Chemical characterization and source apportionment of PM1 and PM2.5 in Tianjin, China: Impacts of biomass burning and primary biogenic sources

The submicron particulate matter (PM₁) and fine particulate matter (PM_2.5) are very important due to their greater adverse impacts on the natural environment and human health. In this study, the daily PM₁ and PM_2.5 samples were collected during early summer 2018 at a sub-urban site in the urban-industrial port city of Tianjin, China. The collected samples were analyzed for the carbonaceous fractions, inorganic ions, elemental species, and specific marker sugar species. The chemical characterization of PM₁ and PM_2.5 was based on their concentrations, compositions, and characteristic ratios (PM₁/PM_2.5, AE/CE, NO₃^?/SO₄^2?, OC/EC, SOC/OC, OM/TCA, K+/EC, levoglucosan/K⁺, V/Cu, and V/Ni). The average concentrations of PM₁ and PM_2.5 were 32.4 µg/m³ and 53.3 µg/m³, and PM₁ constituted 63% of PM_2.5 on average. The source apportionment of PM₁ and PM_2.5 by positive matrix factorization (PMF) model indicated the main sources of secondary aerosols (25% and 34%), biomass burning (17% and 20%), traffic emission (20% and 14%), and coal combustion (17% and 14%). The biomass burning factor involved agricultural fertilization and waste incineration. The biomass burning and primary biogenic contributions were determined by specific marker sugar species. The anthropogenic sources (combustion, secondary particle formation, etc) contributed significantly to PM₁ and PM_2.5, and the natural sources were more evident in PM_2.5. This work significantly contributes to the chemical characterization and source apportionment of PM₁ and PM_2.5 in near-port cities influenced by the diverse sources.     

三峡库区汉丰湖水体氮磷及化学计量比季节变化特征

在分析2017年3月至2018年2月汉丰湖水体氮磷营养盐质量浓度季节性变化的基础上,利用氮磷化学计量摩尔比评估水体氮磷养分限制状态.结果表明：湖体TN、DN和NO₃^--N平均质量浓度分别为1.60、1.25和0.91 mg·L^-1,三者季节变化过程相似,均呈现出冬季最高、夏季最低的特点.NO₃^--N对水体TN贡献较大,NH₄⁺-N和NO₂^--N质量浓度维持在较低水平且变化平稳.TP、DP和PO₄^3--P平均质量浓度分别为0.13、0.09和0.06 mg·L^-1,TP和DP质量浓度变化相似,呈春夏季升高,秋冬季先降低再升高的趋势,而PO₄^3--P质量浓度则波动降低.TN/TP范围在11.07~56.02之间,均值为29.23,TN/TP呈季节性波动变化,最高值出现在冬季,最低值出现在夏季.汉丰湖水体多数时间适宜藻类生长繁殖,少数时间处于N限制状态,极少数时间处于P限制状态.降雨径流、肥料使用、污水排放和水生生物活动等因素皆会影响TN/TP的季节变化,同时根据汉丰湖水质特征提出保护建议.     

A highly porous animal bone-derived char with a superiority of promoting nZVI for Cr(VI) sequestration in agricultural soils

Paddy soil and irrigation water are commonly contaminated with hexavalent chromium [Cr(VI)] near urban industrial areas, thereby threatening the safety of agricultural products and human health. In this study, we develop a porous and high specific area bone char (BC) to support nanoscale zero-valent iron (nZVI) and apply it to remediate Cr(VI) pollution in water and paddy soil under anaerobic conditions. The batch experiments reveal that BC/nZVI exhibits a higher removal capacity of 516.7 mg/(g?nZVI) for Cr(VI) than nZVI when normalized to the actual nZVI content, which is 2.8 times that of nZVI; moreover, the highest nZVI utilization is the nZVI loading of 15% (BC/nZVI15). The Cr(VI) removal efficiency of BC/nZVI15 decreases with increasing pH (4 – 10). Coexisting ions (phosphate and carbonate) and humic acid can inhibit the removal of Cr(VI) with BC/nZVI15. Additionally, BC exhibits a strong advantage in promoting Cr(VI) removal by nZVI compared to the widely used biochar and activated carbon. Our results demonstrate that reduction and coprecipitation are the dominant Cr(VI) removal mechanisms. Furthermore, BC/nZVI15 shows a significantly higher reduction and removal efficiency as well as a strong anti-interference ability for Cr(VI) in paddy soil, as compared to nZVI. These findings provide a new effective material for remediating Cr(VI) pollution from water and soil.     

