用扫描电镜技术识别广州市大气颗粒物主要种类

利用扫描电镜技术对大气颗粒物的来源进行识别，采取手动分析与自动分析两种方法，得出的结果在总趋势上相互一致。手动方法和自动方法各有特点。自动分析在细颗粒，特别是含硫颗粒分析方面有优势，而手动分析在形貌观测和确定有机粗颗粒污染状况方面有独到之处。实验结果表明，大气颗粒物的来源是多样的，治理措施也应是综合性的，既要注意工业点源的污染治理和排放控制，如燃煤飞灰，钙质颗粒富铁颗粒等，也要注意面源排放，如土壤扬尘和碳质颗粒，碳质颗粒的来源复杂，可以是工业过程，燃烧过程，机动车尾气，生物质燃，树木自然排放。     

Water migration coefficients of chemical elements in the hypergenesis zone

The contents of basic salt components in the continental discharge related to weathering processes were calculated taking into account the atmospheric transfer of soluble salts from the ocean and their supply from anthropogenic sources. Real water migration coefficients characterizing the mobility of chemical elements in the hypergenesis zone were calculated on the basis of these data. It has been shown that the water migration coefficient directly depends on the solubility of basic minerals that are stable in the hypergenesis zone.     

Mineralogical evidence for a local volcanic origin of the parent material of Bermuda Quaternary paleosols

The alternation of carbonate deposits and paleosols compose the emerged part of the Bermuda archipelago. The pedological units present a complex and diversified mineralogy. Former studies demonstrated that the paleosols are not primarily a product of the unique dissolution of the surrounding carbonates, but contain a massive input of allochthonous non-carbonate detrital material. Researchers during more than the past three decades have attributed this flux of insoluble residues (IR) to Saharan dusts. We carried out systematic field and mineralogical analyses on the Quaternary paleosols from the Bermuda archipelago. Their mineralogical assemblage predominantly includes carbonates, clay minerals (kaolinite, chlorite and chlorite/vermiculite), phosphates, and aluminium and iron oxides/hydroxides. This assemblage is strikingly close to the mineralogy of the weathered volcanic substrate of Bermuda, but noticeably different from the mineralogy of Saharan dust. Moreover, we found volcanic lithoclasts in numerous paleosol profiles all over the archipelago and in all the recorded time intervals. We thus consider the volcanic seamount underlying Bermuda as the main source of non-carbonate minerals detected in the paleosols. This hypothesis further resolves the anomalous maturity of Bermudan paleosols compared to their southern counterparts in the Bahamas and Barbados.     

Atmospheric Deposition Connected with Marine Primary Production,Nitrogen Cycle: A Review

Atmospheric Deposition (AD) provides external nutrients such as nitrogen (N), phosphorus (P) and iron (Fe) supporting the growth of phytoplankton in oceans and thereby exerts obvious impacts on carbon and nitrogen cycles and climate change associated. Specifically, the external nutrients derived from atmospheric deposition can promote the marine primary production and nitrogen fixation that enhance the ocean capacity in absorbing CO₂; AD may also change a few pathways of carbon and nitrogen cycles in oceans and increase the emissions of biogenic aerosol and radioactive gases such as N₂O, DMS, etc. Due to the underlying important impacts on climate and environmental change, AD and processes related have become the hot topics of multidisciplinary studies in the areas of ocean and atmospheric sciences, and the focus of some international core projects such as Surface Ocean Lower Atmosphere Study (SOLAS), an International Study of Marine Biogeochemical Cycles of Trace Elements and Their Isotopes (GEOTRACES) and Integrated Marine Biogeochemistry and Ecosystem Research (IMBER). With the severe air pollution and high frequencies of Asian dust events, as the downwind areas of big cities and dust sources, the East China Sea and adjacent North Pacific have received increasing influences of AD. Limited studies showed that the increase of AD indeed caused significant influence on carbon and nitrogen cycles in these immediately related oceanic areas and the study there would have a signature effect on global oceans. A multidisciplinary study on the impacts of AD in oceans, e.g., combing molecular biology and experimental ecology techniques to study primary production processes, utilizing isotopic techniques to trace the change of the nitrogen cycle, new evidences of ocean-biogenic aerosol emissions, etc. would be the focus in the future.     

