Characteristic and mechanism of sorption and desorption of benzene on humic acid

Environmental Science and Pollution Research - The sorption/desorption behaviors of benzene, toluene, ethylbenzene, and xylene (BTEX) on soil organic matter (SOM) have a significant influence on...     

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.     

Mechanism and catalytic performance for direct dimethyl ether synthesis by CO2 hydrogenation over CuZnZr/ferrierite hybrid catalyst

Direct synthesis of dimethyl ether(DME) by CO_2 hydrogenation has been investigated over three hybrid catalysts prepared by different methods:co-precipitation,sol-gel,and solid grinding to produce mixed Cu,ZnO,ZrO_2 catalysts that were physically mixed with a commercial ferrierite(FER) zeolite.The catalysts were characterized by N_2 physisorption,X-ray diffraction(XRD),transmission electron microscopy(TEM),X-ray photoelectron spectroscopy(XPS),temperature programmed desorption of CO_2(CO_2-TPD),temperature programmed desorption of NH_3(NH_3-TPD),and temperature programmed H2 reduction(H_2-TPR).The results demonstrate that smaller CuO and Cu crystallite sizes resulting in better dispersion of the active phases,higher surface area,and lower reduction temperature are all favorable for catalytic activity.The reaction mechanism has been studied using in situ diffuse reflectance infrared Fourier transform spectroscopy(DRIFTS).Methanol appears to be formed via the bidentate-formate(b-HCOO) species undergoing stepwise hydrogenation,while DME formation occurs from methanol dehydration and reaction of two surface methoxy groups.     

Advanced molecular-fingerprinting analysis of dissolved organic sulfur by electrospray ionization-Fourier transform ion cyclotron resonance mass spectrometry using optimal spray solvent

Molecular level characterization of dissolved organic sulfur (DOS) by electrospray ionization-Fourier transform ion cyclotron resonance mass spectrometry (ESI-FTICR MS) is necessary for further understanding of the role of DOS in the environment. Here, ESI spray solvent, a key parameter for ion production during ESI process, was investigated for its effect on the molecular characterization of DOS by ESI-FTICR MS. 100% MeOH as spray solvent was found for the first time to remarkably enhance the ionization efficiency of the majority of CHOS-molecules in NOM, which facilitated a total of 1473 CHOS-molecular formulas with one sulfur atom to be detected. The number of CHOS-molecular formulas obtained using 100%MeOH as spray solvent increased notably over 740 in comparison with those using 50% MeOH aqueous solution (731) or 50% ACN aqueous solution (653). Moreover, due to the enhancement of ionization efficiency of DOS during ESI processes, the tandem mass spectra of the NOM CHOS-molecules could be easily obtained using 100% MeOH as spray solvent, which were hardly obtained using 50% MeOH aqueous solution as spray solvent. The results of the tandem mass spectra suggested the first discovery of organosulfates or sulfonic acids in Suwannee River NOM sample. A simple method based on 100% MeOH as ESI spray solvent for advanced molecular characterization of DOS by ESI-FTICR MS was proposed and applied, and the results revealed more molecular information of DOS in sea DOM samples.     

On-going nitrification in chloraminated drinking water distribution system (DWDS) is conditioned by hydraulics and disinfection strategies

Within the drinking water distribution system (DWDS) using chloramine as disinfectant, nitrification caused by nitrifying bacteria is increasingly becoming a concern as it poses a great challenge for maintaining water quality. To investigate efficient control strategies, operational conditions including hydraulic regimes and disinfectant scenarios were controlled within a flow cell experimental facility. Two test phases were conducted to investigate the effects on the extent of nitrification of three flow rates (Q = 2, 6, and 10 L/min) and four disinfection scenarios (total Cl₂=1 mg/L, Cl₂/NH₃-N=3:1; total Cl₂=1 mg/L, Cl₂/NH₃-N=5:1; total Cl₂=5 mg/L, Cl₂/NH₃-N=3:1; and total Cl₂=5 mg/L, Cl₂/NH₃-N=5:1). Physico-chemical parameters and nitrification indicators were monitored during the tests. The characteristics of biofilm extracellular polymetric substance (EPS) were evaluated after the experiment. The main results from the study indicate that nitrification is affected by hydraulic conditions and the process tends to be severe when the fluid flow transforms from laminar to turbulent (2300<Re<4000). Increasing disinfectant concentration and optimizing Cl₂/NH₃-N mass ratio were found to inhibit nitrification to some extend when the system was running at turbulent condition (Q = 10 L/min, Re = 5535). EPS extracted from biofilm that was established at the flow rate of 6 L/min had greater carbohydrate/protein ratio. Furthermore, several nitrification indicators were evaluated for their prediction efficiency and the results suggest that the change of nitrite, together with total organic carbon (TOC) and turbidity can indicate nitrification potential efficiently.     

