Multiphase Chemistry at the Atmosphere–Biosphere Interface Influencing Climate and Public Health in the Anthropocene

Pöschl, Ulrich; Shiraiwa, Manabu

doi:10.1021/cr500487s

Cited by 528 publications

(573 citation statements)

References 1,121 publications

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“…Nevertheless, the detailed heterogeneous mechanism containing individual reaction channels was not included in the present work owing to the chemical complexity of the ambient aerosol. Given the potential importance of atmospheric peroxide compounds on the generation of HO x radicals and aerosol ROS, the aging of mineral dust and SOA and the formation of haze Pöschl and Shiraiwa, 2015;Zhang et al, 2015;, more comprehensive investigations including laboratory, field and modeling studies on the heterogeneous uptake processes of H 2 O 2 , MHP, PAA and other peroxides are indispensable to provide concrete evidence to elucidate the chemical budget of atmospheric peroxides in the future.…”

Section: Y Wang Et Al: Observation Of Atmospheric Peroxides During mentioning

confidence: 99%

Observation of atmospheric peroxides during Wangdu Campaign 2014 at a rural site in the North China Plain

Wang

Chen

et al. 2016

Atmos. Chem. Phys.

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Abstract. Measurements of atmospheric peroxides were made during Wangdu Campaign 2014 at Wangdu, a rural site in the North China Plain (NCP) in summer 2014. The predominant peroxides were detected to be hydrogen peroxide (H 2 O 2 ), methyl hydroperoxide (MHP) and peroxyacetic acid (PAA). The observed H 2 O 2 reached up to 11.3 ppbv, which was the highest value compared with previous observations in China at summer time. A box model simulation based on the Master Chemical Mechanism and constrained by the simultaneous observations of physical parameters and chemical species was performed to explore the chemical budget of atmospheric peroxides. Photochemical oxidation of alkenes was found to be the major secondary formation pathway of atmospheric peroxides, while contributions from alkanes and aromatics were of minor importance. The comparison of modeled and measured peroxide concentrations revealed an underestimation during biomass burning events and an overestimation on haze days, which were ascribed to the direct production of peroxides from biomass burning and the heterogeneous uptake of peroxides by aerosols, respectively. The strengths of the primary emissions from biomass burning were on the same order of the known secondary production rates of atmospheric peroxides during the biomass burning events. The heterogeneous process on aerosol particles was suggested to be the predominant sink for atmospheric peroxides. The atmospheric lifetime of peroxides on haze days in summer in the NCP was about 2-3 h, which is in good agreement with the laboratory studies. Further comprehensive investigations are necessary to better understand the impact of biomass burning and heterogeneous uptake on the concentration of peroxides in the atmosphere.

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Section: Y Wang Et Al: Observation Of Atmospheric Peroxides During mentioning

confidence: 99%

Observation of atmospheric peroxides during Wangdu Campaign 2014 at a rural site in the North China Plain

Wang

Chen

et al. 2016

Atmos. Chem. Phys.

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“…Heterogeneous reactions and multiphase processes alter the physical and chemical properties of organic aerosol particles, but the effects of these reactions are not fully elucidated (e.g. Finlayson-Pitts, 2009;George and Abbatt, 2010;Abbatt et al, 2012;Pöschl and Shiraiwa, 2015). While multiphase chemistry in aerosols and clouds can be described by a sequence of well-understood physical and chemical elementary processes in kinetic models (Hanson et al, 1994;Pöschl et al, 2007;George and Abbatt, 2010), the deduction of parameters or rate coefficients of the individual elementary processes is severely complicated by the inherent coupling of chemical reactions and mass transport processes (Kolb et al, 2010;Berkemeier et al, 2013;Shiraiwa et al, 2014).…”

