Tuning the fill percentage in the hydrothermal synthesis process to increase catalyst performance for ozone decomposition

The performance of Ce-OMS-2 catalysts was improved by tuning the fill percentage in the hydrothermal synthesis process to increase the oxygen vacancy density. The Ce-OMS-2 samples were prepared with different fill percentages by means of a hydrothermal approach (i.e. 80%, 70%, 50% and 30%). Ce-OMS-2 with 80% fill percentage (Ce-OMS-2-80%) showed ozone conversion of 97%, and a lifetime experiment carried out for more than 20?days showed that the activity of the catalyst still remained satisfactorily high (91%). For Ce-OMS-2-80%, Mn ions in the framework as well as K ions in the tunnel sites were replaced by Ce⁴⁺, while for the others only Mn ions were replaced. O₂-TPD and H₂-TPR measurements proved that the Ce-OMS-2-80% catalyst possessed the greatest number of mobile surface oxygen species. XPS and XAFS showed that increasing the fill percentage can reduce the AOS of Mn and augment the amount of oxygen vacancies. The active sites, which accelerate the elimination of O₃, can be enriched by increasing the oxygen vacancies. These findings indicate that increasing ozone removal can be achieved by tuning the fill percentage in the hydrothermal synthesis process.     

Phosphate recovery with granular acid-activated neutralized red mud: Fixed-bed column performance and breakthrough curve modelling

Granular acid-activated neutralized red mud (AaN-RM) has been successfully prepared with good chemical stability and physical strength. However, its potential for industrial application remains unknown. Therefore, the performance of granular AaN-RM for phosphate recovery in a fixed-bed column was investigated. The results demonstrated that the phosphate adsorption performance of granular AaN-RM in a fixed-bed column was affected by various operational parameters, such as the bed depth, flow rate, initial solution pH and initial phosphate concentration. With the optimal empty-bed contact time (EBCT) of 24.27 min, the number of processed bed volumes and the phosphate adsorption capacity reached 496.95 and 84.80 mg/g, respectively. Then, the saturated fixed-bed column could be effectively regenerated with a 0.5 mol/L HCl solution. The desorption efficiency remained as high as 83.45% with a low weight loss of 3.57% in the fifth regeneration cycle. In addition, breakthrough curve modelling showed that a 5-9-1 feed-forward artificial neural network (ANN) could be effectively applied for the optimization of the fixed-bed adsorption system; the coefficient of determination (R²) and the root mean square error (RMSE) evaluated on the validation-testing data were 0.9987 and 0.0183, respectively. Therefore, granular AaN-RM fixed-bed adsorption exhibits promising potential for phosphate removal and recovery from polluted water.     

Effects of SO2 and H2O on low-temperature NO conversion over F-V2O5-WO3/TiO2 catalysts

F-V_2 O_5-WO3/Ti02 catalysts were prepared by the impregnation method.As the content of F ions increased from 0.00 to 0.35 wt.%,the NO conversion of F-V_2 O_5-WO_3/TiO_2 catalysts initially increased and then decreased.The 0.2 F-V_2 O_5-WO_3/TiO_2 catalyst(0.2 wt.% F ion)exhibited the best denitration(De-NOx) performance,with more than 95% NO conversion in the temperature range 160-360℃,and 99.0% N2 selectivity between 110 and 280℃.The addition of an appropriate amount of F ions eroded the surface morphology of the catalyst and reduced its grain size,thus enhancing the NO conversion at low temperature as well as the sulfur and water resistance of the V_2 O_5-WO3/Ti02 catalyst.After selective catalytic reduction(SCR) reaction in a gas flow containing SO_2 and H_2 O,the number of NH3 adsorption sites,active component content,specific surface area and pore volume decreased to different degrees.Ammonium sulfate species deposited on the catalyst surface,which blocked part of the active sites and reduced the NO conversion performance of the catalyst.On-line thermal regeneration could not completely recover the catalyst activity,although it prolonged the cumulative life of the catalyst.In addition,a mechanism for the effects of S02 and H_2 O on catalyst NO conversion was proposed.     

