Release characteristics of mercury in chemical looping combustion of bituminous coal

This study evaluated the release characteristics of mercury from bituminous coal in chemical looping combustion (CLC) using Australian iron ore as the oxygen carrier in a fixed bed reactor. The effects of several parameters, such as temperature in the fuel reactor (FR) and air reactor (AR), gasification medium in the FR, and reaction atmosphere in the AR, on mercury release characteristics, were investigated. The mercury speciation and release amount in the FR and AR under different conditions were further explored. The results indicate that most of the mercury in coal was released in the FR, while the rest of it was released in the AR. Hg⁰ was found to be the major species in the released mercury. The results also indicate that a higher temperature in the FR led to an increase in the total mercury release amount and a decrease in Hg⁰ proportion. However, a higher temperature in the AR resulted in a decrease in the total mercury release amount and Hg⁰ proportion. The increase in the H₂O/CO₂ ratio of gasification mediums in the FR was beneficial for the increase in the total mercury release amount and Hg⁰ proportion. A higher O₂ concentration in reaction atmosphere in AR had a negligible effect on the total mercury release amount, but a positive effect on Hg⁰ oxidization.     

京津冀化工场地地下水污染修复治理对策研究

京津冀化工场地地下水污染问题突出,严重威胁当地饮水安全和可持续发展,亟待开展修复治理.针对京津冀化工场地地下水污染现状,分析了化工场地地下水污染修复面临的挑战,提出了分区分级的修复治理对策.结果表明:①针对可能存在NAPL(非水相液体污染物)的高风险污染源区,采取高强度修复措施,以实现污染物总量的快速削减;②针对中度污染区,采取单位能耗强度更低的长效修复措施,降低修复成本和二次污染风险;③针对低风险的轻度污染区,采取风险管控措施.结合对典型化工场地地下水污染修复技术的分析,提出的分区分级修复治理对策具有以下特点:①多技术耦合,形成互补效应,可提高修复效率;②节约修复成本,降低二次环境影响;③体现基于风险的原则,避免过度修复.      

城市化、外商投资和产业结构因素对中国环境的影响

基于扩展的STIRPAT理论框架,采用动态空间面板模型分析方法,研究城市化、外商直接投资和产业结构因素对中国环境污染的长期与短期空间溢出效应.结果表明,一个地区的城市化率每提高10%,短期会降低当地CO₂排放水平的0.02%、降低邻近地区CO₂排放水平的0.04%;而从长期看会降低本地CO₂排放水平的0.08%、降低临近地区CO₂排放水平的0.2%.在2006年以前,一个地区的能源强度每降低1%,会在短期降低本地CO₂排放水平的0.31%、降低邻近地区CO₂排放水平的0.09%;从长期看则会降低本地CO₂排放水平的1.3%、降低邻近地区CO₂排放水平的0.55%.在2006年后,这种能源强度的变化会使碳排放短期内总共降低0.45%,长期看总共降低2.06%.城市化率每提高10%短期内会减少本地0.05%的SO₂排放、减少邻近地区0.1%的SO₂排放.第二产业比重每降低10%,会分别降低本地和临近区域SO₂排放水平的0.03%和0.09%.人口规模每扩大1%,会提升邻近区域SO₂排放水平的0.55%.能源强度每降低1%,会降低本地SO₂排放水平的0.12%.     

An integrated chemical mass balance and source emission inventory model for the source apportionment of PM2.5 in typical coastal areas

The source apportionment of PM_2.5 is essential for pollution prevention. In view of the weaknesses of individual models, we proposed an integrated chemical mass balance-source emission inventory (CMB-SEI) model to acquire more accurate results. First, the SEI of secondary component precursors (SO₂, NO_x, NH₃, and VOCs) was compiled to acquire the emission ratios of these sources for the precursors. Then, a regular CMB simulation was executed to obtain the contributions of primary particle sources and secondary components (SO₄^2?, NO₃^-, NH₄⁺, and SOC). Afterwards, the contributions of secondary components were apportioned into primary sources according to the source emission ratios. The final source apportionment results combined the contributions of primary sources by CMB and SEI. This integrated approach was carried out via a case study of three coastal cities (Zhoushan, Taizhou, and Wenzhou; abbreviated WZ, TZ, and ZS) in Zhejiang Province, China. The regular CMB simulation results showed that PM_2.5 pollution was mainly affected by secondary components and mobile sources. The SEI results indicated that electricity, industrial production and mobile sources were the largest contributors to the emission of PM_2.5 gaseous precursors. The simulation results of the CMB-SEI model showed that PM_2.5 pollution in the coastal areas of Zhejiang Province presented complex pollution characteristics dominated by mobile sources, electricity production sources and industrial production sources. Compared to the results of the CMB and SEI models alone, the CMB-SEI model completely apportioned PM_2.5 to primary sources and simultaneously made the results more accurate and reliable in accordance with local industrial characteristics.     