2009~2019年中国人为CH4排放量的估算及时空格局

以中国340个地级及以上城市为研究对象,采用自下而上的核算方法,针对农业活动、能源活动和废物处理3个一级CH₄排放源,核算2009年和2019年中国人为CH₄排放量并分析其时空格局.结果表明：2009年中国人为CH₄总排放40.71Tg,2019年为42.89Tg,CH₄排放总量在增加,排放强度和人均排放量基本保持不变.一级排放源中,农业活动、能源活动和废物处理在2009年的CH₄排放量分别为24.88Tg、12.06Tg和3.76Tg,农业活动为主要排放源,2019年三者排放量分别为16.99Tg、21.62Tg和4.28Tg,能源活动成为主要排放源;二级排放源中煤炭开采的CH₄排放最多;不同城市中各排放源的占比存在较大差异,淮安、扬州和南通农业活动排放最多,晋城、大同和太原能源活动排放最多,而北京、上海和广州以废物处理排放为主.城市人为CH₄排放存在显著的空间正相关,高排放—高聚集的城市数量减少,分布集中;低排放—低聚集的城市数量增加,分布重心向东部地区转移;局部城市空间关联类型呈现出较强的空间锁定效应和迁移惰性特征.CH₄排放强度与人均CH₄排放的区域总体差异较大;CH₄排放强度地区间Theil指数差异较大,而地区内差异较小;人均CH₄排放地区间与地区内的Theil指数差异均较小.     

Mechanisms of Pb(II) coprecipitation with natrojarosite and its behavior during acid dissolution

Lead (Pb) coprecipitation with jarosite is common in natural and engineered environments, such as acid mine drainage (AMD) sites and hydrometallurgical industry. Despite the high relevance for environmental impact, few studies have examined the exact interaction of Pb with jarosite and the dissolution behavior of each phase. In the present work, we demonstrate that Pb mainly interacts with jarosite in four modes, namely incorporation, occlusion, physically mixing, and chemically mixing. For comparison, the four modes of Pb-bearing natrojarosite were synthesized and characterized separately. Batch dissolution experiments were undertaken on these synthetic Pb-bearing natrojarosites under pH 2 to simulate the AMD environments. The introduction of Pb decreases the final Fe releasing efficiency of jarosite-type compounds from 18.18% to 3.45%-5.01%, showing a remarkable inhibition of their dissolution. For Pb releasing behavior, PbSO₄ dissolves in preference to Pb-substituted natrojarosite, i.e., (Na, Pb)-jarosite, which primarily results in the sharp increase of Pb releasing concentration (> 40 mg/L). PbSO₄ occlusion by jarosite-type compounds can significantly reduce the release of Pb. The results of this study could provide useful information regarding Fe and Pb cycling in acidic natural and engineered environments.     

Mercury release behaviors of Guizhou bituminous coal during co-pyrolysis: Influence of chlorella

Co-pyrolysis of coal and seaweed can not only effectively decrease the carbon footprint but also improve the quality and output of coal pyrolysis products, however, the influence of seaweed on thermal releasing behaviors of mercury during co-pyrolysis process are still unclear. In this work, the chlorella and Guizhou bituminous coal were mixed and used to reveal the mercury release behavior during co-pyrolysis by the temperature programmed pyrolysis experiments, thermogravimetric and differential thermogravimetric analysis (TG-DTG) and thermogravimetry-mass spectrometry (TG-MS) methods, offering a sufficient explanation on the control technology of mercury pollutants in co-pyrolysis. The results exhibited that a large amount of reducing gases such as CO, H₂ and H₂O were generated in chlorella at the temperature range of 100-500°C, which was favorable for the transformation from oxidized mercury to elemental mercury, thus remarkably increased the release of elemental mercury in the raw coal sample. The mixed chlorella also significantly lowered the decomposition temperature range (from 400-600 to 300-400°C) of pyrite-bound mercury and decreased the decomposition temperatures of the pyrite-bound mercury species. Additionally, in the co-pyrolysis about 91.82% of mercury was released into the gas phase below 400°C and was 13.77% higher than that of in individual pyrolysis of coal.     

