酸沉降对缙云山湖水化学的影响

为了解我国典型酸雨区酸沉降时间变化特征以及对水化学特征的影响,利用2001—2020年东亚酸沉降监测网（EANET）的湿沉降与湖泊监测数据,使用MK检验分析缙云山酸沉降和湖水化学长期变化特征,使用Spearman相关系数明确酸沉降对湖水化学特征的影响。结果表明：2001—2020年,缙云山酸雨问题已得到改善,但降水pH值在3.94—5.15,平均值为4.41,酸雨问题依然严峻。硫和溶解无机氮（dissolved inorganic nitrogen,DIN）沉降通量分别为32.85 kg·hm⁻²·a⁻¹和22.55 kg·hm⁻²·a⁻¹,酸雨类型已由“硫酸型”转变为“硫酸-硝酸混合型”。湖水pH值的范围在5.25—7.50,平均值为5.86,酸化频率为30%。湖水pH值与降水pH值之间的相关性（r=0.56,P＜0.05）表明酸沉降对湖水酸化有一定作用。因此,对于酸化水体的治理须考虑大气沉降因素,只有协同治理大气污染才能根治水生生态系统的退化现象。     

丹江口水库淅川库区大气磷沉降特征

大气磷沉降是向地表水体输送营养元素的重要途径.以丹江口水库淅川库区为研究区,在库区周围设置了6个采样点,于2020年1—12月期间采集并分析了大气总磷干、湿沉降样品,探讨了总磷沉降的时空分布特征及其对库区水体外源磷输入的贡献.结果表明：研究区大气 总磷沉降量为1.19 kg·hm^-2·a^-1,其中,干沉降占比为49.73%,湿沉降占比为50.27%;总磷干、湿沉降量在空间上均具有显著差异性（p_s<0.05）, 湿沉降量在季节上具有极显著差异性（p<0.01）;总磷干沉降量受到气温、气压和风速的显著影响,湿沉降量受到降雨量的显著影响;总磷年沉降量为65.17 t·a^-1,占河流总磷入库量的42.18%.     

短期氮添加对黄山松林土壤碳组分的影响及其微生物机制

人类活动和大气沉降增加了陆地生态系统氮的输入,显著改变了生态系统碳循环.为了更好地理解氮沉降如何调节森林土壤有机碳组分动态,及其潜在的微生物机制.本研究在福建戴云山黄山松林设置3个氮添加梯度（对照（0 kg·hm^-2·a^-1）、低氮（40 kg·hm^-2·a^-1）、高氮（80 kg·hm^-2·a^-1） ）以模拟氮沉降.通过测定土壤基本理化性质、土壤微生物生物量、酶活性和碳利用效率,利用两步硫酸水解法将土壤有机碳分为量小、周转快的活性碳组分和量大、周转慢的惰性碳组分,以探究两年氮添加对亚热带黄山松土壤有机碳组分的影响.与对照相比,氮添加显著降低0~10 cm土壤活性碳组分含量,增加土壤惰性碳含量.氮添加提高了参与碳、氮和磷获取的3种水解酶活性（β-葡萄糖苷酶、β-N-乙酰氨基酸葡糖苷酶、酸性磷酸单酯酶）,并显著降低了土壤微生物碳利用效率.冗余分析和随机森林模型表明,土壤微生物碳利用效率、微生物生物量和β-葡萄糖苷酶是影响土壤碳组分变化的主要因子,且土壤微生物碳利用效率与活性碳呈显著正相关,与惰性碳呈显著负相关;微生物生物量碳与活性碳呈显著正相关,与惰性碳无显著关系.综上所述,土壤微生物生物量减少、碳利用效率的下降导致活性碳组分含量减少,而惰性碳组分含量增加,进而提高黄山松林土壤有机碳的稳定性.     

