中国工程机械使用特征及其尾气排放趋势

非道路移动源的尾气排放因其对空气污染的贡献大而日益受到关注.准确估算非道路移动源的尾气排放清单对空气质量管理至关重要.本研究通过收集整理调研获取的工程机械活动水平数据,分析工程机械使用特征,包括:不同机械间的活动水平差异、活动水平的区域性差异及活动水平与机械车龄的关系等;此外,研究使用BP神经网络模型预测2018～2025年中国工程机械保有量,利用便携式尾气测量系统对47台工程机械进行现实工况下的尾气排放测量,量化其污染物排放水平,并最终结合机械活动水平估算2015～2025年中国工程机械的尾气排放清单.结果表明,工程机械的活动水平随着机械种类的不同而不同,年均使用时间在1 439～4 332 h之间变化.同一类机械在不同区域范围内的活动水平也存在较大的地域差异,最大差别可达3倍以上.此外,工程机械的活动水平一般也随机械车龄的增加而减少,据估计,车龄增加一年,其活动水平减少约140～150 h.经估算, 2015年,中国工程机械CO、 HC、 NO和PM_(2.5)的排放量分别为209.9、 46.2、 345.2和57.4万t;由于2015年后工程机械保有量增速放缓,到2020年,CO、 HC和PM_(2.5)排放量比2015年下降2.4%～33.1%不等,到2025年,排放量将进一步下降7.1%～64.7%.而NO排放量在2015年后稍有增加,但2020年后开始下降.然而,虽然工程机械污染物的排放持续下降,但与道路移动源相比,幅度较小,因此,其排放对大气污染的贡献将在未来日益突出,需引起足够重视.     

四川省基于第二次污染源普查数据的人为源大气污染源排放清单及特征

本研究根据自下而上和自上而下相结合的方法收集四川省人为源活动水平数据,其中工业源活动水平来自四川省第二次污染源普查数据,涵盖11020台锅炉信息、60078家工业企业信息,成都市收集了19152家工业企业数据,占四川省企业总数的32%.各污染源选取合理的排放因子并结合GIS技术,构建了该地区2017年9 km×9 km人为源大气污染物排放清单.结果表明,2017年四川省SO₂、NO_x、CO、PM₁₀、PM_2.5、BC、OC、VOCs和NH₃排放总量分别为308.6×10³、725.7×10³、3131.2×10³、927.6×10³、422.4×10³、30.2×10³、72.0×10³、600.9×10³和887.1×10³t.固定燃烧源和工艺过程源是SO₂主要贡献源,CO的主要贡献源为工艺过程源和移动源,扬尘源和工艺过程源为PM₁₀和PM_2.5的主要贡献源,扬尘源是BC和OC最大贡献源,VOCs排放源主要来自工艺过程源、移动源和溶剂使用源,NH₃排放主要来源于畜禽养殖和氮肥施用.污染空间分布结果显示,各项污染物主要集中分布于人口密集,工业和农业较为发达的四川盆地和攀枝花部分区域,高值点位集中在成都平原地区的德阳—成都—眉山—乐山沿线.本研究建立的排放清单仍具有一定不确定性,后续研究工作中应进一步加强活动水平数据获取的准确性,针对典型污染源开展污染物排放因子测试工作,完善网格化排放清单,为四川省大气污染防治提供科学支撑.     

现实工况下挖掘机尾气排放特征分析

为量化挖掘机在实际施工作业中尾气排放特征,研究选取成都市不同建设工地在用的8台挖掘机,利用便携式尾气测量系统对其进行现实工况下的尾气排放测量,测试按挖掘机的不同作业特点分怠速、行走和作业进行.测量的尾气排放污染物包括CO、HC、NO和PM_2.5.结果表明,挖掘机的尾气排放随工况的不同而不同,怠速时NO排放平稳,行走和作业时排放速率波动较大.满足不同尾气排放标准的挖掘机,其尾气排放也有所不同,例如,国Ⅱ阶段的挖掘机与国Ⅰ阶段的挖掘机相比,其在怠速、行走、作业工况下尾气排放的NO分别减小8%、35%和5%,PM_2.5分别降低88%、87%和80%.另外,本研究中挖掘机尾气排放的实测结果与我国非道路机械尾气排放因子技术指南中推荐的用于排放清单估算的排放因子相比,也均有显著不同.这说明,开展非道路机械尾气排放现实工况下的测量,对于提高尾气排放清单精准度具有重要作用.     

