铁氧化物复合氧化铝催化臭氧化过程中溴酸盐的生成控制简

以市售活性炭、硅藻土和氧化铝小球为载体，考察了负载铁基活性组分对催化臭氧化过程中溴酸盐的控制情况，其中，铁基复合氧化铝小球体现出更好的溴酸盐还原特性和催化剂稳定性，证实催化剂中铁氧化物是溴酸盐得到有效控制的主要活性组分。进一步考察了铁基复合氧化铝小球催化臭氧化处理实际原水过程中对溴酸盐的生成控制，以及反应过程中溶解性有机碳（DOC）的去除情况。结果表明，与单独臭氧化相比，该催化剂既能有效去除水中的溶解性有机物，又能明显抑制溴酸盐的生成，反应50 h，其活性并没有明显下降。催化剂失活主要归因于吸附位点数量的下降，可以通过负载铁氧化物来实现催化剂的再生。     

β-FeOOH/蜂窝陶瓷催化臭氧化高效去除饮用水中有机污染物

市售蜂窝陶瓷经过氧化铝涂层后,进一步负载β-FeOOH活性组分,制得改性蜂窝陶瓷催化剂(β-FeOOH/Ce-ramic honeycomb,β-FeOOH/CH)。与单独臭氧氧化相比,基于该催化剂的固定床反应装置体现出更好的臭氧化活性,反应20 min后,水中的2,4-二氯苯氧乙酸(2,4-D)就可以完全去除,其矿化效率也可以达到80%以上。进一步考察了进水流速、有机物浓度等因素对多相催化臭氧化效率的影响,结果表明:β-FeOOH/CH可以显著提高臭氧的利用效率,能够有效去除水中包括2,4-D在内的多种有机污染物,而且催化剂可以重复使用,在长期的运行实验中其催化性能没有明显下降,该反应装置在饮用水深度处理领域具有很好的应用潜力。     

铁及铁铜氧化物对臭氧氧化酸性红B的催化效能

采用自蔓延溶胶凝胶法分别制备了铁氧化物和铁铜复合氧化物催化剂,以酸性红B为降解对象,对比了单独臭氧氧化、铁氧化物和铁铜复合氧化物催化臭氧氧化对酸性红B的降解效果,考察了磁力搅拌速度(500～1 640 r/min)、溶液pH(3～11)、臭氧投加速率(3.55～28.4 mg/min)对铁铜复合氧化物催化性能的影响。结果表明,与单独臭氧氧化比较,铁氧化物和铁铜复合氧化物均能加速酸性红B的降解,促进色度和COD的去除,结合催化剂的表征结果,推断催化剂表面羟基促进臭氧分解产生.OH是其氧化性能较好的主要原因,另外,催化剂的吸附能力对催化性能也有一定影响。随着磁力搅拌速度、溶液pH、臭氧投加速率的增大,铁铜复合氧化物催化臭氧氧化酸性红B的效果越好。     

硝酸氧化和负载铁氧化物改性活性炭催化臭氧化性能

采用硝酸氧化与硝酸铁负载对颗粒活性炭进行改性处理,研究了活性炭样品表面官能团的变化,分析了活性炭样品对酸性大红3R吸附和催化臭氧化能力,探讨了p H值与·OH捕获剂对催化臭氧化效果的影响。结果表明,硝酸改性后活性炭表面羧基、内酯基、酚羟基以及总官能团的含量均明显增加,其中羧基增幅最大;负载铁氧化物后,活性炭表面官能团数量有所降低。活性炭样品化学吸附性能随官能团含量的增加而增强。催化臭氧化对酸性大红3R的氧化降解效果明显优于单独臭氧化。增加表面官能团含量可以加速催化臭氧化反应,但反应速率随着表面官能团消耗而降低;负载金属组分具有更为稳定和有效的催化臭氧化活性。活性炭催化臭氧化性能在碱性条件下明显优于酸性条件,且随着p H值升高而提高。投加·OH捕获剂(Na2CO3)后,其对·OH的消耗使得催化臭氧化效果显著下降。     

新型复合预氧化技术控制副产物的试验研究

臭氧被广泛应用于饮用水预氧化工艺中,但是成本较高,而且会生成臭氧化副产物,如可同化有机碳(AOC)、溴酸盐和甲醛.因此,提出臭氧/高锰酸钾复合预氧化技术,并对照预臭氧化技术,进行了消毒副产物前质及臭氧化副产物控制的小试试验研究.结果表明,与预臭氧化(1.5 mg/L臭氧)相比,复合预氧化(0.6 mg/L臭氧 0.4 mg/L高锰酸钾)能促进混凝沉淀对消毒副产物前质的去除,总去除率与单独预臭氧化的去除率相当.而且又能降低AOC生成量,并促进混凝沉淀对AOC的去除,合计AOC去除率达43%左右.此外,对溴酸盐和甲醛生成量也有明显去除效果,比单独预臭氧化降低了78.4%和21.2%.     

