Synthesis and physicochemical characterizations of nanostructured Pd/carbon-clinoptilolite-CeO2 catalyst for abatement of xylene from waste gas streams at low temperature

Xylene removal from waste gas streams was carried out via catalytic oxidation over Pd/carbon-clinoptilolite-CeO₂. The synthesized samples were characterized by XRD, FESEM, BET, FTIR and TG techniques. The XRD patterns confirmed the formation of nano ceria with an average crystallite size of 11.6 nm. FESEM results indicated a good morphology for prepared carbon with deep pores, confirmed structure modification of zeolite, and showed that nanocatalyst has nanometric particles with an average size of 60.85 nm. Reaction data illustrated 98% abatement of xylene at 250 °C. The stability test of catalyst demonstrated that the removal efficiency has remained constant for 1200 min.     

低负载Pd/Al2O3催化剂的制备及其对CO室温催化性能研究

采用等体积浸渍法和还原法结合制备了Pd/Al2 O3催化剂,通过N2吸附-脱附、SEM、TEM、X射线衍射、X射线光电子能谱和CO原位漫反射傅里叶变换红外光谱等表征手段对制备的样品微观结构进行了系统分析,考察了不同Pd负载量和测试条件下CO催化氧化性能.实验结果表明,水合肼还原法实现了Pd在Al2 O3载体上的均匀分散...     

Pd/PA-Ca催化剂低温催化苯甲醛氧化制备苯甲酸

以植酸钙(PA-Ca)为载体、H2Pd Cl4为前驱体、甲醇为还原剂,制备了PA-Ca负载Pd的Pd/PA-Ca催化剂,对其进行XRF、BET、SEM、TEM、XRD和XPS表征,并用于苯甲醛氧化制备苯甲酸反应,考察催化剂用量、反应温度和溶剂种类对催化剂催化性能的影响。结果表明,催化剂中负载Pd质量分数为1.03%,钠质量分数为1.05%;合成的PA-Ca载体为晶化程度较低的介孔材料,比表面积为18.85 m~2·g~(-1);催化剂活性物种为Pd0和PdO。在催化剂用量n(苯甲醛)∶n(Pd)=2 000∶1、乙腈作溶剂、O_2压力101.325 k Pa(流速20 m L·min~(-1))、反应温度30℃和反应时间4 h条件下,苯甲醛转化率为83%,苯甲酸选择性为100%;催化剂具有较好的稳定性,可循环使用3~4次。     

Preparation and characterization of core‐shell polystyrene/polyaniline/Pd composites and their catalytic properties for the reduction of 4‐nitrophenol

Herein, polystyrene/polyaniline/Pd (PS/PANI/Pd) core‐shell composite catalysts were prepared by a facile swelling‐diffusion‐interfacial polymerization method. PS microparticles were firstly prepared by dispersion polymerization and were swollen by aniline monomer without any surface modification. H₂PdCl₄ acid was used as palladium precursor. The was adsorbed on the surface of aniline‐swollen PS microparticles because of the electrostatic attraction between and anilinium positive ions protonated by H⁺, which was diffused from the aniline‐swollen PS microparticles. Then HCl solution was added to control the diffusion rate of anilinium positive ions and ammonium persulfate (APS) was used to polymerize the anilinium ions to get PANI shell. Due to the redox activity between PANI and Pd ions, Pd nanoparticles can be in situ formed on the surfaces of PS. Therefore, the core‐shell PS/PANI/Pd composite catalysts were obtained. The morphology and structure of the obtained composites was characterized by TEM, FT‐IR and EDX. Results showed that the products presented excellent catalytic properties for the reduction of 4‐nitrophenol (4‐NP) to 4‐aminophenol (4‐AP) in the presence of NaBH₄ by virtue of the interaction between Pd nanoparticles and conducive PANI shell. The catalytic reaction obeyed the pseudo‐first‐order reaction equations and the reaction rate constants were also calculated in this article. © 2017 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2017 , 134, 44812.     