广东省高分辨率温室气体排放清单及特征

根据典型城市调查与统计数据收集得到的广东省活动水平数据,采用自上而下和自下而上相结合的排放因子法和GIS技术,建立了广东省2018年3 km×3 km高分辨率温室气体排放清单.估算范围包括能源活动、工业生产过程、农业活动、土地利用变化和林业、废弃物处理以及电力调入（出）间接排放等6大类CO₂、CH₄和N₂O这3种温室气体.结果表明,广东省2018年CO₂、CH₄和N₂O的排放量分别为8.5×10⁸、1.9×10⁶和1.1×10⁵ t,以CO₂当量计分别为8.5×10⁸、4.0×10⁷和3.4×10⁷ t,合计9.2×10⁸ t.CO₂是广东省主要的温室气体排放种类,占全省温室气体总排放量的92.0%,能源活动和电力调入（出）间接排放是广东省温室气体排放的主要部门,排放占比分别为77.9%和7.6%,合计占比为85.5%.从温室气体排放的空间分布情况来看,全省大部分地区温室气体表现为排放源,部分区域表现为汇;温室气体排放主要集中在珠三角地区,并呈现一定的沿路网和航道分布的特征;温室气体高排放网格主要为大型电厂、钢铁厂和水泥厂等高耗能企业所在地.     

2010~2017年四川省机动车污染物排放趋势分析

四川省机动车保有量日益增加,本研究基于特定的清单计算方法及多口径的活动水平数据,得到四川省2010~2017年机动车尾气污染物排放量.结果表明,四川省小型载客汽车的保有量增长最快,不管是机动车还是小型载客车保有量的增速,均高于全国平均增速;2017年四川省机动车共排放CO、NO_x、SO₂、NH₃、HC、PM_2.5、PM₁₀、BC和OC分别为706.9、275.3、0.3、5.7、164.8、8.1、8.9、4.1和1.4 kt,除NH₃以外,四川省所排放的其他污染物呈现波动中下降的趋势,在2014~2016年前后达到高值.柴油车的保有量变化与NO_x的变化显示出较强的相关性;新车排放标准加严是最具有减排潜力的措施之一,同时随着实施年份的增长,显示的减排潜力越大,燃油品质的提升对于污染物的减排每年也会有6%以上的减排效力.未来应将HC和NO_x减排作为四川省机动车管控的重要内容.     

超低改造下中国火电排放清单及分布特征

本研究基于2018年火电在线监测和环境统计等数据,自下而上编制了中国高分辨率火电行业排放清单,并核算了排放浓度、排放因子和排放量.结果表明超低排放政策效果显著：2018年火电SO₂、NO_x和烟尘平均排放浓度分别为37.57、56.71和7.41mg ·m^-3.比2015年分别下降58.71%、43.12%和60.79%;中国燃煤机组的SO₂、NO_x和烟尘平均排放因子分别为0.30、0.48和0.06 g ·kg^-1,比2015年分别下降55.2%、36.84%和62.5%;中国火电SO₂、NO_x、烟尘和PM_2.5总排放量分别为72.14、118.38、14.90和13.59万t ·a^-1,比2015年分别下降41.32%、19.29%、48.12%和40.39%.     