Characterization of a new smog chamber for evaluating SAPRC gas-phase chemical mechanism

A new state-of-the-art indoor smog chamber facility (CAPS-ZJU) has been constructed and characterized at Zhejiang University, which is designed for chemical mechanism evaluation under well-controlled conditions. A series of characterization experiments were performed to validate the well-established experimental protocols, including temperature variation pattern, light spectrum and equivalent intensity (J_NO2), injection and mixing performance, as well as gases and particle wall loss. In addition, based on some characterization experiments, the auxiliary wall mechanism has been setup and examined. Fifty chamber experiments were performed across a broad range of experimental scenarios, and we demonstrated the ability to utilize these chamber data for evaluating SAPRC chemical mechanism. It was found that the SAPRC-11 can well predict the O₃ formation and NO oxidation for almost all propene runs, with 6 hr Δ(O₃ – NO) model error of –3% ± 7%, while the final O₃ was underestimated by ~20% for isoprene experiments. As for toluene and p-xylene experiments, it was confirmed that SAPRC-11 has significant improvement on aromatic chemistry than earlier version of SAPRC-07, although the aromatic decay rate was still underestimated to some extent. The model sensitivity test has been carried out, and the most sensitive parameters identified are the initial concentrations of reactants and the light intensity as well as HONO offgasing rate and O₃ wall loss rate. All of which demonstrated that CAPS-ZJU smog chamber could derive high quality experimental data, and could provide insights on chamber studies and chemical mechanism development.     

郑州市典型工业企业VOCs排放特征及风险评估

为了解郑州市不同行业企业挥发性有机物(VOCs)污染特征及潜在危害,通过Summa罐和气袋采集样品,之后采用GC-MS/FID对样品进行测定分析.结果表明:郑州市包装印刷企业排放VOCs组分主要为含氧VOCs(OVOCs),包括乙酸乙酯和异丙醇,占比93.1%以上;汽车制造、家具制造和涂料生产企业VOCs组分主要为芳香烃,占比为33.5%～90.0%,以间/对-二甲苯、邻-二甲苯和乙苯为主;食品加工企业VOCs中卤代烃占比较高,为52.3%;橡胶企业VOCs主要为卤代烃和烷烃,占比分别为25.5%和28.8%;石墨碳素企业VOCs主要为芳香烃和OVOCs,占比分别为28.5%和24.1%.对比以往研究发现,郑州市与其他城市溶剂使用企业VOCs排放特征较为类似,但由于生产工艺及原辅料使用不同,相同行业企业中不同环节VOCs组分存在差异.风险评估结果显示,各企业排放的VOCs组分对臭氧生成潜势(OFP)和危害指数(HI)贡献具有一定正关联性,尤其苯、甲苯、乙苯及二甲苯等C_6～C_8芳香烃对OFP和HI贡献较大.汽车制造企业3号和家具企业5号HI值分别为1.18和2.74,均高于EPA规定限值,主要与该企业生产过程中使用溶剂型原辅料有关,且排放的主要以芳香烃为主,尤其苯、甲苯、乙苯、二甲苯和三甲基苯等C_6～C_9苯系物对HI和OFP的贡献较高,今后需重点管控溶剂型企业VOCs的排放.     

