大气汞氧化还原过程与机制的计算化学研究进展

大气中汞的氧化还原反应对于其全球生物地球化学循环起着极其重要的作用,它促进了汞在全球范围内的扩散.汞主要以气态元素汞的形态释放到大气中,并经历复杂的均相和非均相化学反应,被氧化为活性气态汞和颗粒态汞;同时,活性气态汞也可经过光致还原反应光解生成气态元素汞.计算化学是一种基于理论方法利用计算软件来对化学现象和本质进行解释...     

不同深度脱水污泥的热解特性及动力学分析

选用4种利于深度脱水的复合调理剂(FeCl3/CaO、FeCl3/CaO/煤粉、芬顿试剂(Fe2+和H2O2组成体系)/CaO、芬顿试剂CaO/煤粉)来改善污泥的脱水性能,所得泥饼的含水率为43.7%—56.1%,满足深度脱水的要求.CaO和煤粉的添加能改变污泥的灰分和挥发分含量.与传统聚丙烯酰胺(PAM)脱水污泥的热重分析对比结果表明,由于复合调理剂对EPS的破坏溶解作用,因此对污泥热解性质有较大影响,不仅能前移水分失重峰,还使得热重主要反应阶段峰个数变少.热解动力学计算表明,反应级数在1—2范围内.表观活化能差异表明4种复合调理剂处理后脱水污泥更容易发生热解反应.     

河北口岸进口煤炭中氟、氯、砷、汞、硫的整体特性和分布特征

对河北口岸进口的629批朝鲜、加拿大、俄罗斯和澳大利亚煤炭中灰分、硫、砷、汞、氟和氯元素含量进行了测定,研究了各进口国煤炭中各元素的分布特征,并通过相关性分析推断了各元素的赋存状态.采用稳健统计技术估算了河北进口煤整体样本中硫、砷、汞、氟和氯元素的代表值,采用主成分分析、聚类分析对整体样本进行了分类,采用因子分析确定了各元素的主要影响因子.结果表明,加拿大煤中砷元素含量明显偏高,硫元素分布较窄;朝鲜煤灰分和汞含量较高,汞主要以硫化物或硫化矿物的形式存在;俄罗斯煤中汞含量较高,主要存在于黏土矿物中,赋存状态复杂;澳大利亚煤中氯含量较高,汞元素主要为铝硅酸盐(黏土矿物).整体样本中硫、砷、汞、氟和氯元素的代表值依次为0.3%±0.208%、0.328±0.137μg·g~(-1)、6.56±3.432μg·g~(-1)、0.028%±0.014%和129.7±79.504μg·g~(-1),各元素含量整体水平较为平均,可区分为3个水平,主因子特征描述为Ash-Hg因子和S因子.     

外来入侵植物美洲商陆提取物的化感活性

研究了外来入侵植物美洲商陆(Phytolacca americana)提取物对黄花草木樨(Melilotus officinalis)、大白菜(Brassica pekinensis)、北美车前(Plantago virginica)和马唐(Digitaria sanguinalis)4种植物种子萌发和幼苗生长的影响。结果表明,与对照相比,1 000～4 000、4 000和2 000～4 000μg·mL-1美洲商陆醇提取物分别对大白菜、北美车前和马唐种子萌发率具有显著抑制作用,1 000～4 000μg.mL-1水提取物对马唐种子萌发率也具有显著抑制作用,最大抑制率分别为32.22%、46.56%、32.69%和28.57%。250～500μg·mL-1醇提取物和250～4 000μg·mL-1水提取物对黄花草木樨幼苗根长,250～1 000μg·mL-1醇提取物和250～4 000μg·mL-1水提取物对黄花草木樨幼苗苗高,以及500μg·mL-1水提取物对黄花草木樨幼苗干质量均具有显著促进作用,最大促进率分别为21.32%、37.89%、12.94%、32.07%和18.81%。1 000～4 000μg·mL-1醇提取物和4 000μg·mL-1水提取物对大白菜幼苗根长,2 000～4 000μg·mL-1醇提取物和水提取物对大白菜幼苗苗高,4 000μg·mL-1水提取物对大白菜幼苗干质量具有显著抑制作用,最大抑制率分别为37.00%、20.95%、25.63%、22.30%和13.67%。250～1 000μg·mL-1水提取物对北美车前幼苗根长,250～4 000μg·mL-1水提取物对北美车前苗高具有显著促进作用,而1 000～4 000μg·mL-1醇提取物对北美车前幼苗根长,4 000μg·mL-1醇提取物对北美车前苗高和干质量具有显著抑制作用,最大抑制率分别为58.06%、29.72%和18.36%。500～4 000、1 000～4 000和2 000～4 000μg·mL-1醇提取物分别对马唐幼苗根长、苗高及干质量,4 000μg·mL-1水提取物对马唐幼苗根长具有显著抑制作用,最大抑制率分别为70.31%、44.65%、42.43%和35.50%。由此可见,美洲商陆对大白菜、北美车前和马唐种子萌发和幼苗生长具有较强的化感抑制作用,对入侵植物黄花草木樨具有化感促进作用,这些都直接或间接地增强了美洲商陆的入侵性。     