亚硝酸甲酯羰基化合成草酸二甲酯废旧催化剂Pd/α-Al2O3中Pd的提取

采用HCl+H₂O₂混合溶液浸泡废旧催化剂Pd/α-Al₂O₃,滤掉氧化铝球颗粒,加入氨水沉淀滤液中Pd之外的微量杂质并过滤,在滤液中加入丁基钠黄药,形成Pd化合物沉淀,过滤,100 ℃烘干,350 ℃焙烧,生成PdO,纯度99.541%,再用H₂或CO在≥700 ℃下还原,得到纯Pd。该方法成本低,相对于王水法更环保、高效,Pd回收率>99.99%。     

Degradation of benzene,toluene ethylbenzene and p‐xylene (BTEX) in aqueous solutions using UV/H2O2 system

The homogeneous degradation of benzene (B), toluene (T), ethylbenzene (E) and p‐xylene (X) (BTEX) was studied in aqueous solutions, at pH 3.0, of hydrogen peroxide (5.8 mM ) under UV irradiation in a photoreactor equipped with a 300 nm lamp of light intensity 3.5 × 10^?5 Ein L^?1 min^?1. BTEX was substantially degraded by the H₂O₂/UV system, with >90% disappearing in 10 min of irradiation. The decomposition of BTEX was studied either as single or as multi‐component systems. The effects of irradiation time, amounts of H₂O₂ in molar ratios, rate of degradation and competition between components were thoroughly examined. It can be stated that the rate of BTEX degradation in mixture was higher than those for the individual components due to external effects of the absorption of UV light by the mixture, and their effects on enhancing the formation of OH^? radicals. The appropriate figure of merit, the electrical energy per mass (EE/M), was estimated at various molar ratios and it was confirmed that the best value was the one depicted for p‐xylene (0.065 kWh kg^?1). A theoretical model for the degradation pathway was proposed. Copyright © 2004 Society of Chemical Industry     

Complete oxidation of methane at low temperature over Pt and Pd catalysts for the abatement of lean-burn natural gas fuelled vehicles emissions: influence of water and sulphur containing compounds

The catalytic activity of fresh Pd and Pt catalysts supported on γ-alumina in the complete oxidation of CH₄ traces under lean-burn conditions was studied in the presence or the absence of water or H₂S. Steam-aged catalysts were also studied in order to simulate long-term ageing in real lean-burn natural gas fuelled vehicles (NGVs) exhaust conditions. Without water or H₂S added to the feed, Pd catalysts exhibit a superior catalytic activity in methane oxidation compared to Pt ones, whatever the catalysts were fresh or aged. The addition of 10 vol.% water vapour to the feed strongly affects the activity of the fresh Pd catalyst, thus being only slightly more efficient than the fresh Pt one. H₂S has a strong poisoning effect on the catalytic activity of Pd catalysts, while Pt catalysts are more resistant. The fresh H₂S-poisoned Pd/Al₂O₃ catalyst was studied by TPD in O₂/He. Poisoning species decompose above 873 K as SO₂ and O₂ in relative concentrations consistent with the decomposition of surface sulphate species. However, a treatment in O₂/He at temperatures as high as 923 K does not allow the complete regeneration of the catalytic activity of H₂S-poisoned Pd/Al₂O₃. A mechanism involving the poisoning of PdO by sulphate species is proposed. Different diffusion processes by which these sulphate species can migrate back and forth between PdO and the support, depending on the experimental conditions, are suggested.     

纳米Ce0.9Cu0.1O2-δ 固溶体的制备、表征和CO低温氧化性能

采用改进的柠檬酸溶胶-凝胶法(即前驱体先在N₂气氛下高温预处理)制备了高比表面积纳米Ce_0.9^Cu_0.1O_2-δ固溶体。采用XRD、TEM和Raman等对催化剂进行表征，并考察了它们的低温CO氧化性能。研究结果表明，改进的柠檬酸溶胶 凝胶法可以制得晶相比较完整的Ce_0.9^Cu_0.1O_2-δ 固溶体，晶粒小于10 nm，明显小于常规方法制得的样品。随着样品焙烧温度的提高，表征氧缺位的600 cm^－1左右Raman峰的位置向高波数方向迁移。采用改进方法制得的Ce_0.9^Cu_0.1O_2-δ 固溶体具有更高的CO氧化活性，其原因归结为晶粒的减小，容易形成氧缺位和表面高分散CuO的增加，从而促进了CO的氧化。     

