Effects of metal and acidic sites on the reaction by-products of butyl acetate oxidation over palladium-based catalysts

Catalytic oxidation is widely used in pollution control technology to remove volatile organic compounds. In this study, Pd/ZSM-5 catalysts with different Pd contents and acidic sites were prepared via the impregnation method. All the catalysts were characterized by means of N2 adsorption- desorption, X-ray fluorescence （XRF）, HE temperature programmed reduction （H2-TPR）, and NH3 temperature programmed desorption （NH3-TPD）. Their catalytic performance was investigated in the oxidation of butyl acetate experiments. The by-products of the reaction were collected in thermal desorption tubes and identified by gas chromatography/mass spectrometry. It was found that the increase of Pd content slightly changed the catalytic activity of butyl acetate oxidation according to the yield of CO2 achieved at 90%, but decreased the cracking by-products, whereas the enhancement of strong acidity over Pd-based catalysts enriched the by-product species. The butyl acetate oxidation process involves a series of reaction steps including protolysis, dehydrogenation, dehydration, cracking, and isomerization. Generally, butyl acetate was cracked to acetic acid and 2- methylpropene and the latter was an intermediate of the other by-products, and the oxidation routes of typical by-products were proposed. Trace amounts of 3-methylpentane, hexane, 2-methylpentane, pentane, and 2-methylbutane originated from iso4merization and protolysis reactions.     

Mo-modified Pd/Al2O3 catalysts for benzene catalytic combustion

Mo-modified Pd/Al2O3catalysts were prepared by an impregnation method and tested for the catalytic combustion of benzene. The catalysts were characterized by N2 isothermal adsorption, X-ray diffraction（XRD）, X-ray photoelectron spectroscopy（XPS）, temperatureprogrammed desorption of NH3（NH3-TPD）, H2temperature-programmed reduction（H2-TPR）, and high-angle annular dark-field scanning transmission electron microscopy（HAADF-STEM）. The results showed that the addition of Mo effectively improved the activity and stability of the Pd/Al2O3catalyst by increasing the dispersion of Pd active components, changing the partial oxidation state of palladium and increasing the oxygen species concentration on the surface of catalyst. In the case of the Pd-Mo/Al2O3catalyst,benzene conversion of 90% was obtained at temperatures as low as 190°C, which was 45°C lower than that for similar performance with the Pd/Al2O3catalyst. Moreover, the 1.0% Pd-5% Mo/Al2O3catalyst was more active than the 2.0% Pd/Al2O3catalyst. It was concluded that Pd and Mo have a synergistic effect in benzene catalytic combustion.     

Photocatalytic activity of Fe-doped CaTiO3 under UV-visible light

The photocatalytic degradation of methylene blue（MB） over Fe-doped CaTiO3 under UV-visible light was investigated. The as-prepared samples were characterized using X-ray diffraction（XRD）, scanning electron microscope（SEM） equipped with an energy dispersive spectrometer（EDS） system, Fourier transform infrared spectra（FT-IR）, and UV-visible diffuse reflectance spectroscopy（DRS）. The results show that the doping with Fe significantly promoted the light absorption ability of CaTiO3 in the visible light region. The Fe-doped CaTiO3 exhibited higher photocatalytic activity than CaTiO3 for the degradation of MB.However, the photocatalytic activity of the Fe-doped CaTiO3 was greatly influenced by the calcination temperature during the preparation process. The Fe-doped CaTiO3 prepared at500°C exhibited the best photocatalytic activity, with degradation of almost 100% MB（10 ppm）under UV-visible light for 180 min.     

FBC-DPF在柴油机颗粒物控制中的应用研究

目前针对加装FBC-DPF(燃油添加剂-柴油机颗粒捕集器)后的柴油机放特性研究较少,并且缺乏FBC-DPF对颗粒物中PAHs排放量的影响效果研究.为全面评估加装FBC-DPF后柴油机颗粒物排放特性和FBC-DPF对柴油机尾气中的颗粒物排放污染控制效果,在发动机台架上对装有FBC-DPF的重型柴油机进行了颗粒物排放特性试验.利用电子低压撞击仪(ELPI)测量加装FBC-DPF前、后柴油机颗粒物的数浓度与粒径分布,用玻璃纤维滤膜采集加装FBC-DPF前、后尾气中的固相PAHs,利用色谱质谱联用仪对加装FBC-DPF前、后尾气中的固相PAHs进行定量分析.结果表明:①加装FBC-DPF后柴油机排放的颗粒物数浓度大幅降低,FBC-DPF对尾气中颗粒物的捕集效率平均值在95%左右;②加装FBC-DPF后柴油机固相PAHs总比排放量有所降低,在大负荷区域降幅在25.0%～88.0%之间;③加装FBC-DPF前的颗粒物中位直径为30～89 nm,而加装FBC-DPF后的颗粒物中位直径为41～98 nm,平均增幅为38.2%.对于国Ⅳ及未来国Ⅴ柴油机排放法规,FBC-DPF是解决柴油机颗粒物排放的有效手段;此外,FBC-DPF可以大幅降低柴油机尾气中的有毒成分,并且能够适应高含硫量的燃油环境.     