铈类催化剂催化臭氧化的研究进展

催化臭氧化由于能产生无选择性的羟基自由基(·OH),克服了传统单独臭氧对有机污染物具有选择性的局限。典型非均相催化臭氧化体系常利用金属氧化物作为催化剂,其中铈氧化物由于具有良好的催化臭氧化效果而被广泛研究。整理了铈类催化剂在催化臭氧化中的研究进展,介绍了常规铈类催化剂的制备方法,总结了铈类催化剂的催化臭氧化机理,包括吸附理论、自由基理论和臭氧直接氧化。根据催化剂的复合物形式,可将铈类催化剂分为活性炭负载型、介孔材料负载型和金属氧化物复合型3种。对各种铈类催化剂的应用现状及催化效果进行介绍,并对其发展趋势进行展望。     

催化强化臭氧氧化处理化工园区生化尾水

以陶粒为载体,以Ti O2,Fe2O3,Mn O2为活性组分,考察不同活性组分的陶粒作为催化剂对化工园区生化尾水臭氧氧化能力的强化情况。结果表明,3种负载型催化剂均能有效强化臭氧氧化过程,显著降低生化尾水Abs、UV254以及COD等指标,其中以Fe2O3/陶粒的催化强化效果最为显著,能显著降低生化尾水在200~250 nm处的吸波强度,尾水UV254从0.580降至0.320,COD从240 mg/L降至194 mg/L。     

Mn_3O_4催化臭氧化处理钻井废水

采用锰系氧化物对钻井废水进行催化臭氧化处理,考察了不同初始pH、催化剂投加量以及臭氧投加量等因素对COD去除率的影响,探讨了Mn3O4表面电荷情况、化学吸附特性及催化臭氧产生·OH机理。结果表明,在初始pH为12,催化剂投加量为5g/L,臭氧投加量为18 mg/min,反应时间为20 min时,Mn3O4较Mn O2和单独臭氧氧化去除COD的效果更明显;Mn3O4的表面带负电荷,发生了水合羟基化过程,且Mn3O4与钻井废水中的污染物产生了化学吸附;臭氧与锰原子形成σπ-键合吸附于Mn3O4表面,经π*轨道能级的下降而进入活化状态,最终导致吸附于Mn3O4表面的OH-与臭氧相互作用产生·OH。     

NiO-MgO复合金属氧化物催化分解N_2O

采用溶胶凝胶法制备了一系列不同Ni/Mg比的NiO-MgO复合氧化物催化剂,并考察了其N_2O催化分解性能。结果表明,NiO-MgO催化剂的N_2O催化分解活性明显优于单一NiO和MgO,当MgO含量为5%时,NiO-MgO复合金属氧化物上N_2O分解活性最佳。XRD、H2-TPR和XPS结果表明,Ni2+是催化分解N_2O的主要活性位点。Mg不作为活性组分,但可通过Ni、Mg之间强烈的相互作用提高催化剂氧化还原能力,进而促进N_2O的催化分解。此外,Mg的加入促进了催化剂中NiO的形成。     

锰负载量对MnO_x/PG催化剂低温SCR反应的影响

凹凸棒石负载锰氧化物(MnO_x/PG)催化剂是一种新型高效的低温选择性催化还原(SCR)催化剂。锰氧化物负载量对催化剂的脱硝活性影响显著,针对不同质量分数锰氧化物负载量的催化剂的SCR反应行为进行了动力学研究。结果表明:增加锰的负载量不改变反应表观活化能,锰氧化物负载量的增加在考察范围内具有一致的组分形态和化学活性;反应活性中心的数量随负载量的增加而增长是催化剂活性增长的主要原因。结合前期NH_3-TPD研究,进一步明确氨主要在载体上吸附,锰的负载主要促进了吸附态氨的活化过程。     

Catalytic activity of Ru/Al2O3 for ozonation of dimethyl phthalate in aqueous solution

With dimethyl phthalate as the model pollutant and Ru/Al(2)O(3) as catalyst, this paper systemically investigates the removal of total organic carbon (TOC) of system. Our results have confirmed that Ru/Al(2)O(3) can significantly increase the effect of ozonation. TOC removal in 120 min can reach 72% while only 24% with ozone alone. The optimal catalyst preparing condition was 0.1 wt% Ru content, 600 degrees C calcination temperature, 0.5-1.0mm particle diameter, which is characterized by a high surface area and a large population of surface active sites. The contrasting experiments of ozone alone, catalyst adsorption after ozonation, and catalytic ozonation confirmed that catalytic reaction was the most important process to TOC removal in system with Ru/Al(2)O(3) as catalyst.     

