火山灰-活性炭的制备表征及其催化湿式氧化研究

采用自制的酚醛树脂基火山灰-活性炭负载Ce稀土催化剂在间歇式反应釜中催化湿式氧化(Catalytic wet air oxidation,CWAO)降解高浓度苯酚废水至可生化要求。发现经过浸渍、固化、炭化3个循环后可以获得9%的含炭量、1 020 m2/g的比表面积、0.57 cm3/g的总孔容并能满足后续反应所需的传质要求。同时研究了不同的炭化升温速率和炭化温度对火山灰-活性炭的性能的影响,发现升温速率为4℃/min、炭化温度为850℃时火山灰-活性炭获得最佳的结构特征。通过最佳工艺制备得到的催化剂,COD去除率达到92.4%,甲醛、苯酚去除率接近100%,BOD5/COD=0.42,满足可生化处理的要求。     

Catalytic wet air oxidation of phenol,nitrobenzene and aniline over the multi-walled carbon nanotubes (MWCNTs) as catalysts

Wet air oxidation (WAO) is one of effective technologies to eliminate hazardous, toxic and highly concentrated organic compounds in the wastewater. In the paper, multi-walled carbon nanotubes (MWCNTs), functionalized by O₃, were used as catalysts in the absence of any metals to investigate the catalytic activity in the catalytic wet air oxidation (CWAO) of phenol, nitrobenzene (NB) and aniline at the mild operating conditions (reaction temperature of 155°C and total pressure of 2.5 MPa) in a batch reactor. The MWCNTs were characterized with scanning electron microscopy (SEM), transmission electron microscopy (TEM), gas adsorption measurements (BET), fourier transform infrared spectroscopy (FT-IR), and X-ray photoelectron spectroscopy (XPS). The functionalized MWCNTs showed good catalytic performance. In the CWAO of phenol over the functionalized MWCNTs, total phenol removal was obtained after 90 min run, and the reaction apparent activation energy was ca. 40 kJ·mol^-1. The NB was not removed in the CWAO of single NB, while ca. 97% NB removal was obtained and 40% NB removal was attributed to the catalytic activity after 180 min run in the presence of phenol. Ca. 49% aniline conversion was achieved after 120 min run in the CWAO of aniline.     

Fe2O3-CeO2-Bi2O3/γ-Al2O3 catalyst in the catalytic wet air oxidation (CWAO) of cationic red GTL under mild reaction conditions

Fe₂O₃-CeO₂-Bi₂O₃/γ-Al₂O₃, an environmental friendly material, was investigated. The catalyst exhibited good catalytic performance in the CWAO of cationic red GTL. The apparent activation energy for the reaction was 79 kJ·mol⁻¹. HO₂· and O₂·⁻ appeared as the main reactive species in the reaction. The Fe₂O₃-CeO₂-Bi₂O₃/γ-Al₂O₃ catalyst, a novel environmental-friendly material, was used to investigate the catalytic wet air oxidation (CWAO) of cationic red GTL under mild operating conditions in a batch reactor. The catalyst was prepared by wet impregnation, and characterized by special surface area (BET measurement), X-ray diffraction (XRD) and X-ray photoelectron spectroscopy (XPS). The Fe₂O₃-CeO₂-Bi₂O₃/γ-Al₂O₃ catalyst exhibited good catalytic activity and stability in the CWAO under atmosphere pressure. The effect of the reaction conditions (catalyst loading, degradation temperature, solution concentration and initial solution pH value) was studied. The result showed that the decolorization efficiency of cationic red GTL was improved with increasing the initial solution pH value and the degradation temperature. The apparent activation energy for the reaction was 79 kJ·mol⁻¹. Hydroperoxy radicals (HO₂·) and superoxide radicals (O₂⁻·) appeared as the main reactive species upon the CWAO of cationic red GTL.     

有机污染物湿式氧化降解中Cu系列催化剂的稳定性

在 0.5L高压釜中采用自制 Cu系列催化剂在温度 150～ 230℃和氧分压 3.0 MPa反应条件下对染料中间体 H-酸配水进行催化湿式氧化反应 ,着重研究了非均相 Cu催化剂在催化湿式氧化过程中的稳定性问题 ,发现酸性溶出和反应性溶出是导致Cu列系催化剂不稳定的主要原因 .分别针对溶出原因 ,从改变反应条件 ,优化催化剂的设计和制备等方面进行了控制 ²⁺溶出的试验研究 ,指出克服 Cu²⁺溶出问题是规模化实际应用的关键 .