Effect of the ozone-carbon reaction on the catalytic activity of activated carbon during the degradation of 1,3,6-naphthalenetrisulphonic acid with ozone

The present work investigated the evolution of catalytic activity of activated carbon in 1,3,6-naphthalenetrisulphonic acid (NTS) ozonation in aqueous phase. Activated carbons pre-treated with ozone showed a reduction in NTS oxidation rate and efficacy of TOC removal that increased with ozone exposure time. The ozone treatment increased the number of surface oxygenated (electron-withdrawing) groups on the carbon, therefore reducing its basic character and its reductive properties. This effect reduced the reactivity of the activated carbon to ozone and, therefore, the extent of the ozone decomposition into highly oxidative species.     

Ozonation of 1,3,6-naphthalenetrisulphonic acid catalysed by activated carbon in aqueous phase

This paper presents experimental results of the ozonation of a model aromatic sulphonic compound, 1,3,6-naphthalenetrisulphonic acid (NTS), in the presence of different activated carbons with different physical and chemical surface properties. Carbons used were commercial activated carbons (Ceca AC40, Norit, Merck, Witco, Ceca GAC, Filtrasorb 400, Sorbo) with or without demineralisation pre-treatment. Carbon samples were texturally and chemically characterised using N₂ adsorption isotherms, mercury porosimetry, pH_PZC, selective neutralisation and elemental analysis. Results show that NTS was degraded by ozone at a faster rate in the presence of activated carbon, especially in the case of Sorbo, Ceca GAC and Norit carbons, which display catalytic activity, probably by enhancing ozone decomposition in aqueous phase in highly oxidative species. These catalytic properties seem to be favoured by both the basicity of the carbon surface and the higher macropore volume. Dissolved total organic carbon from the NTS degradation compounds was removed in the presence of activated carbon through both the catalytic activity of activated carbon to mineralise organic matter and the adsorption of these organic compounds on activated carbon.     

Influence of the surface chemistry of multi-walled carbon nanotubes on their activity as ozonation catalysts

Multi-walled carbon nanotubes (MWCNTs) with different surface chemical properties were prepared by oxidative treatments with HNO₃, H₂O₂ and O₂ to introduce oxygen-containing surface groups and by thermal treatments for their selective removal. The texture and surface chemistry of the MWCNTs were characterized by nitrogen adsorption, temperature programmed desorption (TPD) and pH at the point of zero charge. A deconvolution procedure of the TPD spectra was used to quantify the oxygenated surface groups. These materials were used as catalysts for ozone decomposition, and for the ozonation of oxalic and oxamic acids. Generally, all these catalytic processes are favoured by carbon nanotubes with low acidic character. MWCNTs were shown to exhibit higher activity for the ozonation of oxalic and oxamic acids, compared to activated carbon. Successive experimental runs of oxalic acid removal carried out with a selected MWCNT sample show that the catalyst suffers some deactivation as a result of the introduction of oxygenated groups on the surface. Therefore, the effect of the surface chemistry is mainly observed for the fresh catalysts.     

Surface‐Treated Activated Carbon for Removal of Aromatic Compounds from Water

Modifications of commercial activated carbons by chemical treatment with HNO₃ or HCl and HF and the adsorption behavior of simple aromatic compounds (aniline, pyridine, phenol, and benzene) on activated carbon and modified activated carbon were investigated. The results show that the textural properties change a little after these modifications, but the surface acidity (mainly oxygen‐containing groups) of activated carbon modified with HNO₃ increases greatly. The effect of ash of activated carbon on adsorption of the organic compounds mentioned above is insignificant. However, addition of surface acidity (mainly surface oxygen‐containing groups) decreases the adsorption capacity of compounds significantly. The adsorption uptake of compounds on activated carbon with oxidation of HNO₃ is low possibly due to dispersive interaction, water cluster blocking, or competition between water and compounds adsorbed on activated carbon's surface because of hydrophilic increase of the activated carbon surface. The solubility of aromatic compounds in water has an important effect on the adsorption capacity of activated carbon. q_m and K_L (Langmuir adsorption parameters) for the aromatic compounds vary similarly.     

Influence of Ozonation of Humic and Fulvic Acids on Diuron Adsorption on Activated Carbon

The effect of ozonation on the competitor effect of humic and fulvic acids against diuron in adsorption on activated carbon in drinking water process has been studied. Ozonation treatment allows the removal of herbicides from drinking waters by modification of humic and fulvic acids structures. These latest are responsible for their adsorption variation on activated carbon. An ozone dose similar to that used in industrial pre-ozonation (1.3?mg ozone/l) does not cause significant transformations of humic and fulvic acids which could decrease their competitor effect and increase significantly the adsorption capacity of the activated carbon for a well-adsorbed pesticide like diuron.     

