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      Reactive nitrogen chemistry in aerosol water as a source of sulfate during haze events in China

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          Abstract

          Multiphase chemistry of NO 2 and alkaline matter in aerosol water explains rapid sulfate formation and severe haze in China.

          Abstract

          Fine-particle pollution associated with winter haze threatens the health of more than 400 million people in the North China Plain. Sulfate is a major component of fine haze particles. Record sulfate concentrations of up to ~300 μg m −3 were observed during the January 2013 winter haze event in Beijing. State-of-the-art air quality models that rely on sulfate production mechanisms requiring photochemical oxidants cannot predict these high levels because of the weak photochemistry activity during haze events. We find that the missing source of sulfate and particulate matter can be explained by reactive nitrogen chemistry in aerosol water. The aerosol water serves as a reactor, where the alkaline aerosol components trap SO 2, which is oxidized by NO 2 to form sulfate, whereby high reaction rates are sustained by the high neutralizing capacity of the atmosphere in northern China. This mechanism is self-amplifying because higher aerosol mass concentration corresponds to higher aerosol water content, leading to faster sulfate production and more severe haze pollution.

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          Elucidating severe urban haze formation in China.

          As the world's second largest economy, China has experienced severe haze pollution, with fine particulate matter (PM) recently reaching unprecedentedly high levels across many cities, and an understanding of the PM formation mechanism is critical in the development of efficient mediation policies to minimize its regional to global impacts. We demonstrate a periodic cycle of PM episodes in Beijing that is governed by meteorological conditions and characterized by two distinct aerosol formation processes of nucleation and growth, but with a small contribution from primary emissions and regional transport of particles. Nucleation consistently precedes a polluted period, producing a high number concentration of nano-sized particles under clean conditions. Accumulation of the particle mass concentration exceeding several hundred micrograms per cubic meter is accompanied by a continuous size growth from the nucleation-mode particles over multiple days to yield numerous larger particles, distinctive from the aerosol formation typically observed in other regions worldwide. The particle compositions in Beijing, on the other hand, exhibit a similarity to those commonly measured in many global areas, consistent with the chemical constituents dominated by secondary aerosol formation. Our results highlight that regulatory controls of gaseous emissions for volatile organic compounds and nitrogen oxides from local transportation and sulfur dioxide from regional industrial sources represent the key steps to reduce the urban PM level in China.
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            Formation of urban fine particulate matter.

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              Effects of anthropogenic emissions on aerosol formation from isoprene and monoterpenes in the southeastern United States.

              Secondary organic aerosol (SOA) constitutes a substantial fraction of fine particulate matter and has important impacts on climate and human health. The extent to which human activities alter SOA formation from biogenic emissions in the atmosphere is largely undetermined. Here, we present direct observational evidence on the magnitude of anthropogenic influence on biogenic SOA formation based on comprehensive ambient measurements in the southeastern United States (US). Multiple high-time-resolution mass spectrometry organic aerosol measurements were made during different seasons at various locations, including urban and rural sites in the greater Atlanta area and Centreville in rural Alabama. Our results provide a quantitative understanding of the roles of anthropogenic SO2 and NOx in ambient SOA formation. We show that isoprene-derived SOA is directly mediated by the abundance of sulfate, instead of the particle water content and/or particle acidity as suggested by prior laboratory studies. Anthropogenic NOx is shown to enhance nighttime SOA formation via nitrate radical oxidation of monoterpenes, resulting in the formation of condensable organic nitrates. Together, anthropogenic sulfate and NOx can mediate 43-70% of total measured organic aerosol (29-49% of submicron particulate matter, PM1) in the southeastern US during summer. These measurements imply that future reduction in SO2 and NOx emissions can considerably reduce the SOA burden in the southeastern US. Updating current modeling frameworks with these observational constraints will also lead to more accurate treatment of aerosol formation for regions with substantial anthropogenic-biogenic interactions and consequently improve air quality and climate simulations.
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                Author and article information

                Journal
                Sci Adv
                Sci Adv
                SciAdv
                advances
                Science Advances
                American Association for the Advancement of Science
                2375-2548
                December 2016
                21 December 2016
                : 2
                : 12
                : e1601530
                Affiliations
                [1 ]Multiphase Chemistry Department, Max Planck Institute for Chemistry, Mainz 55128, Germany.
                [2 ]State Key Joint Laboratory of Environment Simulation and Pollution Control, School of Environment, Tsinghua University, Beijing 100084, China.
                [3 ]College of Engineering, University of Iowa, Iowa City, IA 52242, USA.
                [4 ]Center for Global and Regional Environmental Research, University of Iowa, Iowa City, IA 52242, USA.
                [5 ]Center for Earth System Science, Tsinghua University, Beijing 100084, China.
                [6 ]Institute for Environmental and Climate Research, Jinan University, Guangzhou 511443, China.
                Author notes
                [*]

                These authors contributed equally to this work.

                []Corresponding author. Email: yafang.cheng@ 123456mpic.de (Y.C.); hekb@ 123456tsinghua.edu.cn (K.H.); u.poschl@ 123456mpic.de (U.P.); h.su@ 123456mpic.de (H.S.)
                Article
                1601530
                10.1126/sciadv.1601530
                5176349
                28028539
                0efb4784-92b6-4432-b712-0f33a229ba9c
                Copyright © 2016, The Authors

                This is an open-access article distributed under the terms of the Creative Commons Attribution-NonCommercial license, which permits use, distribution, and reproduction in any medium, so long as the resultant use is not for commercial advantage and provided the original work is properly cited.

                History
                : 07 July 2016
                : 30 November 2016
                Funding
                Funded by: FundRef http://dx.doi.org/10.13039/501100002855, Ministry of Science and Technology of the People’s Republic of China;
                Award ID: ID0EENBG12639
                Award ID: 2012CB932201
                Award Recipient :
                Funded by: FundRef http://dx.doi.org/10.13039/501100001809, National Natural Science Foundation of China;
                Award ID: ID0EJUBG12640
                Award ID: 51231006
                Award Recipient :
                Funded by: FundRef http://dx.doi.org/10.13039/501100001809, National Natural Science Foundation of China;
                Award ID: ID0EO2BG12641
                Award ID: 51261130091
                Award Recipient :
                Categories
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                Environmental Science
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                Michael Sabado

                nanostructures,gradient nanostructures,friction,coefficient of friction,metals,cu alloys,surface roughening

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