MgO低温催化臭氧降解氨氮的机制研究

研究了低温条件下单独臭氧及MgO催化臭氧化降解水中氨氮的效率和特征,并对其反应机制分别进行了探讨.结果表明,pH是影响臭氧和催化臭氧化除氨的重要因素,不仅影响溶液中NH_3与NH~+_4的比例和臭氧氧化氨氮的速率,还影响氧化产物种类,从而影响脱氮效果.10℃时,单独臭氧对水中氨氮的氧化降解效率随pH的升高而增大,pH≤9时整体降解效率不高,pH=9时仅为16.39%,而pH=10时达到41.77%.臭氧和·OH共同参与降解氨氮的过程.单独臭氧氧化氨氮生成氮气的选择性具有pH依赖性,并与Cl~-密切相关.pH低(≤9)时,氨氮多以NH~+_4形态存在,O_3与Cl~-反应生成ClO~-_x(x=1、3),再氧化NH~+_4,从而生成气态产物N_2或N_2O.MgO在低温条件下具有很强的催化臭氧化降解氨氮的能力且温度升高有利于反应的进行,0、10、20℃时,MgO催化臭氧化氨氮的效率分别为77.53%、80.17%、91.26%.此过程中,·OH参与反应的程度低,一部分氨氮降解依靠ClO~-_x氧化NH~+_4,而氨氮降解的主要途径为O_3对NH_3的直接氧化.     

深圳市综合水质指数研究及其在水资源资产评估上的应用

自然资源资产评估技术是开展自然资源资产负债表实践和实行环境责任离任审计的重要技术支撑。水资源作为一项重要自然资源,如何有效评估水资源资产是不可回避的问题。论文以深圳市为研究区域,一是采用综合污染指数法和主成分分析法,以总氮、氨氮、总磷、化学需氧量、生化需氧量、固体悬浮物为指标参数构建了深圳市综合水质指数以评价水资源综合水质。二是以该综合水质评估模型为基础,通过采用治污成本法分析综合水质与治污成本间的关系,从而构建深圳市景观水和饮用水资源的价值量评估模型。论文还以深圳市大鹏新区为试点开展了水资源价值量评估,评估结果显示,2015年大鹏新区景观水和饮用水资源的价值量分别为3.60亿、0.35亿元。     

Potential of secondary aerosol formation from Chinese gasoline engine exhaust

Light-duty gasoline vehicles have drawn public attention in China due to their significant primary emissions of particulate matter and volatile organic compounds(VOCs). However,little information on secondary aerosol formation from exhaust for Chinese vehicles and fuel conditions is available. In this study, chamber experiments were conducted to quantify the potential of secondary aerosol formation from the exhaust of a port fuel injection gasoline engine. The engine and fuel used are common in the Chinese market, and the fuel satisfies the China V gasoline fuel standard. Substantial secondary aerosol formation was observed during a 4–5 hr simulation, which was estimated to represent more than 10 days of equivalent atmospheric photo-oxidation in Beijing. As a consequence, the extreme case secondary organic aerosol(SOA) production was 426 ± 85 mg/kg-fuel, with high levels of precursors and OH exposure. The low hygroscopicity of the aerosols formed inside the chamber suggests that SOA was the dominant chemical composition. Fourteen percent of SOA measured in the chamber experiments could be explained through the oxidation of speciated single-ring aromatics. Unspeciated precursors, such as intermediate-volatility organic compounds and semi-volatile organic compounds, might be significant for SOA formation from gasoline VOCs. We concluded that reductions of emissions of aerosol precursor gases from vehicles are essential to mediate pollution in China.     

Mercury flows in large-scale gold production and implications for Hg pollution control

Large-scale gold production(LSGP) is one of the five convention-related atmospheric mercury(Hg) emission sources in the Minamata Convention on Mercury. However, field experiments on Hg flows of the whole process of LSGP are limited. To identify the atmospheric Hg emission points and understand Hg emission characteristics of LSGP, Hg flows in two gold smelters were studied. Overall atmospheric Hg emissions accounted for 10%–17% of total Hg outputs and the Hg emission factors for all processes were 7.6–9.6 kg/ton. There were three dominant atmospheric Hg emission points in the studied gold smelters, including the exhaust gas of the roasting process, exhaust gas from the environmental fog collection stack and exhaust gas from the converter of the refining process. Atmospheric Hg emissions from the roasting process only accounted for 16%–29% of total emissions and the rest were emitted from the refining process. The overall Hg speciation profile(gaseous elemental Hg/gaseous oxidized Hg/particulate-bound Hg) for LSGP was 34.1/57.1/8.8. The dominant Hg output byproducts included waste acid, sulfuric acid and cyanide leaching residue. Total Hg outputs from these three byproducts were 80% in smelter A and 84% in smelter B. Our study indicated that previous atmospheric Hg emissions from large-scale gold production might have been overestimated.Hg emission control in LSGP is not especially urgent in China compared to other significant emission sources(e.g., cement plants). Instead, LSGP is a potential Hg release source due to the high Hg output proportions to acid and sludge.     

Effects of Na+ on Cu/SAPO-34 for ammonia selective catalytic reduction

Copper-exchanged chabazite (Cu/CHA) catalysts have been found to be affected by alkali metal and alkaline earth ions. However, the effects of Na⁺ ions on Cu/SAPO-34 for ammonia selective catalytic reduction (NH₃-SCR) are still unclear. In order to investigate the mechanism, five samples with various Na contents were synthesized and characterized. It was observed that the introduced Na⁺ ion-exchanges with H⁺ and Cu^2 + of Cu/SAPO-34. The exchange of H⁺ is easier than that of isolated Cu^2 +. The exchanged Cu^2 + ions aggregate and form “CuAl₂O₄-like” species. The NH₃-SCR activity of Cu/SAPO-34 decreases with increasing Na content, and the loss of isolated Cu^2 + and acid sites is responsible for the activity loss.     