京津冀城市群二氧化碳排放达峰研究

基于IPCC排放因子方法建立了2015—2019年京津冀城市群地级城市CO₂排放清单,基于经济增长与CO₂排放关系的脱钩系数法,得到京津冀城市群13个地级以上城市的脱钩情况,结合历史CO₂排放和脱钩情况提出的京津冀城市群达峰判别方法,对京津冀城市群地级以上城市CO₂排放达峰情况进行了判断。结果表明:近5年来,保定、张家口、秦皇岛、邢台、沧州、廊坊、衡水7市碳排放量暂未达到峰值状态;北京、天津、石家庄、承德、邯郸、唐山6个城市已经处于CO₂排放达峰状态。建议已经具备达峰条件的城市抓紧开展达峰行动方案,制定CO₂排放达峰目标。     

Concentrations and chemical compositions of PM10 during hazy and non-hazy days in Beijing

In order to study the concentrations of major components,characteristics and comparison in hazy and non-hazy days of PM_(10) in Beijing,aerosol samples were collected at urban site in Beijing from December 29,2014 to January 22,2015.Heavy metals like Zn,Pb,Mn,Cu,As,V,Cr and Cd were deeply studied considering their toxic effects on human being;nine water-soluble inorganic ions(SO_4~(2-),NO_3~-,NH_4~+,Na~+,K~+,Cl~-,Ca~(2+) and Mg~(2+)) and carbon fractions(OC and EC) were also analyzed.The concentrations of heavy metals were 1.03–1.98 times higher in hazy days than those in non-hazy days,mainly due to biomass burning and coal burning.The trends in total heavy metals concentrations were basically consistent with the trends in PM concentrations except for two obvious periods(12.29–12.30;1.14–1.15);but when air masses accumulated locally or around Beijing,trends in PM concentrations and heavy metals were opposite.The proportion for NO_3~-/SO_4~(2-) indicated that mobile sources such as automobiles were important reasons for haze in Beijing.Correlation between OC and EC during non-hazy days was strong(R~2= 0.95) but it was low(R~2= 0.67) during hazy days,and large variations for OC/EC values occurred in hazy days.The calculated mass concentration of SOC is 2.58 μg/m~3,which only accounted for 10.1% of the OC concentration.When air masses from the far north-west,they decreased PM concentration in Beijing and they were relatively clean;however,those from the near east,south-east and south of the mainland increased PM concentration and they were dirty.     

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.      

典型西南工业城市春冬季PM2.5来源与潜在源区分析——以柳州市为例

为了揭示柳州城区春冬季PM_2.5的来源及其潜在源区分布和贡献,利用2018年24h自动监测数据和气象数据对柳州市大气污染物浓度变化特征进行了分析,并且使用后向轨迹模型（HYSPLIT）对春冬季柳州市PM_2.5逐日72h气流后向轨迹和前向轨迹进行聚类分析,同时结合潜在源贡献因子分析法（WPSCF）和轨迹浓度权重法（WCWT）对其潜在源区和浓度贡献进行了分析.结果显示,（1）在研究期内,不利的主导风向和工业区布局导致研究区PM_2.5在春冬季污染较严重,且工业源和交通源是其主要本地来源;（2）春冬季PM_2.5高值主要来源于西北和东南方向,其中,西北向PM_2.5主要来源于本地排放,且浓度在空间上呈现西高东低的趋势;（3）春季后向轨迹PM_2.5浓度整体大于冬季,春冬季中对柳州市PM_2.5影响最大轨迹均来自东部的短距离输送,而来自西北的气流轨迹输对PM_2.5贡献最低.春冬季柳州市大气PM_2.5通过气流传输对贵州地区大气环境有较大影响;（4）春季,柳州市PM_2.5的主要潜在源区分布在广西东南部、广东中西部、南海沿岸海域、湖南中部、江西西北部、湖北东部及安徽西北部;冬季,主要分布在广西东南部、广东西南部和南海沿岸海域.