Density functional theory (DFT) studies of vanadium-titanium based selective catalytic reduction (SCR) catalysts

Based on density functional theory (DFT) and basic structure models, the chemical reactions on the surface of vanadium-titanium based selective catalytic reduction (SCR) denitrification catalysts were summarized. Reasonable structural models (non-periodic and periodic structural models) are the basis of density functional calculations. A periodic structure model was more appropriate to represent the catalyst surface, and its theoretical calculation results were more comparable with the experimental results than a non-periodic model. It is generally believed that the SCR mechanism where NH₃ and NO react to produce N₂ and H₂O follows an Eley-Rideal type mechanism. NH₂NO was found to be an important intermediate in the SCR reaction, with multiple production routes. Simultaneously, the effects of H₂O, SO₂ and metal on SCR catalysts were also summarized.     

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.     

Chemical characteristics of road dust PM2.5 fraction in oasis cities at the margin of Tarim Basin

In order to understand the compositions characteristics of particulate matter with aerodynamic diameter less than 2.5 μm (PM_2.5) fraction in road dust (RD_2.5) of oasis cities on the edge of Tarim Basin, 30 road dust (RD) samples were collected in Kashi, Cele, and Yutian in the spring, 2018, and RD_2.5 was collected using the resuspension approach. Eight water-soluble ions, 39 trace elements and 8 fractions of carbon-containing species in PM_2.5 were analyzed. Ca²⁺ and Ca were the most abundant ions and elements in RD_2.5 (7.1% and 9.5%). Cl^- in RD_2.5 was affected not only by attributed to saline-alkali soils in oasis cities of the Tarim Basin and dust from Taklimakan Desert but also by human activities. Moreover, the organic carbon/elemental carbon (OC/EC) ratio indicated that carbon components in RD_2.5 in Cele town mainly come from fossil fuel combustion, while those in Yutian and Kashi mainly come from biomass combustion. It is noteworthy that high Ca in RD_2.5 was seriously affected by anthropogenic emissions, and high Na and K contents in RD_2.5 could be derived from soil and desert dust. It was estimated that Cd, Tl, Sn and Cr were emitted from anthropogenic emissions using the enrichment factor. The coefficients of divergence (COD) result indicated that the influence of local emission on road dust emission is greater than that of long-distance transmission. This study is the first time to comprehensively analyze the chemical characteristics of road dust in oasis cities, and the results provides the sources of road dust at the margin of Tarim Basin.     

Polycyclic aromatic hydrocarbons in benthos of the northern Bering Sea Shelf and Chukchi Sea Shelf

Eighteen polycyclic aromatic hydrocarbons (PAHs) were detected in benthos collected onboard the ‘Snow Dragon’ in the Northern Bering Sea Shelf and Chukchi Sea Shelf during the 6^th Chinese National Arctic Research Expedition (CHINARE 2014). Σ₁₈PAHs for all biota samples ranged from 34.2 to 128.1 ng/g dry weight (dw), with the highest concentration observed in fish muscle (Boreogadus saida) samples close to St. Lawrence Island. The PAH composition pattern was dominated by the presence of lighter 3 ring (57%) and 2 ring (28%) PAHs, indicating oil-related or petrogenic sources as important origins of PAH contamination. Concentrations of alkyl-PAHs (1-methylnaphthalene and 2-methylnaphthalene) were lower than their parent PAH (naphthalene) in all biological tissue, and their percentage also decreased significantly (p<0.05) compared with those in the corresponding sediment. There were no significant relationships between PAH concentrations and trophic levels, which is possibly due to the combined results of the complex benthic foodweb in the subarctic/Arctic shelf region, as well as a low assimilation/effective metabolism for PAHs. According to toxic potency evaluation results from TCDD toxic equivalents (TEQs) and BaP-equivalent (BaPE) values, whelk (Neptunea heros) and starfish (Ctenodiscus crispatus) are two macroinvertebrate species showing relatively higher dioxin-like toxicity and carcinogenic risk.     

Analytical methods and environmental processes of nanoplastics

The degradation of plastic debris may result in the generation of nanoplastics (NPs). Their high specific surface area for the sorption of organic pollutions and toxic heavy metals and possible transfer between organisms at different nutrient levels make the study of NPs an urgent priority. However, there is very limited understanding on the occurrence, distribution, abundant, and fate of NPs in the environment, partially due to the lack of suitable techniques for the separation and identification of NPs from complex environmental matrices. In this review, we first overviewed the state-of-the-art methods for the extraction, separation, identification and quantification of NPs in the environment. Some of them have been successfully applied for the field determination of NPs, while some are borrowed from the detection of microplastics or engineered nanomaterials. Then the possible fate and transport of NPs in the environment are thoroughly described. Although great efforts have been made during the recent years, large knowledge gaps still exist, such as the relatively high detection limit of existing method failing to detect ultralow masses of NPs in the environment, and spherical polystyrene NP models failing to represent the various compositions of NPs with different irregular shapes, which needs further investigation.     

