Atmospheric wet and dry deposition of trace elements at 10 sites in Northern China

Abstract. Atmospheric deposition is considered to be a major process that removes pollutants from the atmosphere and an important source of nutrients and contaminants for ecosystems. Trace elements (TEs), especially toxic metals deposited on plants and into soil or water, can cause substantial damage to the environment and human health due to their transfer and accumulation in food chains. Despite public concerns, quantitative knowledge of metal deposition from the atmosphere to ecosystems remains scarce. To advance our understanding of the spatiotemporal variations in the magnitudes, pathways, compositions and impacts of atmospherically deposited TEs, precipitation (rain and snow) and dry-deposited particles were collected simultaneously at 10 sites in Northern China from December 2007 to November 2010. The measurements showed that the wet and dry depositions of TEs in the target areas were orders of magnitude higher than previous observations within and outside China, generating great concern over the potential risks. The spatial distribution of the total (wet plus dry) deposition flux was consistent with that of the dry deposition, with a significant decrease from industrial and urban areas to suburban, agricultural and rural sites, while the wet deposition exhibited less spatial variation. In addition, the seasonal variation of wet deposition was also different from that of dry deposition, although they were both governed by the precipitation and emission patterns. For the majority of TEs that exist as coarse particles, dry deposition dominated the total flux at each site. This was not the case for potassium, nickel, arsenic, lead, zinc, cadmium, selenium, silver and thallium, for which the relative importance between wet and dry deposition fluxes varied by site. Whether wet deposition is the major atmospheric cleansing mechanism for the TEs depends on the size distribution of the particles. We found that atmospheric inputs of copper, lead, zinc, cadmium, arsenic and selenium were of the same magnitude as their increases in the topsoil of agricultural systems. At a background forest site in Northern China, the total deposition flux of lead observed in this study (14.1 mg m−2 yr−1) was twice that of the critical load calculated for temperate forest ecosystems in Europe. These findings provide baseline data needed for future targeting policies to protect various ecosystems from long-term heavy metal input via atmospheric deposition.

[1]  Dexia Wu,et al.  Wet and dry deposition of atmospheric nitrogen at ten sites in Northern China , 2012 .

[2]  R. Duce,et al.  Atmospheric Trace Metals at Remote Northern and Southern Hemisphere Sites: Pollution or Natural? , 1975, Science.

[3]  M. Sakata,et al.  Atmospheric dry deposition of trace elements at a site on Asian-continent side of Japan , 2011 .

[4]  Shi-chang Kang,et al.  Atmospheric wet deposition of trace elements to central Tibetan Plateau , 2010 .

[5]  M. Sakata,et al.  Dry deposition fluxes and deposition velocities of trace metals in the Tokyo metropolitan area measured with a water surface sampler. , 2004, Environmental science & technology.

[6]  S. Almeida,et al.  Approaching PM(2.5) and PM(2.5-10) source apportionment by mass balance analysis, principal component analysis and particle size distribution. , 2006, The Science of the total environment.

[7]  Stefan Norra,et al.  Efficiency of mitigation measures to reduce particulate air pollution--a case study during the Olympic Summer Games 2008 in Beijing, China. , 2012, The Science of the total environment.

[8]  T. Riis-Nielsen,et al.  Atmospheric heavy metal deposition accumulated in rural forest soils of southern Scandinavia. , 2008, Environmental pollution.

[9]  A. Muezzinoglu,et al.  Deposition of heavy metals in a Mediterranean climate area , 2006 .

[10]  B. Mason Principles of geochemistry , 1958 .

[11]  Y. Tasdemir,et al.  Atmospheric dry deposition fluxes of trace elements measured in Bursa, Turkey. , 2005, Environmental pollution.

[12]  C. W. Sweet,et al.  Atmospheric Deposition of Trace Metals at Three Sites Near the Great Lakes , 1998 .

[13]  Hefa Cheng,et al.  Lead (Pb) isotopic fingerprinting and its applications in lead pollution studies in China: a review. , 2010, Environmental pollution.

[14]  Gary Stern,et al.  Using passive air samplers to assess urban-rural trends for persistent organic pollutants. 1. Polychlorinated biphenyls and organochlorine pesticides. , 2004, Environmental science & technology.

[15]  Michael Collins,et al.  Topical Studies In Oceanography , 2000 .

[16]  J. W. Winchester,et al.  Nonurban aerosol composition near Beijing, China , 1981 .

[17]  Yuesi Wang,et al.  Acid neutralization of precipitation in Northern China , 2012, Journal of the Air & Waste Management Association.

[18]  G. Millward,et al.  Fluxes of Cu, Pb and Mn to the north-eastern Irish Sea: The importance of sedimental and atmospheric inputs , 1998 .

[19]  V. Nguyen,et al.  Atmospheric deposition of acid, heavy metals, dissolved organic carbon and nutrients in the Dutch Delta area in 1980-1986. , 1990 .

[20]  Shigeru Tanaka,et al.  Five-year record of atmospheric precipitation chemistry in urban Beijing, China , 2011 .