活性炭吸附甲烷和甲苯的分子模拟研究

以石墨片微元构建的多孔碳材料作为活性炭的结构模型,采用巨正则蒙特卡罗方法(GCMC)和分子动力学方法(MD),从分子层面研究甲烷和甲苯在活性炭中的吸附和扩散特性. 结果表明,石墨片微元大小对多孔碳材料吸附甲烷和甲苯有一定影响,37个碳环构成的多孔碳材料是最佳的吸附结构;甲烷气体在活性炭材料中扩散较快,甲苯在活性炭中扩散较慢,随碳环碳原子数增加,气体在多孔碳材料中的自扩散系数逐渐增大;引入基团会使最优密度向高密度方向偏移,用不同基团表面改性的吸附量顺序为羟基>氨基>羧基>未改性,基团引入会改善材料的孔结构,有利于吸附量的增加.     

Metal-loaded polystyrene-based activated carbons as dibenzothiophene removal media via reactive adsorption

To improve the desulfurization capability of activated carbons, new metal-loaded carbon-based sorbents containing sodium, cobalt, copper, and silver highly dispersed within the carbon matrix were prepared and tested at room temperature for dibenzothiophene (DBT) adsorption. The content of metals can be controlled by selective washing. The new adsorbents showed good adsorption capacities and selectivity towards DBT. The metals incorporated to the surface act not only as active sites for selective adsorption of sulfur-containing aromatic compounds, but also as structural stabilizers of the carbon materials, and as catalyst initiators in reactive adsorption. Depending on the reactivity of the metal used, the adsorption capacity of the activated carbons significantly varied. Cobalt and copper loaded carbons showed the highest uptakes, due to not-well defined catalytic synergetic effects. Besides, the presence of sulfur compounds in the structure of the carbon as a result of the sulfonic moiety of the precursor, results in sulfur-sulfur specific interactions leading to an enhancement in the adsorption capacity for DBT removal.     

Influence of the Surface and Structural Characteristics of Activated Carbons on Adsorptive Removal of Halo-Olefinic Impurities from 1,1,1,3,3-Pentafluoropropane

abstract Halo-olefinic impurities in 1,1,1,3,3-pentafluoropropane (HFC-245fa) product used as blowing agents, etc. could damage the human body and must be removed. Activated carbon was treated by HCl, ...     

Interaction of O<Subscript>2</Subscript>, O<Subscript>3</Subscript>, and H<Subscript>2</Subscript>O<Subscript>2</Subscript> with an activated carbon

The results of the modification of AG-OV-1 activated carbon under various conditions (by atmospheric oxygen at elevated temperatures and by hydrogen peroxide or ozone) are given. The effect of the used modifier on changes in the porosity, surface state, and adsorption capacity of activated carbon is evaluated.     

活性炭表面含氧官能团对水中卤乙酸吸附去除的影响

为了改善极性、亲水性卤乙酸(HAAs)分子在非极性、疏水性活性炭上的吸附性能,利用N₂等温吸附实验、X射线光电子能谱实验（XPS）、HAAs等温吸附实验等方法,对几种不同产地的活性炭孔隙结构、表面元素形态结构组成,以及HAAs吸附性能进行了研究,考察了活性炭孔结构及含氧官能团对HAAs吸附性能的影响.活性炭表面含氧官能团对HAAs的吸附性能影响显著,当活性炭表面含氧官能团组成较小时,其HAAs吸附能力较强.     

Gallic acid water ozonation using activated carbon

The ozonation of gallic acid in water in the presence of activated carbon has been studied at pH 5. Hydrogen peroxide, ketomalonic and oxalic acids were identified as by-products. The process involves two main periods of reaction. The first period, up to complete disappearance of gallic acid, during which ozonation rates are slightly improved by the presence of activated carbon. The second one, during which activated carbon plays an important role as promoter, and total mineralization of the organic content of the water is achieved. The organic matter removal is due to the sum of contributions of ozone direct reactions and adsorption during the first period and to a free radical mechanism likely involving surface reactions of ozone and hydrogen peroxide on the carbon surface during the second period. There is a third transition period where by-products concentration reach maximum values and ozonation is likely due to both direct and free radical mechanisms involving ozone and adsorption. Discussion on the mechanism and kinetics of the process is also presented both for single ozonation and activated carbon ozonation.     