Assessing the microped size distributions of desert soils erodible by wind

The microped size distribution of erodible soils is one of the main factors controlling the emissions of mineral aerosol. To date, the microped size distributions of desert soils in natural field conditions are not well known and thus the existing dust source models cannot be applied to natural sites. Based on dry sieving and elemental analysis of 26 soil samples collected in arid and semiarid regions, it is shown that the microped size distributions of these desert soil samples involve a combination of four major mass size populations. These four size populations correspond to salty soils, fine quartz sand, coarse dune sand and aluminosilicate silt. We show that the microped size distributions of the various desert soils, according to their mineralogical characteristics, can be calculated by a mixture involving two or three of these four populations. The main field of application for this scheme is the characterization of the erodible soil size distributions for modelling the atmospheric dust cycle.     

Carbonyl Sulfide (COS) in the Surface Ocean and the Atmospheric COS Budget

Carbonyl sulfide (COS) mixing ratioswere measured in the marine atmosphere and in airequilibrated with surface sea water during severalcruises in the North Sea and western NorthAtlantic. In April 1994, North Sea waters weresupersaturated with respect to the atmosphere,resulting in oceanic emissions of COS. Saturationratios varied between the equilibrium value of one inthe central North Sea and high values of >15 in theElbe Estuary. We observed weak diel cycles of surfacewater COS during a three day drift station. During theunderway parts of the cruise, diel COS variations weremasked by the high geographical variability of COSconcentrations in the German Bight. In August 1994, weobserved a pronounced diel cycle of COS off theFlorida coast with saturation ratios varying betweenthe equilibrium value of one in the early morning andmaximum values of four to five in the afternoon. InMarch 1995, we found COS supersaturation as well asextensive undersaturation in the western NorthAtlantic between Norfolk, VA, and Bermuda. Suchundersaturation in marine surface waters results inregional and seasonal uptake of atmospheric COS. Basedon our data and those of other researchers, weestimate the global oceanic COS net emission to bebetween 1.3 and 2.5 Gmol yr^-1. This estimate is significantly smaller than previous ones which had notconsidered the possibility of COS uptake by theoceans. COS hydrolysis in the ocean has a significantinfluence on the atmospheric turnover time of COS,which we estimate to be 5.7 yr. This may contribute tothe lack of an observable increase in atmospheric COSlevels despite substantial anthropogenic emissions. This revised version was published online in July 2006 with corrections to the Cover Date.     

大气降尘TEM观察及其环境矿物学意义

在X射线衍射等分析研究基础上，进一步用透射电镜对半封闭室内长期沉积的大气降尘进行观察，提供了合肥地区大气降尘物相组成和各种物相形貌特征信息，揭示合肥地区大气污染物来源占第1位的是地表扬尘，以粘土矿物为标志；占第2位的是来源于大气化学次生气溶胶，主要和SO2、CO2、NOx等气态污染物排放有关，以石膏、碳酸盐和易溶盐类为标志；占第3位的是来源于汽车尾气排放的烟尘，以炭球为标志；占第4位的是来源于燃煤烟尘排放，以球形玻璃珠为特征。TEM调查不仅为合肥地区大气气溶胶颗粒成因、城市大气污染物来源和污染控制对策提供准确资料和依据，而且为确定大气颗粒物来源提供了有效研究方法和物源判别标志。     

Hafnium and neodymium isotopes in surface waters of the eastern Atlantic Ocean: Implications for sources and inputs of trace metals to the ocean