山西资源型城市创新环境与产业结构转型空间耦合

通过构建耦合协调度模型,分析2003年和2016年山西资源型城市创新环境与产业结构转型的空间耦合关系。结果表明：不同优势的城市创新环境质量随着时间的推移均发生不同程度的变化,其中高水平创新环境骤降,中等水平稳步升高,而低水平创新环境并未实现突破性的提升;产业结构高级化指数均呈增大趋势,产业结构合理化指数较高且变化相对复杂;原创新环境与产业结构高级化、合理化耦合度指数均较高且均为高度耦合区,但随着时间的推移,大部分城市逐渐下降;协调发展度较低,整体始终表现为“南北中度失调、中间严重失调”的格局;大部分城市相对发展度指数逐渐上升,山西“南北”区域属于创新环境超前型或同步发展型,而“中间”区域主要为创新环境滞后型的格局并未发生显著变化。因此,应当充分依托城市创新环境或产业结构转型现有的优势,因地制宜地分类指导其资源型城市建设发展,从而实现创新环境与产业结构转型的并进协同发展。     

HRT对CO2-MBfR去除高SO42-废水中NO3--N的影响

针对含NO₃^--N与较高浓度SO₄^2-实际工业废水处理较难的问题,考察了不同水力停留时间（HRT）下连续运行的CO₂-氢基质膜生物膜反应器（CO₂-MBfR）处理模拟废水和实际工业废水的性能,结果表明,2种废水的出水NO₃^--N浓度均随着HRT的减小而增大,模拟废水中NO₃^--N的处理效果和电子通量分配比例均优于实际废水,但其电子通量分配的格局基本不变：NO₃^--N和SO₄^2-的电子通量分别在90.09%~97.49%和2.51%~9.91%左右.要实现实际废水总氮达到15mg/L的排放标准,需维持HRT不少于10.4h.     

开封市公园地表灰尘PAHs污染与健康风险评价

应用气相色谱-质谱联用仪(GC-MS)测定了开封市相国寺、铁塔公园、龙亭公园、清明上河园等4个公园的53个地表灰尘样品中的16种优控多环芳烃(PAHs)含量,并分析了PAHs的来源、组成、污染水平和健康风险.结果表明:样品∑PAHs含量在332.20~7535.10μg·kg-1之间,平均值为1320.10μg·kg-1,其中,单体PAHs以菲、蒽、荧蒽、芘、苯并(a)蒽、苯并(b)荧蒽和苯并(a)芘等4~5环化合物含量较高;相国寺、铁塔公园、龙亭公园灰尘分别达到重度、中度、轻度PAHs污染,清明上河园未检测到PAHs污染.终生癌症风险增量模型(ILCRs)评价结果显示,儿童健康风险高于成人,皮肤接触灰尘PAHs是导致儿童和成人高风险的最主要暴露途径,其次是手口摄入途径.灰尘PAHs综合致癌风险(CR)的顺序为相国寺铁塔公园龙亭公园清明上河园,其中,相国寺的CR超过10-6,存在人体可耐受的致癌风险,其他公园不存在健康风险.影响公园灰尘PAHs含量、污染程度和健康风险的因素非常复杂,是建园时间、地理位置、公园性质、游客密度及周边环境状况等多种因素综合的结果.灰尘PAHs主要来源于石油、煤和生物质不完全燃烧,以及石油泄漏等.     

Chemical characteristics of fine particles and their impact on visibility impairment in Shanghai based on a 1-year period observation

In this work, a one-year observation focusing on high time resolution characteristics of components in fine particles was conducted at an urban site in Shanghai. Contributions of different components on visibility impairment were also studied. Our research indicates that the major components of PM_2.5 in Shanghai are water-soluble inorganic ions and carbonaceous aerosol, accounting for about 60% and 30% respectively. Higher concentrations of sulfate (SO₄²⁻) and organic carbon (OC) in PM_2.5 occurred in fall and summer, while higher concentrations of nitrate (NO₃⁻) were observed in winter and spring. The mass concentrations of Cl⁻ and K⁺ were higher in winter. Moreover, NO₃⁻ increased significantly during PM_2.5 pollution episodes. The high values observed for the sulfate oxidizing rate (SOR), nitrate oxidizing rate (NOR) and secondary organic carbon (SOC) in OC indicate that photochemical reactions were quite active in Shanghai. The IMPROVE (Interagency Monitoring of Protected Visual Environments) formula was used in this study to investigate the contributions of individual PM_2.5 chemical components to the light extinction efficient in Shanghai. Both NH₄NO₃ and (NH₄)₂SO₄ had close relationships with visibility impairment in Shanghai. Our results show that the reduction of anthropogenic SO₂, NO_x and NH₃ would have a significant effect on the improvement of air quality and visibility in Shanghai.