Air quality diagnosis from comprehensive observations of total OH reactivity and reactive trace species in urban central Tokyo

Yoshino, Akira; Nakashima, Yoshihiro; Miyazaki, Kôji; Kato, S.; Suthawaree, Jeeranut; Shimo, Nobuo; Matsunaga, Sou; Chatani, Satoru; Apel, E. C.; Greenberg, J.; Guenther, Alex; Ueno, Hiroyuki; Sasaki, Hiroyuki; Hoshi, Junya; Yokota, Hisashi; Ishii, Kazushige; Kajii, Yoshizumi

doi:10.1016/j.atmosenv.2011.12.029

Cited by 72 publications

(41 citation statements)

References 29 publications

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“…In contrast, there were no noticeable differences in CO levels between the urban and rural sites (∼ 1-2 ppm). The observed CO, NO x , and SO 2 levels in TRF were much lower than those observed in the suburban regions of Chinese megacities such as Beijing , Shanghai (Tie et al, 2013), and the Pearl River Delta region and similar to the observed levels in Tokyo, Japan (Yoshino et al, 2012).…”

Section: Observational Resultssupporting

confidence: 73%

Impact of isoprene and HONO chemistry on ozone and OVOC formation in a semirural South Korean forest

Kim

Lee³

et al. 2015

Atmos. Chem. Phys.

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Abstract. Rapid urbanization and economic development in East Asia in past decades has led to photochemical air pollution problems such as excess photochemical ozone and aerosol formation. Asian megacities such as Seoul, Tokyo, Shanghai, Guangzhou, and Beijing are surrounded by densely forested areas, and recent research has consistently demonstrated the importance of biogenic volatile organic compounds (VOCs) from vegetation in determining oxidation capacity in the suburban Asian megacity regions. Uncertainties in constraining tropospheric oxidation capacity, dominated by hydroxyl radical, undermine our ability to assess regional photochemical air pollution problems. We present an observational data set of CO, NO x , SO 2 , ozone, HONO, and VOCs (anthropogenic and biogenic) from Taehwa research forest (TRF) near the Seoul metropolitan area in early June 2012. The data show that TRF is influenced both by aged pollution and fresh biogenic volatile organic compound emissions. With the data set, we diagnose HO x (OH, HO 2 , and RO 2 ) distributions calculated using the University of Washington chemical box model (UWCM v2.1) with nearexplicit VOC oxidation mechanisms from MCM v3.2 (Master Chemical Mechanism). Uncertainty from unconstrained HONO sources and radical recycling processes highlighted in recent studies is examined using multiple model simulations with different model constraints. The results suggest that (1) different model simulation scenarios cause systematic differences in HO x distributions, especially OH levels (up to 2.5 times), and (2) radical destruction (HO 2 + HO 2 or HO 2 + RO 2 ) could be more efficient than radical recycling (RO 2 + NO), especially in the afternoon. Implications of the uncertainties in radical chemistry are discussed with respect to ozone-VOC-NO x sensitivity and VOC oxidation product formation rates. Overall, the NO x limited regime is assessed except for the morning hours (8 a.m. to 12 p.m. local standard time), but the degree of sensitivity can significantly vary depending on the model scenarios. The model results also suggest that RO 2 levels are positively correlated with oxygenated VOCs (OVOCs) production that is not routinely constrained by observations. These unconstrained OVOCs can cause higher-than-expected OH loss rates (missing OH reactivity) and secondary organic aerosol formation. The series of modeling experiments constrained by observations strongly urge observational constraint of the radical pool to enable precise understanding of regional photochemical pollution problems in the East Asian megacity region.

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Section: Observational Resultssupporting

confidence: 73%

Impact of isoprene and HONO chemistry on ozone and OVOC formation in a semirural South Korean forest

Kim

Lee³

et al. 2015

Atmos. Chem. Phys.

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“…OH reactivity for the sum of CO, NO, NO y , O 3 , SO 2 and methane is assigned as "inorganics" and that for NMHCs except for biogenic species (isoprene and monoterpenes) is assigned as "anthropogenic". Averaged total OH reactivity at MEF is much lower than that measured in urban (33.4 s À1 ) and suburban (27.7 s À1 ) areas in Tokyo in the same summer season (Yoshino et al, 2006(Yoshino et al, , 2012 using techniques that are the same as that used at MEF for this study. Measurements of OH reactivity in the boreal forest in summer have been reported (Sinha et al, 2010) and the averaged total OH reactivity (9 s À1 ) was similar to that derived from the present study.…”

Section: Contribution To the Oh Reactivitymentioning

confidence: 71%

“…Recently, OH reactivity has been recognized as a useful index for the observation of trace species in ambient air. The results of the measurements of OH reactivity and comparison with the trace species analysis have been reported for some environmental conditions (Sadanaga et al, 2004;Yoshino et al, 2006Yoshino et al, , 2012Ingham et al, 2009;Mao et al, 2009;Lee et al, 2009;Sinha et al, 2008Sinha et al, , 2010Kim et al, 2011, Nakashima et al, 2010. OH reactivity measurements have been reported for several forests which the concentration of isoprene (Di Carlo et al, 2004;Ingham et al, 2009;Sinha et al, 2008;Edwards et al, 2013) and that of monoterpenes (Sinha et al, 2010;Nölscher et al, 2012) is predominant.…”

