pH 3, which was ascribed to the formation of hydroxyl radicals from the surface reaction of surface hydroxyl groups on EG with ozone. The performance of expanded graphite in this catalytic system was basically unchanged after three repeated use. The presence of Cl, , and could inhibit the degradation of oxalic acid in catalytic ozonation with EG. Degradations of oxamic acid and pyruvic acid in catalytic ozonation with EG were pH-dependent, which were lower than that of oxalic acid. The degradations of oxalic acid and oxamic acid were identified as mineralization process by the determination of TOC, while pyruvic acid may transform into organic products such as acetic acid by O/EG. Manganese ion (Mn) could promote the degradation of oxalic acid by O/EG at pH 3 because permanganate was produced by O/EG in oxalic acid solution and then reacted with oxalic acid readily at acidic pH. Catalytic ozonation by EG exhibited great application potential for the destruction of refractory organic compounds.
在本研究中,使用高氯酸和高锰酸钾在不同膨胀温度(300、400、500和600°C)下对天然鳞片石墨进行氧化和插层制备膨胀石墨(EG),并通过扫描电子显微镜(SEM)和X射线光电子能谱(XPS)对其进行表征。发现在500°C制备的EG在pH为3的臭氧化过程中对草酸水溶液的矿化非常有效,这归因于EG表面羟基与臭氧的表面反应形成羟基自由基。在三次重复使用后,膨胀石墨在该催化体系中的性能基本保持不变。Cl、 、 和 的存在会抑制EG催化臭氧化中草酸的降解。EG催化臭氧化中草酰胺酸和丙酮酸的降解与pH有关,低于草酸的降解。通过测定总有机碳(TOC)确定草酸和草酰胺酸的降解为矿化过程,而丙酮酸可能通过O/EG转化为乙酸等有机产物。在pH为3时,锰离子(Mn)可促进O/EG对草酸的降解,因为在草酸溶液中O/EG会产生高锰酸盐,然后在酸性pH下高锰酸盐很容易与草酸反应。EG催化臭氧化在难降解有机化合物的破坏方面具有很大的应用潜力。