[21]  N. Mihalopoulos,et al.  The significance of atmospheric inputs of major and trace metals to the Black Sea , 2013 .

[22]  H. Emons,et al.  Wet deposition in Germany: long-term trends and the contribution of heavy metals. , 1997, Chemosphere.

[23]  J. Dasch Direct measurement of dry deposition to a polyethylene bucket and various surrogate surfaces. , 1985, Environmental science & technology.

[24]  T. Ruoho-Airola,et al.  Trace element deposition and trends during a ten year period in Finland. , 2009, The Science of the total environment.

[25]  R. Chester,et al.  The trace metal chemistry of atmospheric dry deposition samples collected at Cap Ferrat: a coastal site in the Western Mediterranean , 1999 .

[26]  Dexia Wu,et al.  Spatial distribution and temporal variations of atmospheric sulfur deposition in Northern China: insights into the potential acidification risks , 2013 .

[27]  A. Muezzinoglu,et al.  Solubility of deposited airborne heavy metals , 2008 .

[28]  D. Golomb,et al.  Atmospheric deposition of toxics onto Massachusetts Bay—I. Metals , 1997 .

[29]  H. Sakugawa,et al.  Three-year determination of trace metals and the lead isotope ratio in rain and snow depositions collected in Higashi-Hiroshima, Japan , 2000 .

[30]  G. McTainsh,et al.  Dust deposition and particle size in Mali, West Africa , 1997 .

[31]  Yuesi Wang,et al.  Study on dissolved organic carbon in precipitation in Northern China. , 2010 .

[32]  S. Takeda,et al.  Atmospheric deposition of trace metals to the western North Pacific Ocean observed at coastal station in Japan , 2013 .

[33]  M. Sakata,et al.  Factors contributing to seasonal variations in wet deposition fluxes of trace elements at sites along Japan Sea coast , 2009 .

[34]  D. Golomb,et al.  Atmospheric deposition of toxics onto Massachusetts Bay-II. Polycyclic aromatic hydrocarbons , 1997 .

[35]  J. Mateu,et al.  Atmospheric input of dissolved and particulate metals to the northwestern Mediterranean , 1997 .

[36]  Wen-xing Wang,et al.  PAHs distribution in precipitation at Mount Taishan: China. Identification of sources and meteorological influences. , 2010 .

[37]  Yuan Chen,et al.  The influence of governmental mitigation measures on contamination characteristics of PM(2.5) in Beijing. , 2014, The Science of the total environment.

[38]  C. Migon,et al.  Atmospheric deposition of metallic pollutants over the Ligurian Sea: labile and residual inputs. , 2002, Chemosphere.

[39]  W. Meng,et al.  Heavy metal pollution in Tianjin Bohai Bay, China. , 2008, Journal of environmental sciences.

[40]  G. Leeuw,et al.  Deposition of atmospheric trace elements into the North Sea: Coastal, ship, platform measurements and model predictions , 1998 .

[41]  Yong-guan Zhu,et al.  An inventory of trace element inputs to agricultural soils in China. , 2009, Journal of environmental management.

[42]  R. Harriss,et al.  The role of atmospheric deposition in an eastern U.S. deciduous forest , 1981 .

[43]  Ying Zhang,et al.  The distribution, enrichment and source of potential harmful elements in surface sediments of Bohai Bay, North China. , 2010, Journal of hazardous materials.

[44]  M. Hovmand,et al.  Root uptake of lead by Norway spruce grown on 210Pb spiked soils. , 2009, Environmental pollution.

[45]  S. Almeida,et al.  Approaching PM2.5 and PM2.5 − 10 source apportionment by mass balance analysis, principal component analysis and particle size distribution , 2006 .

[46]  G. Tuncel,et al.  Trace element and major ion composition of wet and dry depositon in Ankara, Turkey , 1997 .

[47]  Barak Herut,et al.  Dry atmospheric inputs of trace metals at the Mediterranean coast of Israel (SE Mediterranean): sources and fluxes , 2001 .

[48]  F. Passarini,et al.  Heavy metals monitoring at a Mediterranean natural ecosystem of Central Italy. Trends in different environmental matrixes. , 2004, Environment international.

[49]  B. Hicks,et al.  The atmospheric input of trace species to the world ocean , 1991 .

[50]  Kevin C Jones,et al.  A study of aerosol entrapment and the influence of wind speed, chamber design and foam density on polyurethane foam passive air samplers used for persistent organic pollutants. , 2009, Journal of environmental monitoring : JEM.

[51]  M. Sillanpää,et al.  Concentrations of trace elements in wet deposition over the central Himalayas, Nepal , 2014 .

[52]  K. Hunter,et al.  Wet deposition of trace metals to a remote site in Fiordland, New Zealand , 2000 .

[53]  F. Cao,et al.  Chemical characteristics and sources of organic acids in precipitation at a semi-urban site in Southwest China , 2011 .