Microbial composition and structure of a multispecies biofilm from a trickle‐bed reactor used for the removal of volatile aromatic hydrocarbons from a waste gas

The microbial composition and structure of a multispecies biofilm of a laboratory‐scale trickle‐bed bioreactor for the treatment of waste gas was examined. The model pollutant was a volatile organic compound‐mixture of polyalkylated benzenes called Solvesso 100^®. Fluorescent in‐situ hybridization (FISH) and confocal laser scanning microscopy (CLSM) were applied. Two new Solvesso 100^®‐degrading Pseudomonas sp strains were isolated from the multispecies biofilm. Corresponding isolate‐specific oligonucleotide probes were designed and applied successfully. A major finding was that the fraction of Solvesso 100^®‐degrading bacteria in the biofilm was low (about 3–6% during long‐term operation). The majority of the active cells were saprophytes which utilized intermediates and cell lysis products. The measured fraction of extracellular polymeric substances of the mature biofilm was 89–93% of the total biomass. The CLSM examinations of a 3‐days‐old approx 10 µm thick biofilm revealed highly heterogeneous structures with distinguished three‐dimensional matrix‐enclosed microcolony bodies spread across the substratum surface. The 28‐days‐old 80–960 µm thick biofilm exhibited voids, cell‐free channels, and pores of variable sizes. In both cases, an even distribution of active cells and pollutant‐degrading bacteria throughout the biofilm cross‐section as well as through the biofilm depth was observed. Copyright © 2003 Society of Chemical Industry     

Synthesis, characterization and performance of CuO/La2O3 composite catalyst for ammonia catalytic oxidation

This work considers the oxidation of ammonia (NH₃) by selective catalytic oxidation (SCO) over a CuO/La₂O₃ composite catalyst at temperatures between 150 and 400 °C. A CuO/La₂O₃ composite catalyst was prepared by co-precipitation of copper nitrate and lanthanum nitrate at various molar concentrations. This study also considers how the concentration of influent NH₃ (C₀ = 1000 ppm), the space velocity (GHSV = 92,000 l/h), the relative humidity (RH = 12%) and the concentration of oxygen (O₂ = 4%) affect the operational stability and the capacity for removing NH₃. The catalysts that were characterized using FTIR, XRD, UV-Vis, BET and PSA, have shown that the catalytic behavior is related to the copper (II) oxide, while lanthanum (III) oxide may serve only to provide active sites for the reaction during a catalyzed oxidation run. The experimental results show that the extent of conversion of ammonia by SCO in the presence of the CuO/La₂O₃ composite catalyst was a function of the molar ratio. The ammonia was removed by oxidation in the absence of CuO/La₂O₃ composite catalyst, and around 93.0% NH₃ reduction was achieved during catalytic oxidation over the CuO/La₂O₃ (8:2, molar/molar) catalyst at 400 °C with an oxygen content of 4.0%. Moreover, the effect of the reaction temperature on the removal of NH₃ in the gaseous phase was also monitored at a gas hourly space velocity of under 92,000 h^− 1.     

Nano-gold supported on Fe2O3: A highly active catalyst for low temperature oxidative destruction of methane green house gas from exhaust/waste gases