基于“质心”迁移的典型城市群氮排放-干沉降输送过程研究

含氮化合物的排放、输送和沉降是生物地球化学氮循环的关键过程，对生态系统和气候变化具有重要影响.其中输送过程的定量化表征一直是困扰沉降来源识别的突出难点之一.为此，本研究采用WRF-EMEP模型模拟2015年我国大气氮干沉降时空分布特征，通过标准差椭圆（SDE）"质心"迁移法定量分析京津冀地区（BTH）、长江三角洲（YRD）和珠江三角洲（PRD）3大典型城市群的氮排放-干沉降输送过程，评估不同区域大气氮干沉降输送过程的季节差异和影响因素.研究结果表明，我国典型城市群氮干沉降通量呈现出散布于城市群周边50~200 km地区的空间分布格局，其中氧化态氮（NO_y）和还原态氮（NH_x）沉降的年平均通量水平分别为8.5 （6.0~22.0） kg ·hm^-2·a^-1和10.2 （6.0~31.0） kg ·hm^-2·a^-1.氧化态氮和还原态氮的输送方向均受大气环流运动主导：在同一城市群，各季节氧化态氮和还原态氮的输送方向保持一致；在不同城市群，二者的输送方向具有季节性差异：京津冀地区氮沉降春秋冬三季多向东及东南方向迁移，夏季向南迁移；受西太平洋副热带反气旋环流影响，长三角地区春夏季氮沉降向西迁移；珠三角地区氮沉降在春夏季往偏北方向迁移，秋冬两季向西南方向迁移.氧化态氮和还原态氮的输送距离受其化学性质主导：在相同气象条件下，氧化态氮传输距离约为还原态氮传输距离的1~2倍，使得氧化氮多沉降在城市群的域外，而还原态氮主要沉降在排放源周边区域.其中，不同城市群氮沉降的输送距离有一定差异，除夏季外，京津冀地区（127~541 km）和长三角地区（108~374 km）的输送距离高于珠三角地区（57~285 km），其中京津冀地区和珠三角地区沉降主要在域外，即两地的氮排放更易输送到周边地区.因此，在开展氮沉降生态效应相关研究时，应关注周边地区对本地氧化态氮输送的影响.     

春季南海东沙岛硝酸盐干沉降通量、形成机制及其来源

硝酸盐是大气中主要的酸性离子,也是大气活性氮沉降主要的组成部分。中国目前对大气硝酸盐形成机制及其来源的研究主要集中在陆地区域,对海洋气溶胶的硝酸盐的形成机制及其来源的研究较少。本研究于2013年春季（3—5月）,在中国南海东沙岛共计采集了86个总悬浮颗粒（TSP）气溶胶样本,分析了TSP样品中NO₃⁻浓度、δ¹⁵N-NO₃⁻和δ¹⁸O-NO₃⁻值。结果表明：东沙岛春季TSP中浓度呈现逐月下降的趋势。基于浓度估算东沙岛春季NO₃⁻-N干沉降通量范围为(1.0±0.5)—(3.4±1.7) mg·d⁻¹·m⁻²（以N计,余同）。δ¹⁸O-NO₃⁻值在3月和4月（76.1‰±3.8‰和79.1‰±5.6‰）明显高于5月（67.0‰±7.5‰）,表明东沙岛3月和4月硝酸盐的形成路径不同于5月。贝叶斯同位素混合模型计算结果显示：N₂O₅参与的路径（N₂O₅+H₂O/Cl⁻和NO₃+VOCs）在3月和4月生成了37.2%和43.3%的硝酸盐,5月NO₂+OH路径是硝酸盐的主要形成路径,形成了80.2%的硝酸盐。δ¹⁵N-NO₃⁻值和气团后向轨迹表明,东沙岛春季不同月份TSP中NO₃⁻的来源不同,3月和4月以陆地源为主,5月主要受海洋源影响。     

不同水分管理方式下水稻生长季N2O排放量估算：模型验证和输入参数检验

利用2005～2007年我国稻田N₂O排放通量的田间原位测定资料和国际上其它地区稻田N₂O报道结果,对作者建立的不同水分管理方式下水稻生长季N₂O排放估算模型进行了验证. 结果表明,持续淹水稻田N₂O排放的拟合结果与其他地区淹水稻田N₂O通量值相一致. 淹水-烤田-淹水的水分管理方式下,稻田N₂O排放的拟合值接近于国际上同类研究结果. 淹水-烤田-淹水-湿润灌溉的水分管理方式下,稻田N₂O排放的估算模型对田间原位测定资料有很好的适切性. 为了检验模型输入参数的可信度,将本研究建立的有关我国水稻生产的相关资料数据库与以往研究报道结果进行了比较,结果表明,两者具有高度的一致性. 数据库资料表明,在20世纪50～70年代间,持续淹水稻田占20%～25%,大约75%～80%的稻田采用淹水-烤田-淹水的水分管理方式. 在20世纪80～90年代间,采用持续淹水,淹水-烤田-淹水和淹水-烤田-淹水-湿润灌溉水分管理方式的稻田分别约占12%～16%、 77%和7%～12%. 20世纪50年代水稻生长季平均每季总施氮量为87.49 kg·hm^-2,而90年代平均为224.64 kg·hm^-2. 其中,化学氮肥的施用量从20世纪50年代的37.4 kg·hm^-2增加到了90年代的198.8 kg·hm^-2,分别占水稻生长季氮输入总量的43%和88%. 在20世纪50～70年代间有机氮的输入量相对比较稳定,平均变幅在45.2～48.2 kg·hm^-2之间,随后逐步降低,有机肥料氮占氮输入总量的比例从20世纪50年代的52%降低到了90年代的9%. 作物残体N输入量从20世纪50年代的4.9 kg·hm^-2增加到了80年代的6.3 kg·hm^-2. 20世纪50～70年代水稻生长季氮肥施用量具明显的空间变异性,而80～90年代间其空间变异较小. 模型验证和输入参数检验的结果表明,该模型能较好地模拟我国不同水分管理方式下的稻田N₂O直接排放量.     