[54]  M. Sakata,et al.  Wet and dry deposition fluxes of trace elements in Tokyo Bay , 2008 .

[55]  M. Zheng,et al.  Dry and wet deposition of elements in Hong Kong , 2005 .

[56]  Xiao-yan Li,et al.  Spatial–temporal variations, sources, and transport of airborne inhalable metals (PM 10 ) in urban and rural areas of northern China , 2014 .

[57]  A. S. Shannigrahi,et al.  Comparison of different methods for measuring dry deposition fluxes of particulate matter and polycyclic aromatic hydrocarbons (PAHs) in the ambient air , 2005 .

[58]  G. Gong,et al.  Sources, solubility, and dry deposition of aerosol trace elements over the East China Sea , 2010 .

[59]  Kevin C. Jones,et al.  Further studies on the uptake of persistent organic pollutants (POPs) by polyurethane foam disk passive air samplers , 2009 .

[60]  Min Hu,et al.  5-Year study of rainwater chemistry in a coastal mega-city in South China , 2010 .

[61]  S. Yi,et al.  Dry Deposition Fluxes and Size Distributions of Heavy Metals in Seoul, Korea During Yellow-Sand Events , 2001 .

[62]  Ding-yong Wang,et al.  Wet deposition fluxes of total mercury and methylmercury in core urban areas, Chongqing, China , 2014 .

[63]  Q. Jaradat,et al.  Atmospheric Deposition of Pb, Zn, Cu, and Cd in Amman, Jordan , 2000 .

[64]  D. Eppel,et al.  Modelling the atmospheric transport of trace metals including the role of precipitating clouds , 1991 .

[65]  M. Sakata,et al.  Regional variations in wet and dry deposition fluxes of trace elements in Japan , 2006 .

[66]  Xiangyang Qin,et al.  Multivariate and geostatistical analyses of the spatial distribution and origin of heavy metals in the agricultural soils in Shunyi, Beijing, China. , 2012, The Science of the total environment.

[67]  Yuesi Wang,et al.  Size-resolved aerosol trace elements at a rural mountainous site in Northern China: importance of regional transport. , 2013, The Science of the total environment.

[68]  Leiming Zhang,et al.  Dry deposition fluxes and deposition velocities of seven trace metal species at five sites in central Taiwan – a summary of surrogate surface measurements and a comparison with model estimations , 2011 .

[69]  R. Balasubramanian,et al.  Wet Deposition of Trace Metals in Singapore , 2003 .

[70]  B. Hicks,et al.  A review of the current status of knowledge on dry deposition , 2000 .

[71]  S. Yi,et al.  Overall elemental dry deposition velocities measured around Lake Michigan , 2001 .

[72]  Tom Harner,et al.  Characterization and comparison of three passive air samplers for persistent organic pollutants. , 2002, Environmental science & technology.

[73]  D. Grantz,et al.  Ecological effects of particulate matter. , 2003, Environment international.

[74]  R. Losno,et al.  Dissolution and solubility of trace metals from natural and anthropogenic aerosol particulate matter. , 2005, Chemosphere.

[75]  Raymond Agius,et al.  Total and water-soluble trace metal content of urban background PM10, PM2.5 and black smoke in Edinburgh, UK , 2005 .

[76]  Can Li,et al.  Concentrations and origins of atmospheric lead and other trace species at a rural site in northern China , 2010 .

[77]  D. Ollivon,et al.  Atmospheric bulk deposition of trace metals to the Seine river Basin, France: concentrations, sources and evolution from 1988 to 2001 in Paris , 2005 .

[78]  S. B. Moran,et al.  Trace elements in aerosol and precipitation at New Castle, NH, USA , 2001 .

[79]  K. Yu,et al.  Assessment of heavy metal pollution in surface soils of urban parks in Beijing, China. , 2005, Chemosphere.

[80]  J. Kim,et al.  Factors influencing atmospheric wet deposition of trace elements in rural Korea , 2012 .

[81]  Hongguang Cheng,et al.  The estimated atmospheric lead emissions in China, 1990–2009 , 2012 .

[82]  J. Hao,et al.  Atmospheric emission inventory of hazardous trace elements from China's coal-fired power plants--temporal trends and spatial variation characteristics. , 2014, Environmental science & technology.

[83]  Y. Erel,et al.  Trace elements in the North Atlantic troposphere: Shipboard results of precipitation and aerosols , 1990 .

[84]  Guebuem Kim,et al.  Atmospheric wet deposition of trace elements to Chesapeake and Delaware Bays , 2000 .

[85]  G. Carmichael,et al.  Asian emissions in 2006 for the NASA INTEX-B mission , 2009 .

[86]  Mustafa Odabasi,et al.  Ambient concentrations and dry deposition fluxes of trace elements in Izmir, Turkey , 2002 .

[87]  Kenneth E. Noll,et al.  Characterization of the deposition of particles from the atmosphere to a flat plate , 1988 .

[88]  Gan Zhang,et al.  Atmospheric deposition of heavy metals in the Pearl River Delta, China , 2003 .