燃煤烟气中汞形态分析的实验研究

在一维煤粉燃烧炉台架上采用EPA推荐的Ontario Hydro方法 ,测量了燃烧不同煤种排放的烟气中汞的形态分布情况 .结果表明 ,烟气中汞以颗粒态和气态汞的形式存在 .气态汞总量在 9— 2 3 μg·Nm- 3范围内 ,主要以单质汞的形式存在 ,占气态汞总量的 5 2 %—83 % ,而二价汞占 1 7%— 48% .飞灰中汞的浓度大大超过了底灰中汞的浓度 ,表明汞在飞灰中富集 ,在底灰中分散的行为     

淮南燃煤电厂汞分配、富集与释放通量

汞是一种环境有害元素,燃煤汞排放业已成为当今中国最主要的汞污染源.有效的汞减排政策的制定需要准确了解煤中汞在煤炭燃烧过程中的分配规律及富集模式.本研究针对淮南燃煤电厂的原煤、飞灰、脱硫石膏和脱硫废水进行分析,研究发现,灰渣中的汞含量最低(9.8—27 ng·g~(-1)),其相对于原煤汞(约450 ng·g~(-1))的富集系数一般小于2.1%;飞灰中汞的含量相对较高(121—700 ng·g~(-1)),其富集系数介于9%—54%;而脱硫石膏中汞的浓度最高(1489—4589 ng·g~(-1)).通过物料平衡原理,计算出汞在各个燃煤产物中的分配如下:底灰占1%;飞灰占24%—32%;脱硫石膏及废渣液占7%—22%;大气排放占54%—64%.静电除尘器的脱汞效率为24%—32%,接近世界平均值;而脱硫装置的脱汞效率较低,为10%—29%.根据本研究的汞释放系数(0.24—0.29 g Hg·t~(-1)coal),计算出该电厂在2003—2010年的汞排放通量为1.8—7.3 t.本研究认为燃烧前原煤汞脱除,以及加大对现有脱硫装置的改造能够有效降低大气汞排放.     

常温常压KBH4还原法快速脱除水煤浆中的硫

使用KBH4还原法脱除水煤浆中的硫.在常温常压,KBH4浓度为2.0 mmol.L-1、煤炭粒径109μm、处理时间10 min、搅拌速度为200 r.min-1的条件下,低硫水煤浆中煤炭的总脱硫率可以达到43.0%.而且硫酸盐硫的脱除率约47.8%,黄铁矿硫的脱除率约55.4%;同时有机硫的脱除率约23.9%.硼氢化钾还原法相比其它传统化学脱硫方法,对有机硫和无机硫脱除均有作用,试剂用量少,反应条件温和,脱硫速度快,热值的损耗小,处理后水煤浆中煤炭的热值有所提高,起燃温度降低.     