Section: Introductionmentioning

confidence: 99%

Technical note: Monte Carlo genetic algorithm (MCGA) for model analysis of multiphase chemical kinetics to determine transport and reaction rate coefficients using multiple experimental data sets

et al. 2017

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Abstract. We present a Monte Carlo genetic algorithm (MCGA) for efficient, automated, and unbiased global optimization of model input parameters by simultaneous fitting to multiple experimental data sets. The algorithm was developed to address the inverse modelling problems associated with fitting large sets of model input parameters encountered in state-of-the-art kinetic models for heterogeneous and multiphase atmospheric chemistry. The MCGA approach utilizes a sequence of optimization methods to find and characterize the solution of an optimization problem. It addresses an issue inherent to complex models whose extensive input parameter sets may not be uniquely determined from limited input data. Such ambiguity in the derived parameter values can be reliably detected using this new set of tools, allowing users to design experiments that should be particularly useful for constraining model parameters. We show that the MCGA has been used successfully to constrain parameters such as chemical reaction rate coefficients, diffusion coefficients, and Henry's law solubility coefficients in kinetic models of gas uptake and chemical transformation of aerosol particles as well as multiphase chemistry at the atmosphere-biosphere interface. While this study focuses on the processes outlined above, the MCGA approach should be portable to any numerical process model with similar computational expense and extent of the fitting parameter space.

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“…Oxidation by the OH radical determines the lifetime and concentrations of many trace gases within the troposphere such as NO x (NO and NO 2 ), CH 4 , and volatile organic compounds (VOCs). The reaction of HO 2 with NO also constitutes an important source of ozone, which is damaging to plants, a respiratory irritant, and a greenhouse gas (Pöschl and Shiraiwa, 2015;Fowler et al, 2009). It is therefore important to have a thorough understanding of the reactions and processes that affect HO x concentrations.…”

Section: Introductionmentioning

confidence: 99%

The effect of viscosity and diffusion on the HO<sub>2</sub> uptake by sucrose and secondary organic aerosol particles

et al. 2016

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Abstract. We report the first measurements of HO 2 uptake coefficients, γ , for secondary organic aerosol (SOA) particles and for the well-studied model compound sucrose which we doped with copper(II). Above 65 % relative humidity (RH), γ for copper(II)-doped sucrose aerosol particles equalled the surface mass accommodation coefficient α = 0.22 ± 0.06, but it decreased to γ = 0.012 ± 0.007 upon decreasing the RH to 17 %. The trend of γ with RH can be explained by an increase in aerosol viscosity and the contribution of a surface reaction, as demonstrated using the kinetic multilayer model of aerosol surface and bulk chemistry (KM-SUB). At high RH the total uptake was driven by reaction in the near-surface bulk and limited by mass accommodation, whilst at low RH it was limited by surface reaction. SOA from two different precursors, α-pinene and 1,3,5-trimethylbenzene (TMB), was investigated, yielding low uptake coefficients of γ < 0.001 and γ = 0.004 ± 0.002, respectively. It is postulated that the larger values measured for TMB-derived SOA compared to α-pinene-derived SOA are either due to differing viscosity, a different liquid water content of the aerosol particles, or an HO 2 + RO 2 reaction occurring within the aerosol particles.

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Multiphase Chemistry at the Atmosphere–Biosphere Interface Influencing Climate and Public Health in the Anthropocene

Cited by 528 publications

References 1,121 publications

Observation of atmospheric peroxides during Wangdu Campaign 2014 at a rural site in the North China Plain

Observation of atmospheric peroxides during Wangdu Campaign 2014 at a rural site in the North China Plain

Technical note: Monte Carlo genetic algorithm (MCGA) for model analysis of multiphase chemical kinetics to determine transport and reaction rate coefficients using multiple experimental data sets

The effect of viscosity and diffusion on the HO<sub>2</sub> uptake by sucrose and secondary organic aerosol particles

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Multiphase Chemistry at the Atmosphere–Biosphere Interface Influencing Climate and Public Health in the Anthropocene

Cited by 528 publications

References 1,121 publications

Observation of atmospheric peroxides during Wangdu Campaign 2014 at a rural site in the North China Plain

Observation of atmospheric peroxides during Wangdu Campaign 2014 at a rural site in the North China Plain

Technical note: Monte Carlo genetic algorithm (MCGA) for model analysis of multiphase chemical kinetics to determine transport and reaction rate coefficients using multiple experimental data sets

The effect of viscosity and diffusion on the HO&lt;sub&gt;2&lt;/sub&gt; uptake by sucrose and secondary organic aerosol particles

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The effect of viscosity and diffusion on the HO<sub>2</sub> uptake by sucrose and secondary organic aerosol particles