紫色土丘陵区农田源头沟渠一氧化氮排放的季节差异及影响因素

农田源头沟渠是农田养分迁移的重要水文通道和非常活跃的氮转化场所.本研究以紫色土丘陵区农田源头沟渠为对象,在2014年12月~2015年11月,采用静态箱-化学发光法对其一氧化氮（NO）排放开展原位观测.结果表明,有自然植被覆盖的农田源头沟渠生态系统（V）中的NO年累积排放量为14.17 g·（hm²·a）^-1,而无自然植被覆盖的对照处理（NV,代表沟渠中的沉积物-水界面系统）则为-0.4 g·（hm²·a）^-1.总体而言,沟渠生态系统的年综合排放通量是11.27 g·（hm²·a）^-1,全年平均排放通量为0.13 μg·（m²·h）^-1.农田源头沟渠仅在夏季是NO的排放源,且夏季NO累积排放量显著高于（P<0.05）春季、秋季或冬季.沟渠上覆水NO₃^--N浓度和温度是影响NO排放季节变化的主要控制因素.同时,沟渠生态系统中植物存在可显著提高所观测的NO排放通量,但对全年NO累积排放量无显著影响.     

·Cl引发α-蒎烯的大气氧化机制及动力学

α-蒎烯是大气中含量最丰富的单萜烯类挥发性有机化合物,与氯自由基（·Cl）反应是其重要的转化途径.然而,·Cl引发α-蒎烯大气氧化的分子机制尚不清楚.本研究采用量子化学计算与微观动力学模拟相结合的方法,研究了·Cl与α-蒎烯的引发反应以及引发反应生成的主要α-蒎烯自由基的后续转化机制与动力学.结果发现,·Cl反式加成到α-蒎烯的C₂位置生成加成中间体IM_1-9-a是最可行的反应途径.在298 K和1.013×10⁵ Pa条件下,计算得到·Cl与α-蒎烯的反应速率常数（k_Cl）为3.1×10^-10 cm³·molecule^-1·s^-1,与k_Cl的实验值（4.6±1.3）×10^-10 cm³·molecule^-1·s^-1一致.生成的IM_1-9-a进一步与O₂反应生成过氧自由基IM_3-1-a,在2.5×10⁹ cm^-3（100 ppt） NO和1.25×10⁹ cm^-3（50 ppt） HO₂·条件下,IM_3-1-a后续主要与NO和HO₂·反应生成有机硝酸酯（C₁₀H₁₆ClNO₃和C₁₀H₁₆ClNO₄）、氢过氧化物（C₁₀H₁₇ClO₂和C₁₀H₁₇ClO₃）和烷氧自由基（C₁₀H₁₆ClO₂·）.生成的 闭壳层产物与母体α-蒎烯相比具有较高的O∶C比,可能具有较低的蒸气压,进而贡献二次有机气溶胶.本研究结果可为全面评价α-蒎烯的 大气化学反应对大气质量的影响提供理论支撑.     

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%.     

基于实测的船舶辅机大气污染物排放量估算

于2017年3月—2018年5月在广州市南沙港区选取不同吨位的5艘船舶进行登船实测,建立了基于燃油消耗的排放因子.结果表明,船舶辅机CO₂排放因子为(3085±439)~(3195±121) g·kg^-1,CO排放因子为(5.50±1.33)~(26.10±8.90) g·kg^-1,TVOC排放因子为(0.29±0.02)~(1.68±0.06) g·kg^-1,PM_2.5排放因子为(0.56±0.09)~(12.50±3.11) g·kg^-1,NO_x排放因子为(19.20±4.12)~(83.30±11.80) g·kg^-1,基于燃油消耗量,估算2017年广州港船舶停泊工况辅助发动机SO₂、CO、TVOC、PM_2.5和NO_x排放总量分别为736、(794±209)、(46.40±2.39)、(223.0±49.4)和(3237±698) t.船舶引擎功率对排放CO、TVOC和PM_2.5影响显著,引擎功率较低的船舶以上3种大气污染物排放因子更高.从吨位而言,≥10000总吨的船舶对SO₂、CO、TVOC和NO_x 4种大气污染物的排放分担率均超过50%,≤2999总吨的船舶则对PM_2.5的排放分担率最高.从船舶类型而言,分担率最高的是集装箱船,分别占SO₂、CO、TVOC、PM_2.5和NO_x排放总量的43.8%、30.8%、41.4%、16.3%和40.9%,此外,散货船、其他货船、顶推拖船和油船对排放量的分担率也较高,以上5种船舶占到了各类大气污染物排放总量的90%.     