兰-白城市群主要大气污染物网格化排放清单及来源贡献

甘肃兰-白城市群为我国西北地区重要的重工业基地,大气污染物排放总量较大.研究高空间分辨率的污染物排放清单对于区域空气质量预报预警、减排方案模拟研究及大气污染防治等具有重要的科学意义.本文以兰州和白银为主要研究区域,基于研究区域污染源排放及统计年鉴等数据资料,建立了兰（2015年）-白（2016年）城市群7种（类）主要大气污染物网格化排放清单,并对其空间排放特征以及排放源贡献进行了详尽地讨论分析.结果表明,兰-白城市群7种主要污染物年排放量分别为：NO_x 2.22×10⁵ t、NH₃ 4.53×10⁴ t、VOCs 7.74×10⁴ t、CO 5.62×10⁵ t、PM₁₀ 4.95×10⁵ t、PM_2.5 1.91×10⁵ t和SO₂ 1.37×10⁵ t.其中CO的排放量最大,NH₃的排放量最小.本清单与北大和清华MEIC清单对比结果表明,交通源排放3个清单一致性较高,CO排放总量和其工业源排放与北大和清华MEIC清单排放源相差30%~40%,推测原因主要为清单计算过程中排放因子、分辨率和数据年份的差异.本清单网格化空间分布显示除NH₃外的其他6种（类）污染物,排放主要集中在市区,排放源中工业非燃烧过程源均为最大贡献占比,NH₃的主要贡献源是氮肥的施用及禽畜排放,其污染分布受耕地分布等因素影响较大.因此,减少工业非燃烧过程源、整合优质高效电力供应、使用清洁能源、严格控制工地扬尘、工业粉尘和做好城区绿化等,能有效地降低兰-白城市群NO_x、VOCs、CO、PM₁₀、PM_2.5和SO₂这6种（类）主要污染物的排放.NH₃的减排则主要可从控制氮肥的使用及减少禽畜排放两方面考虑.本研究还利用蒙特卡洛法分析了排放清单的不确定性,NH₃的不确定性最大为-31%~30%,CO的不确定性最小为-18%~16%,清单整体可信度较高.     

兰州市高分辨率人为源排放清单建立及在WRF-Chem中应用评估

城市尺度高分辨率人为源大气污染物排放清单是城市空气质量预报预警、污染成因分析和减排措施制定的重要基础数据,目前我国西部地区城市尺度的人为源排放清单研究仍然相对薄弱,能对接于空气质量模式的排放清单更为缺乏.本文整合已发表的清单文献,建立了可对接于空气质量模式的2016年兰州市城市尺度的人为源清单模型（HEI-LZ16）,将之应用于WRF-Chem模式,评估HEI-LZ16的准确性和适用性.结果表明：兰州市2016年人为源排放的SO₂、NO_x、CO、NH₃、VOCs、PM₁₀、PM_2.5、BC和OC总量分别为25642、53998、319003、10475、35289、49250、19822、2476和1482 t·a^-1.在模拟时间内,HEI-LZ16相比于MEIC,O₃和PM_2.5的NME值分别减小了140.2%和28.8%,HEI-LZ16更加准确适用.分析了HEI-LZ16情景下模拟的PM_2.5和O₃时空分布,兰州市臭氧MDA8呈现冬春季城区低而郊区高,夏秋季河谷城区西部及其下风向地区高的分布特征,夏秋季高浓度区的分布受偏东风和光化学反应的共同影响,冬季城区O₃浓度受NO_x排放的抑制作用浓度反而降低.PM_2.5浓度的高值区主要集中在黄河河谷盆地,本研究表明沿白银—兰州黄河河谷盆地走向的西侧存在一个污染物传输通道,其对兰州市环境空气质量具有较大的影响.     

渭南市道路移动源高分辨温室气体排放清单及特征研究

根据渭南市机动车保有量和抽样调查与观测数据,采用MOVES模型计算了渭南市2017—2019年道路移动源CO₂、CH₄、N₂O和CO 4种 温室气体的排放量,分析了机动车车型、燃料和排放标准对温室气体排放量的影响.基于ArcGIS和渭南市道路网信息,建立了高分辨率（1 km× 1 km和1 h×1 h）的温室气体排放清单.结果表明,渭南市2019年道路移动源CO₂、CH₄、N₂O和CO的排放量分别为424.322×10⁴、0.044×10⁴、0.007×10⁴和2.808×10⁴ t,以CO₂当量计,机动车温室气体的总排放量为432.843×10⁴ t. 4种道路移动源温室气体中,CO₂占总温室气体排放量的98.03%.渭南市小型客车对温室气体的贡献率最大,分别排放了43.41%的CO₂、74.78%的N₂O和57.17%的CO.大型客车排放了34.47%的CH₄, 汽油车和天然气汽车是N₂O和CH₄的主要排放源,分别排放了86.76%的N₂O和61.87%的CH₄.渭南市道路移动源温室气体排放强度24 h变化呈“双峰”分布,空间分布呈明显的“线-面”特征,这与道路分布密度高度相关,路网密集的城市中心为机动车温室气体的高排放区.     