We present hafnium (Hf) and neodymium (Nd) isotopic compositions and concentrations in surface waters of the eastern Atlantic Ocean between the coast of Spain and South-Africa. These data are complemented by Hf and Nd isotopic and concentration data, as well as rare earth element (REE) concentrations, in Saharan dust.Hafnium concentrations range between a maximum of 0.52 pmol/kg in the area of the Canary Islands and a minimum value of 0.08 pmol/kg in the southern Angola Basin. Neodymium concentrations also show a local maximum in the area of the Canary Islands (26 pmol/kg) but are even higher between ∼20°N and ∼4°N reaching maximum concentrations of 35 pmol/kg. These elevated concentrations provide evidence of inputs from weathering of the Canary Islands and from the partial dissolution of dust from the Sahara/Sahel region. The inputs from ocean island weathering are also reflected in radiogenic Hf and Nd isotopes.The Hf isotopic compositions of dust samples themselves are highly variable, ranging between ε_Hf = −20 and −0.6. The combined Hf and Nd isotopic compositions of dust plot close to the “terrestrial array” during periods of appreciable dust load in the atmosphere. During low atmospheric dust loading combined Hf and Nd isotopic compositions similar to seawater are observed. Most of the variability can be explained in terms of variable degrees of zircon loss from the dust samples, which in turn is linked to sorting during atmospheric transport to the eastern Atlantic Ocean and possibly presorting by sedimentary redistribution on the continent. In addition, increasing relative proportions of radiogenic clay minerals with decreasing grain size may contribute to the radiogenic Hf isotopic compositions observed.While the Nd isotopic composition in the surface ocean reflects the Nd isotopic composition of the Saharan dust adjacent to the Sahara/Sahel region, the release of Hf from that dust appears to be incongruent and results in surface ocean Hf isotopic compositions which are ∼10 ε_Hf more radiogenic than the bulk dust. Radiogenic Hf appears to be released from clays and possibly from trace apatite. Rare earth element patterns of dust samples indicate the presence of apatite but provide no evidence for ferromanganese grain coatings, suggesting that such coatings are insignificant in the release of Hf and Nd from Saharan dust to the surface ocean.The Nd isotopic composition of the surface waters becomes less radiogenic south of the equator, most likely reflecting the release of Nd from Congo river sediments. The release of Hf from Saharan dust and the Congo river sediments, however, does not produce distinct Hf isotopic signatures in the surface ocean, implying that the mobile fraction of Hf integrated over large continental areas is isotopically uniform. The Hf isotopic uniformity in the surface ocean means that the limited variability in deep water isotopic compositions is consistent with a short deep water residence time and reflects homogenous continental inputs rather than efficient deep water homogenization.     

Modifications in aerosol physical,optical and radiative properties during heavy aerosol events over Dushanbe,Central Asia

The location of Central Asia,almost at the center of the global dust belt region,makes it susceptible for dust events.The studies on atmospheric impact of dust over the region are very limited despite the large area occupied by the region and its proximity to the mountain regions(Tianshan,Hindu Kush-Karakoram-Himalayas,and Tibetan Plateau).In this study,we analyse and explain the modification in aerosols'phys-ical,optical and radiative properties during various levels of aerosol loading observed over Central Asia utilizing the data collected during 2010-2018 at the AERONET station in Dushanbe,Tajikistan.Aerosol epi-sodes were classified as strong anthropogenic,strong dust and extreme dust.The mean aerosol optical depth(AOD)during these three types of events was observed a factor of～3,3.5 and 6.6,respectively,higher than the mean AOD for the period 2010-2018.The corresponding mean fine-mode fraction was 0.94,0.20 and 0.16,respectively,clearly indicating the dominance of fine-mode anthropogenic aerosol during the first type of events,whereas coarse-mode dust aerosol dominated during the other two types of events.This was corroborated by the relationships among various aerosol parameters(AOD vs.AE,and EAE vs.AAE,SSA and RRI).The mean aerosol radiative forcing(ARF)at the top of the atmosphere(ARFTOA),the bottom of the atmosphere(ARFBOA),and in the atmosphere(ARFATM)were-35±7,-73±16,and 38±17 Wm-2 during strong anthropogenic events,-48±12,-85±24,and 37±15 Wm-2 during strong dust event,and-68±19,-117±38,and 49±21 Wm-2 during extreme dust events.Increase in aerosol loading enhanced the aerosol-induced atmospheric heating rate to 0.5-1.6 K day-1(strong anthropogenic events),0.4-1.9 K day-1(strong dust events)and 0.8-2.7 K day 1(extreme dust events).The source regions of air masses to Dushanbe during the onset of such events are also identified.Our study con-tributes to the understanding of dust and anthropogenic aerosols,in particular the extreme events and their disproportionally high radiative impacts over Central Asia.     