Section: Introductionmentioning

confidence: 98%

Total OH reactivity measurements in ambient air in a southern Rocky mountain ponderosa pine forest during BEACHON-SRM08 summer campaign

Nakashima

Kato

Greenberg

et al. 2014

Atmospheric Environment

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h i g h l i g h t sThe averaged total OH reactivity for ambient pine forest air in Colorado was 6.8 s À1 . 2-methyl-3-buten-2-ol was the most prominent contribution to OH reactivity. About 30% of total OH reactivity was not assigned, implying the existence of missing OH sinks. One of the candidates of missing OH is thought to be the oxidation products of biogenic species. a r t i c l e i n f o Yoshino et al., 2006) areas in Tokyo in the same season, while sporadically high OH reactivity was also observed during some evenings. The total OH reactivity measurements were accompanied by observations of traces species such as CO, NO, NO y , O 3 and SO 2 and Volatile Organic Compounds (VOCs). From the calculation of OH reactivity based on the analysis of these trace species, 46.3% of OH reactivity for VOCs came from biogenic species that are dominated by 2-methyl-3-buten-2-ol (MBO), and monoterpenes. MBO was the most prominent contribution to OH reactivity of all trace species. A comparison of observed and calculated OH reactivity shows that the calculated OH reactivity is 29.5% less than the observed value, implying the existence of missing OH sinks. One of the candidates of missing OH is thought to be the oxidation products of biogenic species.

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“…High OH reactivity has also been observed in Paris during the MEGAPOLI campaign in 2010, with k OH reaching 130 s −1 for continental air masses and calculations based on measured VOC concentrations underestimating the reactivity by up to 75 % (Dolgorouky et al, 2012). Reactivity measurements in Tokyo were underestimated in summer, spring and autumn, but reproduced to within 5 % in winter, with the reactivity correlating well with NO x throughout the year (Sadanaga et al, 2004b;Yoshino et al, 2006;Chatani et al, 2009;Yoshino et al, 2012). Aircraft measurements of OH reactivity have also shown that reactivity tends to decrease with altitude, with discrepancies between observed and calculated reactivity most pronounced at altitudes up to 2 km and tending towards agreement at altitudes above 4 km (Mao et al, 2009).…”

Section: Overcome This Issuementioning

confidence: 89%

Measurement of OH reactivity by laser flash photolysis coupled with laser-induced fluorescence spectroscopy

et al. 2016

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Abstract. OH reactivity (k OH ) is the total pseudo-first-order loss rate coefficient describing the removal of OH radicals to all sinks in the atmosphere, and is the inverse of the chemical lifetime of OH. Measurements of ambient OH reactivity can be used to discover the extent to which measured OH sinks contribute to the total OH loss rate. Thus, OH reactivity measurements enable determination of the comprehensiveness of measurements used in models to predict air quality and ozone production, and, in conjunction with measurements of OH radical concentrations, to assess our understanding of OH production rates. In this work, we describe the design and characterisation of an instrument to measure OH reactivity using laser flash photolysis coupled to laserinduced fluorescence (LFP-LIF) spectroscopy. The LFP-LIF technique produces OH radicals in isolation, and thus minimises potential interferences in OH reactivity measurements owing to the reaction of HO 2 with NO which can occur if HO 2 is co-produced with OH in the instrument. Capabilities of the instrument for ambient OH reactivity measurements are illustrated by data collected during field campaigns in London, UK, and York, UK. The instrumental limit of detection for k OH was determined to be 1.0 s −1 for the campaign in London and 0.4 s −1 for the campaign in York. The precision, determined by laboratory experiment, is typically < 1 s −1 for most ambient measurements of OH reactivity. Total uncertainty in ambient measurements of OH reactivity is ∼ 6 %. We also present the coupling and characterisation of the LFP-LIF instrument to an atmospheric chamber for measurements of OH reactivity during simulated experiments, and provide suggestions for future improvements to OH reactivity LFP-LIF instruments.

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Air quality diagnosis from comprehensive observations of total OH reactivity and reactive trace species in urban central Tokyo

Cited by 72 publications

References 29 publications

Impact of isoprene and HONO chemistry on ozone and OVOC formation in a semirural South Korean forest

Impact of isoprene and HONO chemistry on ozone and OVOC formation in a semirural South Korean forest

Total OH reactivity measurements in ambient air in a southern Rocky mountain ponderosa pine forest during BEACHON-SRM08 summer campaign

Measurement of OH reactivity by laser flash photolysis coupled with laser-induced fluorescence spectroscopy

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