A number of nano-gold catalysts were prepared by depositing gold on different metal oxides (viz. Fe₂O₃, Al₂O₃, Co₃O₄, MnO₂, CeO₂, MgO, Ga₂O₃ and TiO₂), using the homogeneous deposition precipitation (HDP) technique. The catalysts were evaluated for their performance in the combustion of methane (1 mol% in air) at different temperatures (300–600 °C) for a GHSV of 51,000 h⁻¹. The supported nano-gold catalysts have been characterized for their gold loading (by ICP) and gold particle size (by TEM/HRTEM or XRD peak broadening). Among these nano-gold catalysts, the Au/Fe₂O₃ (Au loading = 6.1% and Au particle size = 8.5 nm) showed excellent performance. For this catalyst, temperature required for half the methane combustion was 387 °C, which is lower than that required for Pd(1%)/Al₂O₃ (400 °C) and Pt(1%)/Al₂O₃ (500 °C) under identical conditions. A detailed investigation on the influence of space velocity (GHSV = 10,000–100,000 cm³ g⁻¹ h⁻¹) at different temperatures (200–600 °C) on the oxidative destruction of methane over the Au/Fe₂O₃ catalyst has also been carried out. The Au/Fe₂O₃ catalyst prepared by the HDP method showed much higher methane combustion activity than that prepared by the conventional deposition precipitation (DP) method. The XPS analysis showed the presence of Au in the different oxidation states (Au⁰, Au¹⁺ and Au³⁺) in the catalyst.     

An optimization and modeling approach for H2O2/UV‐C oxidation of a commercial non‐ionic textile surfactant using central composite design

BACKGROUND: Industrial surfactants are biologically complex organics that are difficult to degrade and may cause ecotoxicological risks in the environment. Until now, many scientific reports have been devoted to the effective treatment of surfactants employing advanced oxidation processes, but there is no available experimental study dealing with the optimization and statistical design of surfactant oxidation with the well‐established H₂O₂/UV‐C process. RESULTS: Considering the major factors influencing H₂O₂/UV‐C performance as well as their interactions, the reaction conditions required for the complete oxidation of a commercial non‐ionic textile surfactant, an alkyl ethoxylate, were modeled and optimized using central composite design‐response surface methodology (CCD‐RSM). Experimental results revealed that for an aqueous non‐ionic surfactant solution at an initial chemical oxygen demand (COD) of 450 mg L^?1, the most appropriate H₂O₂/UV‐C treatment conditions to achieve full mineralization at an initial pH of 10.5 were 47 mmol L^?1 H₂O₂ and a reaction time of 86 min (corresponding to a UV dose of 30 kWh m^?3). CONCLUSION: CCD allowed the development of empirical polynomial equations (quadratic models) that successfully predicted COD and TOC removal efficiencies under all experimental conditions employed in the present work. The process variable treatment time, followed by the initial COD content of the aqueous surfactant solution were found to be the main parameters affecting treatment performance, whereas the initial H₂O₂ concentration had the least influence on advanced oxidation efficiencies. The H₂O₂ concentration and surfactant COD were found to be more important for TOC abatement compared with COD abatement. Copyright © 2009 Society of Chemical Industry     

Modification and characterization of poly (ethylene terephthalate)‐grafted‐acrylic acid/acryl amide fiber for removal of lead from human plasma and environmental samples

A new fibrous adsorbent was prepared by grafting acrylic acid/acryl amide (AA/AAm) comonomers onto poly (ethylene terephthalate) (PET) fibers. The resulting sorbent has been characterized by Fourier transform infrared (FT‐IR), elemental analysis, thermogravimetric analysis (TGA), FT‐Raman, and scanning electron microscopy (SEM) and studied for the preconcentration and determination of trace Pb (II) ion from human biological fluid and environmental water samples. The optimum pH value for sorption of the metal ion was 8. The sorption capacity of functionalized resin is 44.1 mg g^?1. The chelating sorbent can be reused for 20 cycles of sorption–desorption without any significant change in sorption capacity. A recovery of 100.2% was obtained for the metal ion with 0.5M nitric acid as eluting agent. Effect of grafting yield, shaking time, shape of sorbent, and pH of the medium on adsorption of the metal ion were investigated. Scatchard analysis revealed that the homogeneous binding sites were formed in the polymers. The equilibrium adsorption data of Pb (II) on modified fiber were analyzed by Langmuir, Freundlich, Temkin, and Redlich‐Peterson models. Based on equilibrium adsorption data, the Langmuir, Freundlich, and Temkin constants were determined as 0.236, 10.544, and 9.497 at pH 8 and 20°C, respectively. The method was applied for lead ions determination from human plasma and sea water sample. © 2011 Wiley Periodicals, Inc. J Appl Polym Sci, 2011