活性炭表面热氧化对其吸附二苯并噻吩性能影响

本文主要研究活性炭表面氧化对其吸附二苯并噻吩性能的影响。将活性炭在不同低温下氧化制得表面氧化活性炭，用静态吸附法进行了二苯并噻吩在初始及氧化活性炭上的吸附等温线，应用Langmuir方程对吸附等温线进行拟合，用漫反射红外谱（DRIFTS）表征活性炭表面含氧基团，用Boehm滴定测定活性炭表面官能团含量，讨论了活性炭表面化学性质对其吸附二苯并噻吩的影响。结果表明：活性炭表面酸性含氧基团对二苯并噻吩的吸附有重要影响，酸性含氧基团越多，其吸附量越大。低温气相氧化活性炭提高了活性炭表面酸性含氧基团，提高了其对二苯并噻吩的吸附。氧化温度越高，其表面含氧基团含量越多，其对二苯并噻吩的吸附量也越大。Langmuir吸附等温线可适用于描述二苯并噻吩在活性炭表面上的吸附。     

酸、碱改性活性炭对甲醇、甲苯吸附性能

分别采用硝酸和氢氧化钠对活性炭进行改性,利用比表面积及孔径分析仪（BET）、扫描电镜（SEM）、Boehm滴定法对活性炭物化性质进行表征,测试改性活性炭对甲醇、甲苯吸附性能。结果表明,经过酸、碱改性后的活性炭比表面积、总孔容、微孔孔容均有所增大。酸改性表面酸性基团增加,碱改性后活性炭酸性基团减少。酸改性后的活性炭对甲醇、甲苯吸附能力有所下降,后经碱改性的活性炭吸附能力均有不同程度的提高。单组分吸附实验时,甲醇穿透曲线斜率要大于甲苯,穿透时间早于甲苯。在多组分吸附过程中会出现甲苯取代甲醇的吸附现象,使得已经被吸附的甲醇发生脱附,此时甲醇的出口浓度大于进口浓度,形成峰值效应。     

Adsorption of o-xylene and p-xylene from water by SWCNTs

The influences of nitric acid oxidation on the surface properties and the adsorption capacity of single-walled carbon nanotubes (SWCNTs) were investigated in this work. To eliminate the size effects on the adsorption capacity, o-xylene and p-xylene were used as model adsorbates. It was found that purification of the SWCNTs by nitric acid significantly increased the internal surface area as well as the micropore volume of the SWCNTs, and introduced oxygen-containing surface groups. The adsorption capacities of the SWCNTs for o-xylene and p-xylene were mainly influenced by the positions of the methyl groups on the xylene molecules and the presence of oxygen-containing groups on the surface of the SWCNTs. Results also indicated that purification greatly changes the adsorption of o-xylene by the SWCNTs. This could be attributed to the dispersive attractions and the electrostatic repulsions between o-xylene molecules and the surface of the purified SWCNTs, which are introduced by the oxygen-containing surface groups. When compared to the as-grown and the purified SWCNTs, activated carbon had a greater adsorption capacity because of its large specific surface area and the absence of oxygen-containing surface groups. However, when the adsorption capacity was calculated based on surface area, the as-grown SWCNTs had a greater adsorption capacity than did the activated carbons because the micropore size of the activated carbon is mainly smaller than the size of a xylene molecule.     

改性活性炭的表面特性及其对苯酚的吸附性能

研究了表面改性对活性炭吸附苯酚性能的影响。研究发现,硫酸氧化可增加活性炭表面酸性基团的含量,提高了活性炭的表面亲水性,降低pHPZC值,因而对吸附水中的苯酚的性能产生明显影响,降低了对苯酚的吸附。     

Effect of ozone and ozone/activated carbon treatments on genotoxic activity of naphthalenesulfonic acids

Naphthalenesulfonic compounds are widely used, mainly by the textile industry in the synthesis of azoic colorants. The presence of the sulfonic group is known to endow these compounds with high water‐solubility and low biodegradability, although its influence on their genotoxic activity is unknown. The use of energetic oxidants is recommended for the degradation of organic compounds which are refractory to biological treatment. Ozone and ozone/activated carbon have been proposed as the best alternatives to remove these compounds. The results showed that the more sulfonic groups there are on the aromatic ring of this family of contaminants, the lower is their genotoxic activity. All the compounds studied presented genotoxic activity at elevated concentrations. Ames test results indicate that DNA damage was produced by substitution of nitrogenated bases. The system based on the combined use of ozone and activated carbon was the most efficacious in the depuration of water containing these contaminants. This approach rapidly degraded the naphthalenesulfonic acids, eliminated their genotoxic activity and reduced their organic material content using low doses of ozone. © 2002 Society of Chemical Industry     