高灵敏黄曲霉毒素B1酶联免疫试剂盒的研制及应用

为实现对环境及食品样品中黄曲霉毒素B1的高灵敏检测,通过优化一系列试剂盒参数,研制了一步间接竞争ELISA检测试剂盒.优化后的包被缓冲液为90 mmol·L-1、pH 4.6的柠檬酸缓冲液,最佳反应pH值为7.4,抗体包被浓度为0.2μg·m L-1,HRP-BSA-AFB1稀释比为1/4000,标品稀释液为含7%甲醇的PBST溶液.优化后试剂盒IC50值为66 pg·m L-1,检测限为7.6 pg·m L-1,检测线性范围为10—810 pg·m L-1.试剂盒对不同AFB1添加水平(0.5μg·kg-1,1μg·kg-1)的玉米、豆粕和鱼粉样品平均回收率为108.4%—134.8%.对玉米、豆粕和鱼粉样品各20份盲样测试结果表明,试剂盒检测结果与HPLC-MS/MS检测结果吻合.     

可见光下苯醌类化合物诱导磷酸铁芬顿反应的铁离子源汇机制

构建了可见光下苯醌类化合物诱导磷酸铁产生芬顿反应的体系,分析了苯醌类化合物对磷酸铁释放亚铁离子的影响,比较了苯醌类化合物诱导磷酸铁芬顿反应降解橙Ⅱ的效率,研究了橙Ⅱ降解过程中铁离子和亚铁离子之间的转化以及羟基自由基浓度的变化,讨论了可见光下苯醌类化合物诱导磷酸铁芬顿反应铁离子的源汇机制.结果表明,可见光下苯醌类化合物诱导的磷酸铁是芬顿反应铁离子的间接铁源和直接铁汇.当可见光-磷酸铁-过氧化氢体系分别添加2-氯-1,4-苯醌、苯醌和对二甲基醌,溶液中亚铁离子浓度峰值(对应时间)从基础实验的0.86 mg·L^-1 (120 min)分别提高到2.06 mg·L^-1 (40 min)、1.61 mg·L^-1 (40 min)和1.04 mg·L^-1 (120 min);铁离子引发的芬顿反应能极大提高橙Ⅱ的脱色率和矿化率：反应60 min时,橙Ⅱ脱色率分别是99.5%、98.1%和77.7%;反应180 min时,橙Ⅱ矿化率分别为78.8%、77.6%和52.4%;反应结束时,总铁离子的浓度会大幅降低至0....     

气升式反应器中微生物对H2S的脱除研究

筛选驯化得到具有高效脱硫性能的菌群,在气升式反应器中进行了H2S脱除实验研究. 在温度为28 ℃、初始pH 8.0的条件下考察了不同通气量对反应体系中H2S脱除能力、脱除效率的影响以及H2S进气负荷和通气量对SO2-4生成率的影响. 结果表明,最佳通气量为0.2 L/min.在此通气量下,当H2S进气负荷为5.76 kg m-3 d-1时,脱除负荷可达5.62 kg m-3 d-1,而脱除率可以保持在97.8%以上;当H2S负荷为4.37～4.93 kg m-3 d-1时, H2S去除率可达到99%以上,且主要副产物为单质硫.通过增大进气负荷、降低通气量可以获得较高的单质硫回收率.图3表2参15     

Achieving Open Access to Conservation Science

Conservation science is a crisis discipline in which the results of scientific enquiry must be made available quickly to those implementing management. We assessed the extent to which scientific research published since the year 2000 in 20 conservation science journals is publicly available. Of the 19,207 papers published, 1,667 (8.68%) are freely downloadable from an official repository. Moreover, only 938 papers (4.88%) meet the standard definition of open access in which material can be freely reused providing attribution to the authors is given. This compares poorly with a comparable set of 20 evolutionary biology journals, where 31.93% of papers are freely downloadable and 7.49% are open access. Seventeen of the 20 conservation journals offer an open access option, but fewer than 5% of the papers are available through open access. The cost of accessing the full body of conservation science runs into tens of thousands of dollars per year for institutional subscribers, and many conservation practitioners cannot access pay‐per‐view science through their workplace. However, important initiatives such as Research4Life are making science available to organizations in developing countries. We urge authors of conservation science to pay for open access on a per‐article basis or to choose publication in open access journals, taking care to ensure the license allows reuse for any purpose providing attribution is given. Currently, it would cost $51 million to make all conservation science published since 2000 freely available by paying the open access fees currently levied to authors. Publishers of conservation journals might consider more cost effective models for open access and conservation‐oriented organizations running journals could consider a broader range of options for open access to nonmembers such as sponsorship of open access via membership fees. Obtención de Acceso Abierto a la Ciencia de la Conservación     