Seasonal variation and size distribution of biogenic secondary organic aerosols at urban and continental background sites of China

Size-resolved biogenic secondary organic aerosols(BSOA) derived from isoprene and monoterpene photooxidation in Qinghai Lake, Tibetan Plateau(a continental background site) and five cities of China were measured using gas chromatography/mass spectrometry(GC/MS). Concentrations of the determined BSOA are higher in the cities than in the background and are also higher in summer than in winter. Moreover, strong positive correlations(R2= 0.44–0.90) between BSOA and sulfate were found at the six sites,suggesting that anthropogenic pollution(i.e., sulfate) could enhance SOA formation,because sulfate provides a surface favorable for acid-catalyzed formation of BSOA. Size distribution measurements showed that most of the determined SOA tracers are enriched in the fine mode( 3.3 μm) except for cis-pinic and cis-pinonic acids, both presented a comparable mass in the fine and coarse( 3.3 μm) modes, respectively. Mass ratio of oxidation products derived from isoprene to those from monoterpene in the five urban regions during summer are much less than those in Qinghai Lake region. In addition, in the five urban regions relative abundances of monoterpene oxidation products to SOA are much higher than those of isoprene. Such phenomena suggest that BSOA derived from monoterpenes are more abundant than those from isoprene in Chinese urban areas.     

Regionalization based on spatial and seasonal variation in ground-level ozone concentrations across China

Owing to the vast territory of China and strong regional characteristic of ozone pollution,it's desirable for policy makers to have a targeted and prioritized regulation and ozone pollution control strategy in China based on scientific evidences. It's important to assess its current pollution status as well as spatial and temporal variation patterns across China.Recent advances of national monitoring networks provide an opportunity to insight the actions of ozone pollution. Here, we present rotated empirical orthogonal function(REOF)analysis that was used on studying the spatiotemporal characteristics of daily ozone concentrations. Based on results of REOF analysis in pollution seasons for 3 years' observations, twelve regions with clear patterns were identified in China. The patterns of temporal variation of ozone in each region were separated well and different from each other, reflecting local meteorological, photochemical or pollution features. A rising trend in annual averaged Eight-hour Average Ozone Concentrations(O_3-8 hr) from 2014 to 2016 was observed for all regions, except for the Tibetan Plateau. The mean values of annual and 90 percentile concentrations for all 338 cities were 82.6 ± 14.6 and 133.9 ± 25.8 μg/m~3,respectively, in 2015. The regionalization results of ozone were found to be influenced greatly by terrain features, indicating significant terrain and landform effects on ozone spatial correlations. Among 12 regions, North China Plain, Huanghuai Plain, Central Yangtze River Plain, Pearl River Delta and Sichuan Basin were realized as priority regions for mitigation strategies, due to their higher ozone concentrations and dense population.     

一种模拟动力学边界条件的环境振动试验方法研究

目的提高环境振动试验的可靠性。方法以某典型钛合金蜂窝夹芯壁板试验件为例,提出一种模拟试验件动力学边界条件的试验方法,在试验件周围引入弹性连接件,再通过刚性转接工装与振动台台面连接,以试验件在试验安装状态下的共振频率及振型节线位置为优化目标,以弹性连接件的外形尺寸及厚度为优化变量,对弹性连接件进行优化设计,从而模拟试验件真实的动力学边界条件。结果弹性连接件的优化设计使得试验件在试验安装状态下前两阶共振频率与试验要求相差小于8%,而且振型节线位置与试验要求基本重合,达到了模拟试验件真实动力学边界条件的设计目标。结论对于壁板类试验件,在传统刚性夹具的基础上引入弹性连接件的试验方法,可以较好地模拟试验件真实动力学边界条件,提高环境振动试验的可靠性,并且这种方法对试验费用及试验周期影响较小,具有良好的工程应用前景。     

聚丙烯酰胺降解菌株的分离及其油田含聚污水生物强化处理研究

应用厌氧Hungate技术,从大庆油田分离到一株聚丙烯酰胺降解菌株,菌株与Clostridium bifermentans(AY781385)相似性为99%,命名为Clostridium bifermentans H5。菌株能以聚丙烯酰胺为唯一碳源,静态试验表明,在附加乳酸钠和硫酸钠的条件下,聚合物去除率为52.5%;首次采用纯菌培养的厌氧污泥作为底物,水解酸化试验表明,乳酸钠作为碳源要好于砂糖,聚合物去除率为50.89%左右,砂糖为碳源聚合物去除率为43.55%左右;初步试验表明,应用高效降解菌株和水解酸化工艺处理含聚污水具有可行性。     

同槽双极锰电积生产工艺的现状及进展研究

为解决传统锰和二氧化锰制备过程中单独电解的高能耗、高污染问题,目前国内外在同槽电解制备金属锰和微粒二氧化锰方面已有一定的探索和研究。总结介绍了锰和二氧化锰的研究进展,电解液的制备方法、电极的制备研究以及最新同槽电解工艺的研究动态和发展,并在此基础上展望了电解制备锰和二氧化锰工业的发展趋势,致力于开发一种同槽双极锰电积清洁节能工艺,在同槽电解降低能耗的基础上发展清洁工艺,回收生产过程中产生的废酸,对环境保护、水体治理以及可持续发展具有重大意义。