应用大气化学模型解析华北地区大气氮沉降时空分布特征及影响因素

本研究基于大气化学传输模型模拟结果,分析了2005—2015年华北地区大气氮沉降的时空分布特征,通过对2005年和2015年的结果进行模型敏感性实验,定量分析了全国和华北本地的人为源排放以及气象场对华北地区氮沉降年际变化的贡献。结果表明：（1）2005—2015年华北地区氮沉降年均量为28.7 kg·hm⁻²·a⁻¹（以N计,余同）,其中18.7 kg·hm⁻²·a⁻¹来自还原态氮（NH_x）,10.0 kg·hm⁻²·a⁻¹来自氧化态氮（NO_y）。湿沉降占比为56%（16.1 kg·hm⁻²·a⁻¹）,略高于干沉降（12.6 kg·hm⁻²·a⁻¹）。氮沉降的高值主要集中在华北的东南地区,低值集中在华北的西北地区,整体呈夏季高冬季低的季节特征。（2）2005—2015年,华北地区氮沉降整体呈先增加后减少的趋势,波动范围在27.4—30.4 kg·hm⁻²·a⁻¹。相较2005年,2015年氧化氮沉降增加了2.2 kg·hm⁻²·a⁻¹,而还原氮沉降减少了1.9 kg·hm⁻²·a⁻¹。其中氮氧化物（NO_x）和氨气NH₃）人为源排放的变化分别导致了1.0 kg·hm⁻²·a⁻¹氧化氮沉降的增加和2.5 kg·hm⁻²·a⁻¹还原氮沉降的减少,分别占全国人为源排放贡献的89%和53%,这说明区域传输对于2005—2015年还原氮沉降变化的影响较大。（3）华北地区干沉降的年际变化主要取决于前体物排放的变化,而湿沉降不仅受前体排放的影响,也受到降水等气象场的驱动。     

Distribution and ecological effect of mercury in Laogang landfill, Shanghai, China

Laogang landfill near Shanghai is the largest landfill in China, and receives about 10000 t of daily garbage per day, Samples of topsoil and plants were analyzed to evaluate mercury pollution from the landfill. For topsoil samples, there were significant correlations among total mercury （HgT）, combinative mercury （Hgc） and gaseous mercury （HgG）, and content of total organic carbon （TOC）, but, no significantly relationship was found between Hg content and filling time. Hg content changes in vertical profiles with time showed that the average Hgv of profiles 1992, 1996, and 2000 was similar, but their average HgG was quite different. HgT was significantly correlated with Hgc in profile 1992 and 2000, and Hgv was significantly correlated with Hg6 in profile 1996. HgG/Hgv ratio in profile samples decreased in the order of （HgG,/HgT）1992〉（HgG/HgT）1996〉〉（HgG/HgT）2000. A simple outline of Hg release in landfill could be drawn： with increasing of filling time, degradation undergoes different biodegradation, accordingly, gaseous mercury goes through small, more, and small proportion to total mercury. Distribution of Hg in plants was inhomogeneous, following the order of leaf〉root〉stem. The highest value of leaf may be associated with higher atmospheric Hg from landfill. Ligneous plants （e.g. Phyllostachys glanca, Prunus salicina and Ligustrum lucidum） are capable of enriching more Hg than herbaceous plants.     