Development of a static test apparatus for evaluating the performance of three PM2.5 separators commonly used in China

PM_(2.5) separator directly affects the accuracy of PM_(2.5) sampling.The specification testing and evaluation for PM_(2.5) separator is particularly important,especially under China's wide variation of terrain and climate.In this study,first a static test apparatus based on polydisperse aerosol was established and calibrated to evaluate the performance of the PM_(2.5) separators.A uniform mixing chamber was developed to make particles mix completely.The aerosol concentration relative standard deviations of three test points at the same horizontal chamber position were less than 0.57%,and the particle size distribution obeyed logarithmic normal distribution with an R~2 of 0.996.The flow rate deviation between the measurement and the set point flow rate agreed to within ± 1.0% in the range of -40 to 50℃.Secondly,the separation,flow and loading characteristics of three cyclone separators(VSCC-A,SCC-A and SCC112) were evaluated using this system.The results showed that the 50% cutoff sizes(D_(50)) of the three cyclones were 2.48,2.47 and 2.44 μm when worked at the manufacturer's recommended flow rates,respectively.The geometric standard deviation(GSD) of the capture efficiency of VSCCA was 1.23,showed a slightly sharper than SCC-A(GSD = 1.27),while the SCC112 did not meet the relevant indicator(GSD = 1.2 ± 0.1) with a GSD = 1.44.The flow rate and loading test had a great effect on D_(50),while the GSD remained almost the same as before.In addition,the maintenance frequency under different air pollution conditions of the cyclones was summarized according to the loading test.     

An investigation of changes in water quality throughout the drinking water production/distribution chain using toxicological and fluorescence analyses

Changes in water quality from source water to finished water and tap water at two conventional drinking water treatment plants(DWTPs) were monitored.Beside the routine water quality testing,Caenorhabditis elegans-based toxicity assays and the fluorescence excitation–emission matrices technique were also applied.Both DWTPs supplied drinking water that met government standards.Under current test conditions,both the investigated finished water and tap water samples exhibited stronger lethal,genotoxic and reprotoxic potential than the relative source water sample,and the tap water sample was more lethal but tended to be less genotoxic than the corresponding finished water sample.Meanwhile,the nearly complete removal of tryptophan-like substances and newly generated tyrosine-like substances were observed after the treatment of drinking water,and humic-like substances were identified in the tap water.Based on these findings,toxic pollutants,including genotoxic/reproductive toxicants,are produced in the drinking water treatment and/or distribution processes.Moreover,further studies are needed to clarify the potentially important roles of tyrosine-like and humic-like substances in mediating drinking water toxicity and to identify the potential sources of these contaminants.Additionally,tryptophan-like fluorescence may be adopted as a useful parameter to monitor the treatment performance of DWTPs.Our observations provided insights into the importance of utilizing biotoxicity assays and fluorescence spectroscopy as tools to complement the routine evaluation of drinking water.     

Recent advances in catalytic decomposition of ozone

Ozone (O₃), as a harmful air pollutant, has been of wide concern. Safe, efficient, and economical O₃ removal methods urgently need to be developed. Catalytic decomposition is the most promising method for O₃ removal, especially at room temperature or even subzero temperatures. Great efforts have been made to develop high-efficiency catalysts for O₃ decomposition that can operate at low temperatures, high space velocity and high humidity. First, this review describes the general reaction mechanism of O₃ decomposition on noble metal and transition metal oxide catalysts. Then, progress on the O₃ decomposition performance of various catalysts in the past 30 years is summarized in detail. The main focus is the O₃ decomposition performance of manganese oxides, which are divided into supported manganese oxides and non-supported manganese oxides. Methods to improve the activity, stability, and humidity resistance of manganese oxide catalysts for O₃ decomposition are also summarized. The deactivation mechanisms of manganese oxides under dry and humid conditions are discussed. The O₃ decomposition performance of monolithic catalysts is also summarized from the perspective of industrial applications. Finally, the future development directions and prospects of O₃ catalytic decomposition technology are put forward.     

Effects of calcination temperature on physicochemical property and activity of CuSO4/TiO2 ammonia-selective catalytic reduction catalysts

CuSO_4/TiO_2 catalysts with high catalytic activity and excellent resistant to SO_2 and H_2 O,were thought to be promising catalysts used in Selective catalytic reduction of nitrogen oxides by NH_3.The performance of catalysts is largely affected by calcination temperature.Here,effects of calcination temperature on physicochemical property and catalytic activity of CuSO_4/TiO_2 catalysts were investigated in depth.Catalyst samples calcined at different temperatures were prepared first and then physicochemical properties of the catalyst were characterized by N2 adsorption-desorption,X-ray diffraction,thermogravimetric analysis,Raman spectra,Fourier-transform infrared spectroscopy,X-ray photoelectron spectroscopy,temperature-pro grammed desorption of NH_3,temperature-programmed reduction of H_2 and in situ diffuse reflectance infrared Fourier transform spectroscopy.Results revealed that high calcination temperature had three main effects on the catalyst.First,sintering and anatase transform into rutile with increase of calcination temperature,causing a decrement of specific surface area.Second,decomposition of CuSO_4 under higher calcination temperature,resulting in disappears of Br(?)nsted acid sites(S-OH),which had an adverse effect on surface acidity.Third,CuO from the decomposition of CuSO_4 changed surface reducibility of the catalyst and favored the process of NH_3 oxidation to nitrogen oxides(NO_x).Thus,catalytic activity of the catalyst calcined under high temperatures(≥600℃) decreased largely.     