Advanced oxidation of natural organic matter using hydrogen peroxide and iron-coated pumice particles

The oxidative removal of natural organic matter (NOM) from waters using hydrogen peroxide and iron-coated pumice particles as heterogeneous catalysts was investigated. Two NOM sources were tested: humic acid solution and a natural source water. Iron coated pumice removed about half of the dissolved organic carbon (DOC) concentration at a dose of 3000 mg l(-1) in 24 h by adsorption only. Original pumice and peroxide dosed together provided UV absorbance reductions as high as 49%, mainly due to the presence of metal oxides including Al(2)O(3), Fe(2)O(3) and TiO(2) in the natural pumice, which are known to catalyze the decomposition of peroxide forming strong oxidants. Coating the original pumice particles with iron oxides significantly enhanced the removal of NOM with peroxide. A strong linear correlation was found between iron contents of coated pumices and UV absorbance reductions. Peroxide consumption also correlated with UV absorbance reduction. Control experiments proved the effective coating and the stability of iron oxide species bound on pumice surfaces. Results overall indicated that in addition to adsorptive removal of NOM by metal oxides on pumice surfaces, surface reactions between iron oxides and peroxide result in the formation of strong oxidants, probably like hydroxyl radicals, which further oxidize both adsorbed NOM and remaining NOM in solution, similar to those in Fenton-like reactions.     

NH_4＋和H_2O_2抑制臭氧氧化过程中溴酸盐形成的效能研究

通过纯水条件下的模拟研究,考察NH4＋和H2O2在单独和联用时对臭氧氧化过程中溴酸盐形成的抑制效能。结果表明,单独投加NH4＋能显著降低溴酸盐的生成量,并对水中臭氧浓度衰减无明显影响;投加H2O2大于0.20 mmol/L时,能在一定程度上抑制溴酸盐的形成,但加快了水中臭氧浓度的衰减;同时投加过量H2O2和NH4＋时,...     

Catalytic reduction of N2O over Ag-Pd/Al2O3 bimetallic catalysts

A study of the catalytic conversion of N2O to N2 over a bimetallic Ag-Pd catalyst is described in this article. Several Ag-Pd catalytic systems were prepared supported on Al2O3 with different ratios and their catalytic activity for the direct decomposition of N2O and their reduction with CO was measured. Based on the experimental results, it was observed that Ag-Pd bimetallic catalyst (5-0.5%) was the most active for both nitrous oxide reduction and direct decomposition. This high activity seems to be connected with a synergistic effect between Ag and Pd.     

NH_4＋和H_2O_2抑制臭氧氧化过程中溴酸盐形成的效能研究

通过纯水条件下的模拟研究,考察NH4＋和H2O2在单独和联用时对臭氧氧化过程中溴酸盐形成的抑制效能。结果表明,单独投加NH4＋能显著降低溴酸盐的生成量,并对水中臭氧浓度衰减无明显影响;投加H2O2大于0.20 mmol/L时,能在一定程度上抑制溴酸盐的形成,但加快了水中臭氧浓度的衰减;同时投加过量H2O2和NH4＋时,相对单独投加过量H2O2条件进一步抑制了溴酸盐的形成,但相对单独投加NH4＋条件却促进了溴酸盐的形成。     

Silane removal at ambient temperature by using alumina-supported metal oxide adsorbents

Copper, zinc, and cerium oxide adsorbents supported on alumina were used to remove silane gas (SiH4). The adsorbents were prepared using a coprecipitation method and characterized by the inductively coupled plasma mass spectrometry, X-ray powder diffractometer, and Brunauer-Emmett-Teller method (BET). The silane removal efficiency and adsorption capacity of the adsorbents were investigated in this study. Test results showed that the adsorbents containing active species had a removal efficiency >99.9% for SiH4 before breakthrough. Adsorbents containing mixed oxides (CuO-CeO2/ Al2O3 and CuO-ZnO/Al2O3), which showed well-dispersed active species and high BET surface areas, had a greater adsorption capacity than the adsorbents containing single metal oxide. However, when the CuO-ZnO/ Al2O3 adsorbents contain >40 wt% of active metal oxides, the increase of active species lowered the BET surface area leading to a decrease of the adsorption capacity. Additionally, when the content of the active metal oxides was between 20% and 40%, the CuO-ZnO/Al2O3 adsorbents demonstrated higher adsorption capacity.     

Effects of copper and palladium on the reduction of bromate by Fe(0)

Bromate reduction by Fe(0) with incorporation of copper or palladium was investigated in batch tests. The incorporation of copper led to an increase in the rate of bromate reduction, while incorporation of palladium did not show any effect on bromate reduction by Fe(0), regardless of the bimetal application techniques (either simultaneous addition of Cu(II) or Pd(IV) into the Fe-BrO3- reaction system or using copper or palladium amended iron for bromate removal). Surface analyses by X-ray photoelectron spectroscopy (XPS) and X-ray powder diffraction (XRD) techniques indicated that aqueous Cu(II) was reduced and incorporated into the iron surface to form Cu2O and Cu(0). Among these two species, pure Cu(0) is not an active electron donor to the bromate reduction reaction, as shown by there being no reduction from using Cu(0) powders alone and no enhancement by Fe(0) when physically mixed with Cu(0). Although it has been proposed in the literature that the enhancement of adsorption also contributes to the enhancement of chemical reduction, this is not the case here because adsorption decreased when Cu increased. The enhanced bromate reduction rate in the presence of copper observed here is most likely the result of the newly formed active Cu(I). The presence of PdO was evidenced by XPS but yielded no enhancement in bromate reduction. Finally, the Cu2O present on the iron surface because of copper impurities in commercially available iron was found to be involved in the bromate reduction and to accelerate the reduction rate.