EDTA-enhanced phytoremediation of lead contaminated soil by Bidens maximowicziana

Phytoremediation is a potential cleanup technology for the removal of heavy metals from contaminated soils.Bidens maximowicziana is a new Pb hyperaccumulator,which not only has remarkable tolerance to Pb but also extraordinary accumulation capacity for Pb.The maximum Pb concentration was 1509.3 mg/kg in roots and 2164.7 mg/kg in overground tissues.The Pb distribution order in the B. maximowicziana was:leaf>stem>root.The effect of amendments on phytoremediation was also studied.The mobility of soil Pb and the Pb concentrations in plants were both increased by EDTA application.Compared with CK(control check),EDTA application promoted translocation of Pb to overground parts of the plant.The Pb concentrations in overground parts of plants was increased from 24.23-680.56 mg/kg to 29.07-1905.57 mg/kg.This research demonstrated that B.maximowicziana appeared to be suitable for phytoremediation of Pb contaminated soil,especially,combination with EDTA.     

Decomposition of alachlor by ozonation and its mechanism

Decomposition and corresponding mechanism of alachlor, an endocrine disruptor in water by ozonation were investigated. Results showed that alachlor could not be completely mineralized by ozone alone. Many intermediates and final products were formed during the process, including aromatic compounds, aliphatic carboxylic acids, and inorganic ions. In evoluting these products, some of them with weak polarity were qualitatively identified by GC-MS. The information of inorganic ions suggested that the dechlorination was the first and the fastest step in the ozonation of alachlor.     

Enzymatic oxidation of aqueous pentachlorophenol

The influence of the nonionic surfactant Tween 80 on pentachlorophenol （PCP） oxidation catalyzed by horseradish peroxidase was studied. The surfactant was tested at concentrations below and above its critical micelle concentration （CMC）. Enhancement of PCP removal was observed at sub-CMCs. The presence of Tween 80 in the reaction mixture reduced enzyme inactivation which occurred through a combination of free radical attack and sorption by precipitated products. A simple first-order model was able to simulate time profiles for enzyme inactivation in the presence or absence of Tween 80. At supra-CMCs, the surfactant caused noticeable reductions in PCP removal, presumably through micelle partitioning of PCP which precluded the hydrophobic PCP molecule from interacting with the enzyme.     

基于综合水质标识指数和对应分析法的校园河道水质评价

以三峡大学的校园河道求索溪为研究对象,利用综合水质标识指数法确定求索溪水质类别,分析其水质时空变化规律,并利用对应分析法得出求索溪中不同监测点的主要污染因子.研究结果表明:求索溪整体的综合水质标识指数为7.423,整体水质为劣V类(地表水环境质量标准GB 3838-2002)且黑臭.从时间变化来看,求索溪4月份的水质最差,5月份次之,4、5月份所有监测点的水质都劣于V类且黑臭;8月份水质最好,水质为Ⅳ类;从空间分布来看,8个监测点综合水质标识指数均超过6.0,水质为劣V类,其中6号监测点的水质相对最好,监测点3号的水质相对最差;对应分析法得出求索溪的整体水体污染程度受总氮因子的影响最大,其次为总磷.该研究拟为求索溪及类似校园河道的水环境治理研究提供基础依据和参考.     

Effects of chitosan on growth of an aquatic plant (Hydrilla verticillata) in polluted waters with different chemical oxygen demands

Effects of chitosan on a submersed plant, Hydrilla verticillata, were investigated. Results indicated that H. venicillata could prevent ultrastructure phytotoxicities and oxidativereaction from polluted water with high chemical oxygen demand (COD). Superoxide dismutase (SOD) activity and malondialdehyde (MDA) contents in H. verticillata treated with 0.1% chitosan in wastewater increased with high COD (980 mg/L) and decreased with low COD (63 mg/L), respectively. Ultrastructural analysis showed that the stroma and grana of chloroplast basically remained normal. However, plant cells from the control experiment (untreated with chitosan) were vacuolated and the cell interval increased. The relict of protoplast moved to the center, with cells tending to disjoint. Our findings indicate that wastewater with high COD concentration can cause a substantial damage to submersed plant, nevertheless, chitosan probably could alleviate the membrane lipid peroxidization and ultrastructure phytotoxicities, and protect plant cells from stress of high COD concentration polluted water.     