Clues from Current High CO2 Environments on the Effects of Ocean Acidification on CaCO3 Preservation

Acidification of surface seawater owing to anthropogenic activities has raised serious concerns on its consequences for marine calcifying organisms and ecosystems. To acquire knowledge concerning the future consequences of ocean acidification (OA), researchers have relied on incubation experiments with organisms exposed to future seawater conditions, numerical models, evidence from the geological record, and recently, observations from aquatic environments exposed to naturally high CO₂ and low pH, e.g., owing to volcanic CO₂ vents, upwelling, and groundwater input. In the present study, we briefly evaluate the distribution of dissolved CO₂–carbonic acid parameters at (1) two locations in the Pacific and the Atlantic Ocean as a function of depth, (2) a mangrove environment in Bermuda, (3) a seasonally stratified body of water in a semi-enclosed sound in Bermuda, and (4) in temporarily isolated tide pools in Southern California. We demonstrate that current in situ conditions of seawater pCO₂, pH, and CaCO₃ saturation state (Ω) in these environments are similar or even exceed the anticipated changes to these parameters in the open ocean over the next century as a result of OA. The observed differences between the Pacific and Atlantic Oceans with respect to seawater CO₂–carbonic acid chemistry, preservation of CaCO₃ minerals, and the occurrence and distribution of deep-sea marine calcifiers, support the hypothesized negative effects of OA on the production and preservation of CaCO₃ in surface seawater. Clues provided from shallow near-shore environments in Bermuda and Southern California support these predictions, but also highlight that many marine calcifiers already experience relatively high seawater pCO₂ and low pH conditions.     

大气有机氮沉降及其对海洋生态系统的影响

有机氮是大气中含氮物质的重要组成部分。大气中有机氮化合物的种类繁多,按其存在的形态可分为：氧化型、还原型以及生物/颗粒型有机氮,这些有机氮可来自自然源和人为源的直接释放,也可来自于无机氮与碳氢化合物间的大气化学反应。大气有机氮对海洋的输入不仅可以促进海洋初级生产力的增长、进而增加二氧化碳的吸收速率,还可能影响海洋生态系统的结构和功能。分析了海洋大气有机氮沉降的最新研究进展,结果表明：气溶胶中的有机氮在总氮中所占的比例为39.6%±14.7%;陆地雨水中以有机形式存在的溶解氮为30.2%±15.0%,而海洋上,溶解有机氮可达到雨水中总氮的62.8%±3.3%。可见,目前仅包括无机氮沉降的入海通量可能低估了1/3。因此,开展大气有机氮沉降的研究,有助于评价有机氮在全球氮循环中的作用,以及对海洋生态系统的短期和长期的影响。     

Instability of seawater pH in the South China Sea during the mid-late Holocene: Evidence from boron isotopic composition of corals

We used positive thermal ionization mass spectrometry (PTIMS) to generate high precision δ¹¹B records in Porites corals of the mid-late Holocene from the South China Sea (SCS). The δ¹¹B values of the Holocene corals vary significantly, ranging from 22.2‰ to 25.5‰. The paleo-pH records of the SCS, reconstructed from the δ¹¹B data, were not stable as previously thought but show a gradual increase from the Holocene thermal optimal and a sharp decrease to modern values. The latter is likely caused by the large amount of anthropogenic CO₂ emissions since the Industrial Revolution but variations of atmospheric pCO₂ cannot explain the pH change of the SCS before the Industrial Revolution. We suggest that variations of monsoon intensity during the mid-late Holocene may have driven the sea surface pH increase from the mid to late Holocene. Results of this study indicate that the impact of anthropogenic atmospheric CO₂ emissions may have reversed the natural pH trend in the SCS since the mid-Holocene. Such ocean pH records in the current interglacial period can help us better understand the physical and biological controls on ocean pH and possibly predict the long-term impact of climate change on future ocean acidification.     