中国东海水体中多氯联苯的浓度及其组成特征

东海由于受到长江和闽浙沿岸工业污水输入以及电子垃圾处理场排放的影响,被认为是多氯联苯重污染区域。本研究利用"科学三号"科学考察船,于2012年10月执行的东海航次期间,从中国东海不同区域采集到11个表层水样,测定其中溶解态多氯联苯的浓度。中国东海水体中多氯联苯浓度为（0.59~1.68）ng/L,相比国内外海域,属于中低等水平。研究结果表明,海水多氯联苯浓度和盐度之间存在显著负相关性,说明沿岸河流冲淡水搬运的多氯联苯是东海水体中多氯联苯的重要来源;此外其组成以三氯,四氯和五氯为主,这与我国历史上多氯联苯的使用情况吻合。通过水体中不同氯代化合物浓度和对应K_OW理论浓度值的比较发现,两者之间整体吻合较好,表明化合物的物理化学属性是控制其在水体中浓度的重要因素。然而,东海近岸水体中六氯联苯污染程度略高于理论浓度值,这一潜在的污染来源可能和东海沿岸省市电子垃圾处理场有关。     

重庆废弃煤矿区表层土壤多环芳烃污染特征及风险评价

随着煤炭行业的萧条,废弃煤矿逐渐增加。为有效管理和改善矿区废弃地环境生态系统,采集废弃22年的重庆中梁山马家沟煤矿区内18个表层土壤样品和1个煤矸石样品,以及矿区之外的2个背景土壤样品,分析样品中多环芳烃（USEPA 16 PAHs）、正构烷烃（n-alkanes）、汞（Hg）和有机质（OM）含量水平。结果表明,表层土壤中PAHs的平均含量为170.3 ng/g,低于我国正在运行的煤矿区土壤PAHs含量水平,高于山区背景土壤PAHs含量水平。主成分分析（PCA）结果表明煤燃烧释放和原煤残渣分别贡献78.3%和17.6%,是表层土壤中PAHs的主要来源。PAHs与n-alkanes的相关系数r=0.83（P<0.01）,表明土壤中两者具有类似的输入途径和富集行为。PAHs与Hg之间不存在相关性,表明煤矿长期废弃后,这两种与矿区活动释放有关的污染物的环境归趋有显著差异。PAHs和OM之间也不存在相关性,表明与煤矿相关的有机质来源已经被植物、微生物的分泌物质及其残体的有机质替代,生态环境正逐步恢复。风险评价结果表明PAHs含量水平相对安全。值得注意的是,Hg含量超过农用地土壤污染风险筛选值。因此,政府对矿区旧址的土地利用应当基于多污染参数的叠加结果,避免单一指标的片面性评价与诊断。     

哈尔滨市大气细颗粒物污染特征及其毒性效应

为研究哈尔滨市大气细颗粒物的污染特征及其毒效应,分别采集PM_2.5、PM_1.0样品,分析其质量浓度、数浓度的变化分布特征以及对小鼠肺损伤的影响.结果表明：2017年全年PM_2.5、PM_1.0的质量浓度均呈冬高夏低趋势;PM_1.0质量浓度占PM_2.5总质量浓度的62%~85%,PM_1.0数浓度变化趋势为两边高中间低,且其大小与温度呈负相关,与相对湿度无显著相关性;研究大气颗粒物对小鼠肺损伤影响时发现,染毒组小鼠肺组织细胞中LDH、ACP、AKP、ALB增高,说明大气颗粒物PM_2.5和PM_1.0对小鼠肺组织细胞具有毒效应;肺灌洗液中MDA、NO、NOS水平升高,SOD活性下降,说明PM_2.5和PM_1.0都使机体发生氧化损伤,且PM_2.5和PM_1.0质量浓度增加,会使小鼠肺组织细胞毒效应增强,由此引发的机体氧化损伤程度增大.     

GIS-based analysis of population exposure to PM2.5 air pollution—A case study of Beijing

PM_(2.5), formally defined as particulate matter with diameter less than 2.5 μm, is one of most harmful air pollutants threatening human health. Numerous epidemiological studies have shown that both short-term and long-term exposures to PM_(2.5) are strongly linked with respiratory diseases. In this study, various types of spatio-temporal data were collected and used to estimate the spatio-temporal variation of PM_(2.5) exposure in Beijing in 2014. The seasonal and daily variation of the population-weighted exposure level(PWEL) in 2014 was estimated and compared. The results show that the population exposure to ambient air pollution differs significantly in the four seasons, and the exposure levels in winter and spring are notably higher than the other seasons; the exposure level changes greatly from North to South, and each sub-district maintains similarity to neighboring sub-districts.