Rapid,recurring, structured survey versus bioblitz for generating biodiversity data and analysis with a multispecies abundance model

A bioblitz inexpensively and quickly generates biodiversity data, but bioblitzes are often conducted with haphazard, unreplicated sampling. Results tend to be taxonomically, geographically, or temporally biased, lack metadata, and consist of lists of observed taxa that do not enable further analyses or correction for imperfect detection. A rapid, recurring, structured survey (RRSS) uses a structured sampling design and temporal and spatial replication to survey randomly selected sites on a conservation property. We participated in a loosely structured bioblitz and a subsequent RRSS at Big Canoe Creek Nature Preserve in Springville (St. Clair County), Alabama (USA) to compare observed richness derived from the 2 survey approaches. The RRSS data structure enabled us to fit models that accounted for imperfect detection to estimate abundances, occupancy probabilities, and habitat associations. The loosely structured bioblitz data could not be used in such models. We present a new integrated multispecies abundance model that we applied to avian RRSS data. Our model extension enables estimation for the community, employs data augmentation to estimate the number of undetected species, and incorporates covariates. The RRSS generated a more comprehensive and less biased list of observed taxonomic richness than the loosely structured bioblitz (e.g., 73 vs. 45 bird species and 104 vs. 63 insect families from the RRSS vs. loosely structured bioblitz, respectively). Models fit to the RRSS data identified seasonal patterns in avian community composition and allowed for estimation of habitat–occupancy relationships for insect taxa. The RRSS protocol has potential for broad transferability as a standardized, quick, and inexpensive way to inventory biodiversity and estimate ecological parameters while providing an outreach opportunity.     

Compliance with and ecosystem function of biodiversity offsets in North American and European freshwaters

Land-use change via human development is a major driver of biodiversity loss. To reduce these impacts, billions of dollars are spent on biodiversity offsets. However, studies evaluating offset project effectiveness that examine components such as the overall compliance and function of projects remain rare. We reviewed 577 offsetting projects in freshwater ecosystems that included the metrics project size, type of aquatic system (e.g., wetland and creek), offsetting measure (e.g., enhancement, restoration, and creation), and an assessment of the projects’ compliance and functional success. Project information was obtained from scientific and government databases and gray literature. Despite considerable investment in offsetting projects, crucial problems persisted. Although compliance and function were related to each other, a high level of compliance did not guarantee a high degree of function. However, large projects relative to area had better function than small projects. Function improved when projects targeted productivity or specific ecosystem features and when multiple complementary management targets were in place. Restorative measures were more likely to achieve targets than creating entirely new ecosystems. Altogether the relationships we found highlight specific ecological processes that may help improve offsetting outcomes.     

Some polyphagous Homoptera gain protection from their natural enemies by feeding on the toxic plantsSpartium junceum andErythrina corallodendrum (Leguminosae)