New constraints on elemental and Pb and Nd isotope compositions of South American and Southern African aerosol sources to the South Atlantic Ocean

Improving the geochemical database available for characterising potential natural and anthropogenic aerosol sources from South America and Southern Africa is a critical precondition for studies aimed at understanding trace metal controls on the marine biogeochemical cycles of the South Atlantic Ocean. We here present new elemental and isotopic data for a wide range of sample types from South America and Southern Africa that are potentially important aerosol sources. This includes road dust from Buenos Aires and lichen samples from Johannesburg, soil dust from Patagonia, volcanic ash from the Andean volcanic belt, and aerosol samples from São Paulo. All samples were investigated for major (Al, Ca, Fe, Mg, Na, K, Mn) and trace element (Cd, Co, Cr, Cu, Ni, Pb, REE, Sc, Th, Y, V, Zn) concentrations and Nd and Pb isotopic compositions. We show that diagrams of ²⁰⁸Pb/²⁰⁷Pb vs. ε_Nd, ²⁰⁸Pb/²⁰⁷Pb vs. Pb/Al, 1/[Pb], Zn/Al, Cd/Al, Cu/Al, and ε_Nd vs. Pb/Al, and 1/[Nd] are best suited to separate South American and South African source regions as well as natural and anthropogenic sources. A subset of samples from Patagonia and the Andes was additionally subjected to separation of a fine (<5?μm) fraction and compared to the composition of the bulk sample. We show that differences in the geochemical signature of bulk samples between individual regions and source types are significantly larger than between grain sizes. Jointly, these findings present an important step forward towards a quantitative assessment of aeolian trace metal inputs to the South Atlantic Ocean.     

A non-steady-state compartmental model of global-scale mercury biogeochemistry with interhemispheric atmospheric gradients

A box model of mercury (Hg) cycling between the atmosphere and ocean is described and used to estimate Hg fluxes on a global scale (The Global/Regional Interhemispheric Mercury Model, GRIMM). Unlike previous simulations of this system, few assumptions are made concerning the rate of prominent marine biogeochemical processes affecting Hg (e.g., evasion, particle scavenging, and deep ocean burial). Instead, consistency with two observed atmospheric distributions was required: the interhemispheric gradient in total atmospheric Hg and the value for changes in the deposition of Hg from the atmosphere since industrialization observed in both hemispheres. Sensitivity analyses underscore the importance to modeling of the atmospheric lifetime of Hg, the magnitude of the interhemispheric gradient, the historical changes in Hg concentrations of various reservoirs, and vertical exchange between the surface ocean and the permanent thermocline. Results of the model indicate: lower evasional fluxes of Hg from the global ocean than previous estimates; a prominent role for particle scavenging as a removal mechanism from the surface ocean; a modest influence of dry processes (dust and gas) on Hg removal from the atmosphere; and an estimate of natural land-based sources of Hg to the atmosphere that is no more than about half that of anthropogenic sources.     

Zoogeography and imperial defence: Tracing the contours of the Nearctic region in the temperate North Atlantic, 1838–1880s

This paper focuses on the ‘zoogeographic region’ and the ‘zoogeographical boundary-line’ as key biogeographical constructs of empire. More specifically, it investigates how army and navy officers stationed at Halifax and Bermuda on the North America and West Indies Station helped to create an imperial, militarized ‘New World’ region in the North Atlantic through zoogeography in the British post-emancipation era. The tracing of the boundary-line between the temperate (Nearctic) and tropical (Neotropical) North Atlantic involved designating Bermuda and Halifax as strategic winter and summer ‘homes’ on the Station, and highlighting the ‘natural’ connections between the two sites through mobile fauna, ocean currents, and weather systems. Making visible the geographic distribution of migratory animals, the Gulf Stream, and hurricanes – through maps, natural collections, sketches, and travel-writing – provided new ways of seeing and thinking about British imperial defence in the North Atlantic. This paper also considers the role of non-human mobilities in animating these regions.     