Toxic effects of acetochlor, methamidophos and their combination on nifH gene in soil

Toxic effects of two agrochemicals on nifH gene in agricultural black soil were investigated using denaturing gradient gel electrophoresis （DGGE） and sequencing approaches in a microcosm experiment. Changes of soil nifH gene diversity and composition were examined following the application of acetochlor, methamidophos and their combination. Acetochlor reduced the nifH gene diversity （both in gene richness and diversity index values） and caused changes in the nifH gene composition. The effects of acetochlor on nifH gene were strengthened as the concentration of acetochlor increased. Cluster analysis of DGGE banding patterns showed that nifH gene composition which had been affected by low concentration of acetochlor （50 mg/kg） recovered firstly. Methamidophos reduced nifH gene richness that except at 4 weeks. The medium concentration of methamidophos （150 mg/kg） caused the most apparent changes in nifH gene diversity at the first week while the high concentration of methamidophos （250 mg/kg） produced prominent effects on nifH gene diversity in the following weeks. Cluster analysis showed that minimal changes of nifH gene composition were found at 1 week and maximal changes at 4 weeks. Toxic effects of acetochlor and methamidophos combination on nifH gene were also apparent. Different nifH genes （bands） responded differently to the impact of agrochemicals： four individual bands were eliminated by the application of the agrochemicals, five bands became predominant by the stimulation of the agrochemicals, and four bands showed strong resistance to the influence of the agrochemicals. Fifteen prominent bands were partially sequenced, yielding 15 different nifH sequences, which were used for phylogenetic reconstructions. All sequences were affiliated with the alpha- and beta-proteobacteria, showing higher similarity to eight different diazotrophic genera.     

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.     

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.     

Arsenic uptake by arbuscular mycorrhizal maize （Zea mays L.） grown in an arsenic-contaminated soil with added phosphorus

The effects of arbuscular mycorrhizal (AM) fungus (Glomus mosseae) and phosphorus (P) addition (100 mg/kg soil) on arsenic (As) uptake by maize plants (Zea mays L.) from an As-contaminated soil were examined in a glasshouse experiment.Non-mycorrhizal and zero-P addition controls were included.Plant biomass and concentrations and uptake of As,P,and other nutrients,AM colonization,root lengths,and hyphal length densities were determined.The results indicated that addition of P significantly inhibited root colonization and development of extraradical mycelium.Root length and dry weight both increased markedly with mycorrhizal colonization under the zero-P treatments,but shoot and root biomass of AM plants was depressed by P application.AM fungal inoculation decreased shoot As concentrations when no P was added,and shoot and root As concentrations of AM plants increased 2.6 and 1.4 times with P addition,respectively.Shoot and root uptake of P,Mn,Cu,and Zn increased,but shoot Fe uptake decreased by 44.6%,with inoculation, when P was added.P addition reduced shoot P,Fe,Mn,Cu,and Zn uptake of AM plants,but increased root Fe and Mn uptake of the nonmycorrhizal ones.AM colonization therefore appeared to enhance plant tolerance to As in low P soil,and have some potential for the phytostabilization of As-contaminated soil,however,P application may introduce additional environmental risk by increasing soil As mobility.     

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.     

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.     

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.     

Potential of plant polyphenol oxidases in the decolorization and removal of textile and non-textile dyes

In this study an effort has been made to use plant polyphenol oxidases; potato （Solanum tuberosum） and brinjal （Solanum melongena）, for the treatment of various important dyes used in textile and other industries. The ammonium sulphate fractionated enzyme preparations were used to treat a number of dyes under various experimental conditions. Majority of the treated dyes were maximally decolorized at pH 3.0. Some of the dyes were quickly decolorized whereas others were marginally decolorized. The initial first hour was sufficient for the maximum decolorization of dyes. The rate of decolorization was quite slow on long treatment of dyes. Enhancement in the dye decolorization was noticed on increasing the concentration of enzymes. The complex mixtures of dyes were treated with both preparations of polyphenol oxidases in the buffers of varying pH values. Potato polyphenol oxidase was significantly more effective in decolorizing the dyes to higher extent as compared to the enzyme obtained from brinjal polyphenol oxidase. Decolorization of dyes and their mixtures, followed by the formation of an insoluble precipitate, which could be easily removed simply by centrifugation.     

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 heavy metals from sewage sludge by low costing chemical method and recycling in agriculture

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