Summary Interactions were studied among alkaloid-containing legumes (Erythrina corallodendrum andSpartium junceum) and non-toxic plants (Citrus sinensis, Cucurbita moschata andEuphorbia tirucalli), several polyphagous homopterans,Aphis craccivora (Aphididae),Icerya purchasi, I. aegyptiaca (Margarodidae),Lepidosaphes ulmi (Diaspididae) andPlanococcus citri (Pseudococcidae), and some major natural enemies of these homopterans. Significant reductions in survival due to negative effects of alkaloid containing as compared with non-alkaloidal plants were recorded for the predatorsRodolia cardinalis andChilocorus bipustulatus, but not forCryptolaemus montrouzieri (Coleoptera: Coccinellidae),Chrysoperla carnea (Neuroptera: Chrysopidae) andSympherobius sanctus (Neuroptera: Sympherobiidae). The development time of the larvae or pupae ofR. cardinalis, C. carnea andS. sanctus was longer on the toxic plants than on the non-toxic ones. The percentage of parasitism ofA. craccivora collected from the non-alkaloidal plantsVicia palaestina andMelilotus albus was much higher than that onS. junceum. The parasitoid complexes ofA. craccivora differed between both plant groups. The nutritive value of honeydew ofI. purchasi andA. craccivora, as expressed by the life span ofEncyrtus infelix (Hymenoptera: Encyrtidae) adults, was also investigated. Life spans were significantly longer when the wasps fed on honeydew produced on non-alkaloidal plants (C. sinensis andPittosporum tobira) than on alkaloid containing plants whenI. purchasi — but notA. craccivora — was the producer. It is suggested that the chemical defense ofE. corallodendrum andS. junceum is exploited by polyphagous phytophages to reduce predation. In nature, population growth and density of four of the investigated homopterans are conspicuously high when they developed on the alkaloid containing plant species, and very low on non-alkaloid plants. The efficiency of their natural enemies may be reduced by sequestration of alkaloids (or other toxic plant compounds) or their transfer into excreted honeydew. Therefore it is assumed that a generalist phytophagous homopteran may be protected from its natural enemies, although at different rates of efficiency, if it can safely sequester the host allelochemical when it develops on toxic species within its host range.     

A palaeo-hydrogeological model for arsenic contamination in southern and south-east Asia

An argument is presented in which areas of natural arsenic contamination of modern groundwaters throughout Asia have a common origin. Arsenic originally accumulated in oceanic ferro-manganoan sediments of the eastern Palaeo-Tethys. This was further concentrated through oceanic crustal extinction in what later became the south-east Chinese accreted mineralised terrain. Proto-Himalayan uplift of this area created the palaeo-drainage systems of the Ganges – Brahmaputra, Irrawaddy, Mekong, and Red Rivers, with consequent headwater erosion of arsenic-rich sediments. Their downstream deposition as immature and easily redistributed Neogene sandstones, silts, and iron-rich clays has created secondary and tertiary reservoirs of adsorbed and authigenic arsenic, from which the current arsenic-rich groundwaters have evolved. Considering river basins within the above palaeo-hydrogeological framework provides a basis for assessing the risk of arsenic in groundwater basins of south and south-eastern Asia.     

Sequestration of cucurbitacin analogs by New and Old World chrysomelid leaf beetles in the tribe Luperini

Summary Two South American polyphagous leaf beetles,Diabrotica speciosa andCerotoma arcuata, selectively accumulated the bitter tasting compound 23,24-dihydrocucurbitacin D in their body after ingesting root tissues of cucurbit plants. Similarly, three Asian Cucurbitaceae-feeding specialists in the genusAulacophora were found to sequester the same compound. Cucurbitacin analogs were shown to deter feeding by a bird predator, indicating an allomonal role for these compounds in cucurbitacin-associated chrysomelid leaf beetles both of New and Old Worlds. The strong affinity to cucurbitacins, selective sequestration of the analogs and consequent protection from predators suggested an ecological adaptation mechanism developed in common among these two geographically isolated subtribes in the Luperini.     