日本城市有机废弃物甲烷发酵资源化系统案例分析及最新研究进展

为建设可持续发展社会,日本近年来大力推动甲烷发酵以实现城市有机废弃物的减量化和资源化。首先介绍了日本城市有机废弃物资源化的2个实用案例,长冈市厨余垃圾沼气发电中心和丰桥市生物质资源利用中心的设计和运营状况。两者的长期稳定运行及产能效果验证了甲烷发酵技术在城市有机废弃物减量化和资源化上的可行性。其次,为了应对社会发展趋势和城市有机废弃物处理的技术需求,介绍了日本有关厨余垃圾、污泥以及废纸（城市有机废弃物的3大组分）的单独发酵及共发酵的部分研究成果。此外,简要介绍了应用厌氧膜生物反应器（AnMBR）进行相关高效甲烷发酵的最新研究成果。并根据实用案例调查和实验研究结果,以100万人口城市为例,对城市有机废弃物的各种甲烷发酵系统的产能效果进行了模拟概算。     

洞庭湖区南汉垸水体浮游植物群落结构特征及其影响因素

环境要素的变化对浮游植物的群落结构和功能具有重要影响.为揭示洞庭湖南汉垸湖区浮游植物群落结构特征及其影响因素,分别于2017年11月（关泵封水期）和2018年6月（开泵放水期）在洞庭湖区典型堤垸——南汉垸进行了采样调查,并对调查区域内的浮游植物及主要水环境因子进行了系统监测和分析.结果表明:①调查期间共检出浮游植物8门62属,主要隶属于绿藻门（Chlorophyta）、硅藻门（Bacillariophyta）和蓝藻门（Cyanophyta）,浮游植物分布表现出较为显著的时间差异性,11月浮游植物的丰度为8.34×106~3.02×108 L-1,6月为1.13×106~2.04×107 L-1.②Shannon-Wiener多样性指数（H'）介于1.10~3.24之间,Margalef丰富度指数（d）介于1.42~6.40之间,Pielou均匀度指数（J）介于0.48~0.87之间,多样性评价表明,南汉垸整体上介于轻污染与β-中污染之间,局部采样点为α-中污染.③PCA（主成分分析）结果表明,ρ（TN）、ρ（TP）和ρ（NH₄+-N）为南汉垸水体的主要污染因子.④RDA（冗余分析）结果表明,南汉垸浮游植物群落结构分布与pH、ρ（NH₄+-N）及ρ（TN）呈正相关,与WT（水温）呈负相关.研究显示,南汉垸水体介于轻污染与β-中污染之间,营养状态及浮游植物群落结构在时间上差异较大.      

基于土壤重金属特征的绿色食品产地环境评价——以重庆(江津)现代农业园区为例

以重庆市江津区现代农业园区内4种农用地类型的653个表层土样为研究对象,测定土壤重金属元素含量.依据绿色食品产地环境相关标准,采用重金属污染指数法对标准中所涉及的Cu、Cr、Cd、Hg、As和Pb共6种重金属元素开展土壤环境质量评价和潜在生态风险评价,并结合用地类型确定绿色农产品生产的适宜性土壤分区.结果表明：除元素Cu、Cr和As外,其他元素的平均含量均高于重庆市土壤背景值;除元素As和Hg外,其他元素的平均含量均高于我国土壤背景值.土壤重金属元素Cu、Cr、Cd、Hg、As和Pb的平均浓度均达到《绿色食品产地环境质量》标准要求,但Cd污染已处于安全警戒线内,应高度警惕和严格监管园区内该元素的污染.水田、旱地和果园的土壤环境均以尚清洁为主,其他园地的土壤环境以轻度污染水平为主.部分水田存在一定程度的Pb污染（轻度）、Hg污染（中度）和Cd污染（中度）,旱地存在一定程度的Hg污染（中度）和Cd污染（中度）,果园和其他园地的土壤存在一定程度的Cd的轻、中度污染.全区符合《绿色食品产地环境质量》标准要求的土壤面积为12.47km²,占农用地总面积的63.64%,旱地、果园、水田和其他园地中符合该标准的面积分别占各自总面积的84.83%、68.07%、56.51%和42.09%.4种用地类型的土壤环境生态风险水平均以低等为主,共占研究区总面积的74.70%.Cd和Hg在园区表层土壤重金属生态风险评估中占有较大的贡献率,应列为优先控制污染元素并对其生态效应开展进一步研究.     

CeO2形貌结构对催化湿式空气氧化苯酚性能的影响

采用水热法、沉淀法和溶胶凝胶法制备了3种不同形貌的CeO₂催化材料,并将其用于湿式空气氧化苯酚水溶液过程中,探讨了CeO₂形貌结构对催化湿式氧化苯酚水溶液性能的影响.采用扫描电子显微镜（SEM）、透射电子显微镜（TEM）、X射线衍射（XRD）、程序升温还原（TPR）等手段对CeO₂催化材料进行了表征.结果表明,水热法制备的CeO₂催化材料表现出较好催化性能,主要原因是水热法合成的CeO₂呈现交错的纳米棒状结构,主要暴露（220）晶面,且沿着（220）晶向生长.在反应温度为200℃、空气压力为2MPa、苯酚初始浓度500mg/L的条件下,最终（240min）COD的去除率为95.5%.