Synergistic effects of Cu species and acidity of Cu-ZSM-5 on catalytic performance for selective catalytic oxidation of n-butylamine

In this work, a series of Cu-ZSM-5 catalysts with different SiO₂/Al₂O₃ ratios (25, 50, 100 and 200) were synthesized and investigated in n-butylamine catalytic degradation. The n-butylamine can be completely catalytic degradation at 350°C over all Cu-ZSM-5 catalysts. Moreover, Cu-ZSM-5 (25) exhibited the highest selectivity to N₂, exceeding 90% at 350°C. These samples were investigated in detail by several characterizations to illuminate the dependence of the catalytic performance on redox properties, Cu species, and acidity. The characterization results proved that the redox properties and chemisorption oxygen primarily affect n-butylamine conversion. N₂ selectivity was impacted by the Brønsted acidity and the isolated Cu²⁺ species. Meanwhile, the surface acid sites over Cu-ZSM-5 catalysts could influence the formation of Cu species. Furthermore, in situ diffuse reflectance infrared Fourier transform spectra was adopted to explore the reaction mechanism. The Cu-ZSM-5 catalysts are the most prospective catalysts for nitrogen-containing volatile organic compounds removal, and the results in this study could provide new insights into catalysts design for VOC catalytic oxidation.     

UV/H2O2 oxidation of tri(2-chloroethyl) phosphate: Intermediate products, degradation pathway and toxicity evaluation

Tri(2-chloroethyl) phosphate (TCEP) with the initial concentration of 5 mg/L was degraded by UV/H₂O₂ oxidation process. The removal rate of TCEP in the UV/H₂O₂ system was 89.1% with the production of Cl^? and PO₄^3? of 0.23 and 0.64 mg/L. The removal rate of total organic carbon of the reaction was 48.8% and the pH reached 3.3 after the reaction. The oxidative degradation process of TCEP in the UV/H₂O₂ system obeyed the first order kinetic reaction with the apparent rate constant of 0.0025 min^?1 (R²=0.9788). The intermediate products were isolated and identified by gas chromatography-mass spectrometer. The addition reaction of HO? and H₂O and the oxidation reaction with H₂O₂ were found during the degradation pathway of 5 mg/L TCEP in the UV/H₂O₂ system. For the first time, environment risk was estimated via the “ecological structure activity relationships” program and acute and chronic toxicity changes of intermediate products were pointed out. The luminescence inhibition rate of photobacterium was used to evaluate the acute toxicity of intermediate products. The results showed that the toxicity of the intermediate products increased with the increase of reaction time, which may be due to the production of chlorine compounds. Some measures should be introduced to the UV/H₂O₂ system to remove the highly toxic Cl-containing compounds, such as a nanofiltration or reverse osmosis unit.     

达里诺尔湖水体DOM荧光特征及其来源解析

达里诺尔湖（简称“达里湖”）是内蒙古自治区高原地区重要的生态屏障,探究达里湖水质状况及污染来源,对加强流域水环境治理、改善水环境质量具有十分重要的意义.于2018年9月及2019年6月对湖水进行采样,并通过三维荧光光谱结合PARAFAC（平行因子分析）模型,探究达里湖水体DOM（溶解性有机质）来源及其与水质的关系.结果表明:①达里湖水体中pH较高,ρ（DOC）（DOC为溶解性有机碳）、ρ（NH₄+-N）、ρ（TP）相对较高,均超过GB 3838—2002《地表水环境质量标准》Ⅴ类水质标准限值.②水体中DOM含4种荧光组分.夏季水体DOM主要分布于河流入湖口附近,其中,类腐殖质荧光组分（紫外区类富里酸和可见区类富里酸）占总组分的62.93%,类蛋白类荧光组分（类色氨酸和类酪氨酸）占总组分的36.07%;秋季水体DOM主要分布于东南侧,其中,类腐殖质荧光组分占总组分的40.52%,类蛋白类荧光组分占总组分的59.48%.③达里湖采样点荧光参数表明,达里湖DOM自生源特征较强,腐殖化程度较低.类腐殖质荧光组分与ρ（DOC）、ρ（Chla）均呈正相关,类色氨酸荧光组分与pH呈正相关,类络氨酸与ρ（DTN）、ρ（NH4+-N）、ρ（DTP）均呈正相关.研究显示,达里湖DOM具有陆源与生物源双重特性,DOM的形成与微生物、细菌、浮游生物的生命活动密切相关.