Threats to intact tropical peatlands and opportunities for their conservation

Large, intact areas of tropical peatland are highly threatened at a global scale by the expansion of commercial agriculture and other forms of economic development. Conserving peatlands on a landscape scale, with their hydrology intact, is of international conservation importance to preserve their distinctive biodiversity and ecosystem services and maintain their resilience to future environmental change. We explored threats to and opportunities for conserving remaining intact tropical peatlands; thus, we excluded peatlands of Indonesia and Malaysia, where extensive deforestation, drainage, and conversion to plantations means conservation in this region can protect only small fragments of the original ecosystem. We focused on a case study, the Pastaza‐Marañón Foreland Basin (PMFB) in Peru, which is among the largest known intact tropical peatland landscapes in the world and is representative of peatland vulnerability. Maintenance of the hydrological conditions critical for carbon storage and ecosystem function of peatlands is, in the PMFB, primarily threatened by expansion of commercial agriculture linked to new transport infrastructure that is facilitating access to remote areas. There remain opportunities in the PMFB and elsewhere to develop alternative, more sustainable land‐use practices. Although some of the peatlands in the PMFB fall within existing legally protected areas, this protection does not include the most carbon‐dense (domed pole forest) areas. New carbon‐based conservation instruments (e.g., REDD+, Green Climate Fund), developing markets for sustainable peatland products, transferring land title to local communities, and expanding protected areas offer pathways to increased protection for intact tropical peatlands in Amazonia and elsewhere, such as those in New Guinea and Central Africa which remain, for the moment, broadly beyond the frontier of commercial development.     

Effects of Controlled Fire and Livestock Grazing on Bird Communities in East African Savannas

Abstract: In East Africa fire and grazing by wild and domestic ungulates maintain savannas, and pastoralists historically set fires and herded livestock through the use of temporary corrals called bomas. In recent decades traditional pastoral practices have declined, and this may be affecting biodiversity. We investigated the effects of prescribed fires and bomas on savanna bird communities in East Africa during the first and second dry seasons of the year (respectively before and after the rains that mark the onset of breeding for most birds). We compared abundance, richness, and community composition on 9‐ha burned plots, recently abandoned bomas, and control plots in the undisturbed matrix habitat over a 3‐year period. Generally, recently burned areas and abandoned bomas attracted greater densities of birds and had different community assemblages than the surrounding matrix. The effects of disturbances were influenced by interactions between primary productivity, represented by the normalized difference vegetation index, and time. Bird densities were highest and a greater proportion of species was observed on burned plots in the months following the fires. Drought conditions equalized bird densities across treatments within 1 year, and individuals from a greater proportion of species were more commonly observed on abandoned bomas. Yearly fluctuations in abundance were less pronounced on bomas than on burns, which indicate that although fire may benefit birds in the short term, bomas may have a more‐lasting positive effect and provide resources during droughts. Several Palearctic migrants were attracted to burned plots regardless of rainfall, which indicates continued fire suppression may threaten their already‐declining populations. Most notably, the paucity of birds observed on the controls suggests that the current structure of the matrix developed as a result of fire suppression. Traditional pastoralism appears critical to the maintenance of avian diversity in these savannas.     

Cost‐effective conservation of an endangered frog under uncertainty

How should managers choose among conservation options when resources are scarce and there is uncertainty regarding the effectiveness of actions? Well‐developed tools exist for prioritizing areas for one‐time and binary actions (e.g., protect vs. not protect), but methods for prioritizing incremental or ongoing actions (such as habitat creation and maintenance) remain uncommon. We devised an approach that combines metapopulation viability and cost‐effectiveness analyses to select among alternative conservation actions while accounting for uncertainty. In our study, cost‐effectiveness is the ratio between the benefit of an action and its economic cost, where benefit is the change in metapopulation viability. We applied the approach to the case of the endangered growling grass frog (Litoria raniformis), which is threatened by urban development. We extended a Bayesian model to predict metapopulation viability under 9 urbanization and management scenarios and incorporated the full probability distribution of possible outcomes for each scenario into the cost‐effectiveness analysis. This allowed us to discern between cost‐effective alternatives that were robust to uncertainty and those with a relatively high risk of failure. We found a relatively high risk of extinction following urbanization if the only action was reservation of core habitat; habitat creation actions performed better than enhancement actions; and cost‐effectiveness ranking changed depending on the consideration of uncertainty. Our results suggest that creation and maintenance of wetlands dedicated to L. raniformis is the only cost‐effective action likely to result in a sufficiently low risk of extinction. To our knowledge we are the first study to use Bayesian metapopulation viability analysis to explicitly incorporate parametric and demographic uncertainty into a cost‐effective evaluation of conservation actions. The approach offers guidance to decision makers aiming to achieve cost‐effective conservation under uncertainty.