铁碳微电解法预处理聚氯乙烯(PVC)离心母液废水

采用铁碳微电解法对聚氯乙烯(PVC)离心母液废水进行预处理。分别考察反应时间、铁粉投加量、Fe/C(质量比)、pH值及曝气速率对母液废水中的COD和聚乙烯醇(PVA)去除率的影响,并在此基础上通过正交实验确定了废水COD的最佳处理条件。结果表明,最佳处理条件为:反应时间为4 h、铁粉投加量为30 g/L、Fe/C为1:2、pH值为2、曝气速率为0.8 L/min。在该条件下,废水中COD、PVA和TOC的平均去除率分别为(67%±2)%、(98%±1)%和(55%±3)%,废水的BOD/COD值从0.3提高到0.5,可生化性得到了显著提高。同时,废水中的NH3-N、浊度也在很大程度上得到了去除,出水中总铁含量也很低。     

催化臭氧氧化降解水溶液中亚甲基蓝的动力学研究

以废啤酒酵母为原材料、采用吸附-活化法制备得到负载过渡金属铁的活性炭(Fe/AC),对Fe/AC吸附亚甲基蓝(MB)性能和催化臭氧氧化MB效果进行了评价。Fe/AC对MB的吸附符合Langmuir等温吸附模型;20℃,pH=7的条件下,Fe/AC对MB的最大吸附量达到107.43 mg/g。吸附MB达到平衡的Fe/AC催化臭氧氧化降解水中MB,30 min内MB的转化率达到99%以上,5 h后总有机碳(TOC)的降解率达到70%。结合Fe/AC吸附MB特性和催化臭氧氧化MB行为,将Langmuir等温吸附模型分别与近似一级和二级反应动力学模型进行耦合,构建了Langmuir-Kinetic近似一级和近似二级耦合模型,均能较好地拟合MB转化率的动力学数据,但对体系的TOC去除率动力学数据的拟合度较低。     

MIL-101(Cr~(3+))可见光催化氧化降解甲基橙的研究

以金属有机多孔材料MIL-101(Cr3+)为非均相催化剂,过硫酸钠(Na2S2O8)为类Fenton体系的氧化剂,在可见光(300 W)下对甲基橙进行催化氧化降解研究。结果表明,MIL-101(Cr3+)在反应时间为120 min时对甲基橙降解率高达91.0%,且回收利用3次后仍表现出优异的降解性能(降解率达到81.0%)。同样条件下,把MIL-101(Cr3+)替换为TiO2或者不添加任何催化剂,甲基橙的降解率分别为25.6%和8.8%。采用紫外-可见漫反射光谱考察了常温下MIL-101(Cr3+)的禁带宽度大小,进一步证明其优异的光催化降解性能;同时还探讨了MIL-101(Cr3+)催化降解甲基橙的可能机理。     

高效去除难降解毒害污染物的零价铁技术装备

文章综述了可高效去除硝基芳烃、氯代有机物、毒害重金属等典型难降解毒害污染物的零价铁技术的降解机理及应用效能,重点总结了其技术装备的改良优化与集成强化方式,系统比较了多种技术装备及应用流程的性能优势及应用缺陷。进一步展望了该技术国内外的最新方向及应用前景。     

欢迎订阅《工业水处理》杂志

正《工业水处理》杂志于1981年创刊,是经国家科委和国家新闻出版署批准,由中海油天津化工研究设计院主办的专业性科技刊物。专门报道国内外循环冷却水、锅炉水、工艺用水及工业废水的水处理技术动态、科研成果、实践经验及科学管理等内容,设有专论与综述、试验研究、分析与监测、经验交流、工程实例、油气田水处理、科学管理等栏目。涵盖领域广阔、内容丰富严谨、信息反应快捷,是反映当代水处理技术面貌的权威性杂志,深受水处理工作者的喜爱。适于从事工业水处理领域科研、设计、生产、教学等工作的单位及个人订阅。     

强化混凝处理低温低浊松花江水研究

针对低温低浊水出水浊度不达标的问题进行了絮凝试验研究。结果表明,投加混凝剂聚合氯化铝(PAC)或聚合氯化铝铁(PAFC),剩余浊度、剩余CODMn均有所降低,继续加大投药量,浊度反而升高。进一步试验表明:在PAFC用量为12 mg/L,改性活化硅酸用量为0.12 mg/L条件下,剩余浊度、剩余CODMn分别达到0.21 mg/L和0.64 mg/L。改性活化硅酸的投加时间对混凝效果有一定的影响,混凝开始后330s投加改性活化硅酸可以提高混凝效果。