Mechanisms of surfactant adsorption on non-polar, air-oxidized and ozone-treated carbon surfaces

Ozone treatment of fly ash carbon has recently been reported to inhibit the adsorption of commercial surfactants in concrete paste, thus mitigating the known negative effects of carbon on ash utilization. This paper examines the general mechanism of surfactant adsorption on carbon and its suppression by surface oxidation. Experimental results are presented for two carbon types (carbon black, fly ash carbon), both raw and surface oxidized (by ozone and molecular oxygen) and several commercial anionic and non-ionic surfactants (Darex II, SDS, Tergitol). The treated carbon surfaces were characterized with XPS, FT-IR, thermal desorption in N₂ and H₂/He, surface acidity, hygroscopic behavior, interfacial energy and its components through contact angle measurement involving standard liquid probes. Surface oxidation is found to decrease surfactant adsorption in each of the carbon/oxidant/surfactant systems examined, and its effect correlates with the amount of surface oxides by XPS. The combined results suggest that surfactant adsorption primarily occurs on non-polar carbon surface patches where it is driven by hydrophobic interactions. The main mechanism of oxidative suppression is the destruction of this non-polar surface, though micropore blockage and increased negative surface charge may also contribute for some systems.     

花生壳活性炭的表征,表面改性及吸附脱除水中Pb2+离子

Metal ion contamination of drinking water and waste water, especially with heavy metal ion such as lead, is a serious and ongoing problem. In this work, activated carbon prepared from peanut shell (PAC) was used for the removal of Pb2 from aqueous solution. The impacts of the Pb2 adsorption capacities of the acid-modified carbons oxidized with HNO3 were also investigated. The surface functional groups of PAC were confirmed by Fourier transform infrared (FTIR) spectroscopy, X-ray photoelectron spectroscopy (XPS), Boehm titration. The textural properties (surface area, total pore volume) were evaluated from the nitrogen adsorption isotherm at 77K. The experimental results presented indicated that the adsorption data fitted better with the Langmuir adsorption model. A comparative study with a commercial granular activated carbon (GAC) showed that PAC was 10.3 times more efficient compared to GAC based on Langmuir maximum adsorption capacity. Further analysis results by the Langmuir equation showed that HNO3 [20% (by mass)] modified PAC has larger adsorption capacity of Pb2 from aqueous solution (as much as 35.5mg.g1). The adsorption capacity enhancement ascribed to pore widening, increased cation-exchange capacity by oxygen groups, and the promoted hydrophilicity of the carbon surface.     

Effect of Sonication in the Preparation of Activated Carbon Particles on Adsorption Performance

The impact of acid and base adsorption capacities of activated carbon (AC) particles with activation condition, contact time, specific surface area (SSA), particle size, concentration, and temperature was studied. AC was pre-treated by sonication to improve the surface characteristics and enhance its adsorption capacity. Sonication increased the SSA of AC. SEM imaging showed good dispersion and uniform AC particles with an average diameter of about 0.6 μm. The adsorption results demonstrated that AC surfaces possessed effective interactions with acids and bases, and the greatest adsorption capacity was achieved with CH₃COOH, where data were analyzed by Freundlich and Langmuir isotherms. It was found that the isotherm data correlated well with the Freundlich isotherm. Adsorption of raw AC particles increased under sonication conditions. The adsorption process with sonicated and unsonicated AC particles obeyed pseudo first-order kinetics.     

一步快速活化法制备生物质活性炭及其对乙酸乙酯的吸附再生

活性炭吸附法因技术成熟、简单易行、吸附效率高等优点而被广泛应用于挥发性有机化合物（VOCs）的处理中。本文以山林废弃物的野山桃核为原料,烟道废气及硝酸铁为活化剂,制备了一系列生物质活性炭,并利用固定床吸附装置对其吸附、再生性能进行了研究。利用二氧化碳和水蒸气模拟烟气,在固定流量的烟气活化氛围中进行活化,并探讨了不同硝酸铁的量对活性炭的孔隙结构及其吸附再生性能的影响。利用N₂ 吸附-脱附实验、扫描电镜、拉曼光谱和红外光谱等技术研究了活性炭详细特征。结果表明：当硝酸铁的质量分数为0.2% 时,所制备的活性炭AC-3具有最大的比表面积和平均孔径,分别为923m2/g及2.57nm。其对乙酸乙酯的饱和吸附量也最大,为973.04mg/g。利用烟气对AC-3活性炭进行活化再生处理,经过3次重复吸附-解吸再生实验,其饱和吸附能力仍可达91.5％以上,实现了废弃烟气资源化利用及活性炭的循环回收,从而达到废气治理的目标。