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.     

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。     

关于在长江经济带布局以水质改善为目标的流域生态缓冲体系的思考

生态缓冲带能够有效减缓流域内的人类活动或自然过程对水环境和水生态系统的影响.在长江经济带构建流域生态缓冲体系,对长江生态保护修复具有十分重要的意义.讨论了构建流域生态缓冲体系涉及的生态缓冲带位置选择、缓冲体系所占最低面积比率、宽度划定等一些基本的原则要求;利用卫星遥感影像数据,提取各汇水单元的地形特征、土地利用类型特征、土壤类型、土壤侵蚀强度、水文水系等数据,对长江经济带流域生态缓冲体系进行布局.结果表明:①长江经济带内林草地是主要土地利用类型,占区域总面积的62.46%,但是分布很不均匀,主要集中在西部高地和中下游的丘陵地带,在人口密集、农田密集的区域分布偏少;城镇用地主要集中在长江中下游地区.②土壤类型空间差异显著,浙江省、江苏省、湖南省、江西省及安徽省大部分区域的土壤多是黏性比较大,污染物迁移能力较低;而污染物迁移能力较强的砂质土或者土层较薄的山地草甸土主要分布在四川省北部、西北部.水力侵蚀、风力侵蚀和冻融侵蚀均有分布,且以水力侵蚀为主,建议在中度及以上侵蚀强度区域尽量减少污染源,重点布置缓冲带,增加该区域的缓冲力度.③长江经济带范围内可以利用的中小型湿地、小型河流支浜的面积至少有1.4×104 km2,再结合林草缓冲带,就可以形成一个生态缓冲体系.④在土地利用类型分布结果基础上,叠加土壤侵蚀强度和水系分布,将污染源区、中度及以上侵蚀强度区、水体区作为缓冲对象,建立缓冲体系的重点区域,总面积约14.26×104 km2,占长江经济带总面积的6.95%.对照欧美地区的研究,6.95%的缓冲体系面积占比是偏低的,需要在长江经济带开展深入研究来确定适宜的缓冲体系面积比,推进长江经济带流域生态缓冲体系的构建.      

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%.     

沈阳市郊区环境空气中醛酮类化合物的污染特征与来源分析

为探究沈阳市郊区环境空气中醛酮类化合物的污染特征,于2017年8月24日—9月2日采用2,4-二硝基苯肼固相吸附/高效液相色谱方法对沈阳市郊区醛酮类化合物进行观测分析,利用美国环境保护局推荐的人体健康风险评价方法对部分有毒有害醛酮类化合物的人体健康风险进行了评价,并利用比值法对醛酮类化合物的来源进行了初步分析.结果表明:醛酮类化合物质量浓度日均值范围为23.16~38.38 μg/m3;质量浓度最高的4种醛酮类化合物依次是丙酮、甲醛、正丁醛和乙醛,其质量浓度日均值的平均值分别为8.71、5.90、5.48和2.95 μg/m3.对·OH消耗速率(L_OH)贡献较大的醛酮类化合物物种是正丁醛、甲醛和乙醛,臭氧生成潜势贡献(OFP)较大的醛酮类化合物物种是甲醛、正丁醛和乙醛,在研究区影响醛酮类化合物光化学反应活性的物种主要是甲醛、乙醛和正丁醛.研究区观测期间,环境空气中甲醛和乙醛的致癌性风险值分别为1.18×10-5和5.91×10-6,对暴露人群存在潜在的致癌风险;乙醛的非致癌风险值为0.05,对暴露人群不存在非致癌风险.在研究区的一次臭氧轻度污染过程期间,环境空气中的甲醛和乙醛受天然源排放的挥发性有机物二次转化的影响减弱,甲醛、乙醛和丙酮受到炼焦工业和机动车等人为源排放的影响增强,而正丁醛主要受当地精细化工产业排放的影响.研究显示,沈阳市应加大对炼焦工业、精细化工和机动车来源排放醛酮类化合物的管制,以降低环境空气中活性醛酮类化合物及有毒有害醛酮类化合物的浓度.