Removal of cadmium using MnO2 loaded D301 resin

MnO2 loaded weak basic anion exchange resin D301 （Anion exchange resin, macroreticular weak basic styrene） as adsorbent has been prepared and applied to the removal of cadmium. The adsorption characteristics have been investigated with respect to effect of pH, equilibrium isotherms, removal kinetic data, and interference of the coexisting ions. The results indicated that the Cd^2＋ could be efficiently removed using MnO2 loaded D301 resin in the pH range of 3-8 from aqueous solutions with the co-existence of high concentration of alkali and alkaline-earth metals ions. The saturate adsorption capacity of the Cd^2＋ was 77.88 mg/g. The adsorption process followed the pseudo first-order kinetics. The equilibrium data obtained in this study accorded excellently with the Langmuir adsorption isotherm.     

Effect of coagulation pretreatment on the fouling of ultrafiltration membrane

The purpose of this study is to understand the effect and mechanism of preventing membrane fouling, by coagulation pretreatment, in terms of fractional component and molecular weight of natural organic matter （NOM）. A relatively higher molecular weight （MW） of hydrophobic compounds was responsible for a rapid decline in the ultrafiltration flux. Coagulation could effectively remove the hydrophobic organics, resulting in the increase of flux. It was found that a lower MW of neutral hydrophilic compounds, which could remove inadequately by coagulation, was responsible for the slow declining flux. The fluxes in the filtration of coagulated water and supernatant water were compared and the results showed that a lower MW of neutral hydrophilic compounds remained in the supernatant water after coagulation could be rejected by a membrane, resulting in fouling. It was also found that the coagulated flocs could absorb neutral hydrophilic compounds effectively. Therefore, with the coagulated flocs formed on the membrane surface, the flux decline could be improved.     

Penetration analysis of elements and bioleaching treatment of spent refractory for recycling

Acidithiobacillus ferrooxidans ATCC23270 and Acidithiobacillus thiooxidans TM-32 were used for bioleaching of spent refractories of aluminium and copper melting furnaces for their recycling.Firstly,penetration of elements into aluminium melting furnace refractory was investigated and it was found that up to 7 cm from surface was contaminated.Comparison on leaching efficiency by the strains ATCC23270 and TM-32 found that the strain ATCC23270 could treat larger amount of the refractories than the strain TM-32 could do.In the experiment of bioleaching of spent refractory aluminium melting furnace by the strain ATCC23270,high leaching efficiency were obtained on Al,Si,and Ca,and extremely low leaching performance was,however,shown on the rest of elements i.e.,Na,Mn,and Zn.Under the strain TM-32 use,relatively high leaching performance was recognized on Al,Si,Ca,Na,Mn,and Zn.In the experiment of bioleaching for spent refractory copper melting furnace,almost the same leaching trends were shown on Cu,Zn,Al,and Si under the strains ACTT23270 and TM-32 uses.     

Simultaneous removal of ammonium and phosphate by zeolite synthesized from coal fly ash as influenced by acid treatment

Zeolite synthesized from fly ash （ZFA） without modification is not efficient for the purification of NH4＋ and phosphate at low concentrations that occur in real effluents, despite the high potential removal capacity. To develop an effective technique to enhance the removal efficiency of ammonium and phosphate at low concentrations, ZFA was modified with acid treatment and the simultaneous removal of ammonium and phosphate in a wide range of concentration was investigated. It was seen that when compared with untreated ZFA, only the treatment by 0.01 mol/L of H2SO4 significantly improved the removal efficiency of ammonium at low initial concentrations. The behavior was well explained by the pH effect. Treatment by more concentrated H2SO4 led to the deterioration of the ZFA structure and a decrease in the cation exchange capacity. Treatment by 0.01 mol/L H2SO4 improved the removal efficiency of phosphate by ZFA at all initial P concentrations, while the treatment by concentrated H2SO4 （≥0.9 mol/L） resulted in a limited maximum phosphate immobilization capacity （PIC）. It was concluded that through a previous mild acid treatment （e.g. 0.01 mol/L of H2SO4）, ZFA can be used in the simultaneous removal of NH4＋ and P at low concentrations simulating real effluent.