Influence of circulation parameters on the AOD variations over the Bay of Bengal during ICARB

MODIS (Moderate Resolution Imaging Spectroradiometer) level-3 aerosol data, NCEP (National Centers for Environmental Prediction) reanalysis winds and QuikSCAT ocean surface winds were made use of to examine the role of atmospheric circulation in governing aerosol variations over the Bay of Bengal (BoB) during the first phase of the ICARB (Integrated Campaign for Aerosols, gases and Radiation Budget) campaign (March 18–April 12, 2006). An inter-comparison between MODIS level-3 aerosol optical depth (AOD) data and ship-borne MICROTOPS measurements showed good agreement with correlation 0.92 (p < 0.0001) and a mean MODIS underestimation by 0.01. During the study period, the AOD over BoB showed high values in the northern/north western regions, which reduced towards the central and southern BoB. The wind patterns in lower atmospheric layers (> 850 hPa) indicated that direct transport of aerosols from central India was inhibited by the presence of a high pressure and a divergence over BoB in the lower altitudes. On the other hand, in the upper atmospheric levels, winds from central and northern India stretched south eastwards and converged over BoB with a negative vorticity indicative of a downdraft. These wind patterns pointed to the possibility of aerosol transport from central India to BoB by upper level winds. This mechanism was further confirmed by the significant correlations that AOD variations over BoB showed with aerosol flux convergence and flux vorticity at upper atmospheric levels (600–500 hPa). AOD in central and southern BoB away from continental influences displayed an exponential dependence on the QuikSCAT measured ocean surface wind speed. This study shows that particles transported from central and northern India by upper atmospheric circulations as well as the marine aerosols generated by ocean surface winds contributed to the AOD over the BoB during the first phase of ICARB.     

撒哈拉地区沙尘气溶胶南北空间型分布特征及其成因

本次研究利用MODIS、CALIPSO等卫星观测资料以及MERRA-2再分析资料分析了2007–2017年撒哈拉地区气溶胶光学厚度的空间分布特征.结果表明,撒哈拉地区气溶胶光学厚度的空间分布具有明显的季节变化,夏季沙尘气溶胶光学厚度高值区位于撒哈拉北部地区,高达0.6以上;而冬季沙尘气溶胶光学厚度高值区位于撒哈拉南部地...     

A study on the effects of soil moisture,air humidity,and air temperature on wind speed threshold for dust emissions in the Taklimakan Desert

Natural Hazards - Soil and the atmospheric conditions are important factors that affect wind speed threshold of surface dust emissions. Based on the observed data of surface dust emissions in the...     

唐山市曹妃甸地区大气降尘矿物学特征及环境意义——以华北理工大学校区为例

大气降尘矿物学特征研究具有重要的环境学意义。文章以华北理工大学校区采集样品为例,应用激光粒度分析仪、扫描电镜、X射线粉末衍射、电感耦合等离子体质谱等对河北省唐山市曹妃甸地区大气降尘矿物学特征进行了初步分析研究。结果表明,曹妃甸地区大气降尘粒径较粗,颗粒物包括块状、柱状、片状、球状及不规则粒状集合体,主要由石英、长石、石膏、云母、绿泥石、角闪石、白云石、方解石和赤铁矿等矿物组成;降尘样品中Cr、Cu、Zn、As、Cd、Pb等重金属元素含量均较高。研究分析表明,降尘样品中硅酸盐矿物主要源自地面扬尘,而石膏、方解石等碳酸盐矿物可能为环境中的次生矿物,样品中重金属污染主要来源于燃煤、工矿企业生产排放和少部分汽车尾气排放。