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Committee on Atmospheric Environment Observation SatellitesőĉÎeŶĵŭųŎŞŉŝŊŘŎŞŤƜơƊƍŝŃŚŘ

(2012), Science plan for Geostationary mission forŉƫŗţŝƫ=š~ŐŴŘùĄÆšmeteorology and atmospheric pollution in Asia (GMAP-?ūŴųũŊ~ŝŤŠńňŞţpýŮŃŚŘĿĝšƫ

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Importance of aqueous reactions in cloud/fog droplets anddeliquescent aerosols for the formation of water-soluble secondaryorganic aerosols





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(C1-C4)(C2-C7)(C3-C5)(C2-C4)(C2-C4)
SOA

WIOC
n-

SOA

water-soluble organiccarbon, WSOC

(C10-C34)(C9-C30)

water-n-(C9-C14)insoluble organic carbon, WIOC)

water-soluble organic matter, WSOM

(PAH)

water-insoluble organic matter, WIOM
Saxena and Hildemann[1996]

n-

WSOM

WSOM
1

(C10-C35)(

  42  (2020)

cloud condensation(pesticides)

nuclei activity, CCN activity[Glotfelty

et

al.,

1987]

PAH[Leuenberger et al., 1988; Capel et al., 1991][Kanakidou et al., 2005; Mochida, 2007; Kuwata,
2012; Kulmala et al., 2014]
WSOC

1990

volatile organic compound, VOC[

Ervens et al., 2011; Miyazaki,

WSOC

2012]

1)

(C3-C12)2)—(C10-C32)

3)(C10-C32)[Herrmann et al., 2015;[Facchini et al., 1999]

WSOC

Akimoto, 2016]

humiclike substance, HULIS
high molecular weight compounds,

WSOC

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[Zappoli et al., 1999;

Krivacsy et al., 2000; Feng ad Möller, 2004],(
SOA

particles, INT
WSOC

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HMWC

40%

[Facchini et al., 1999][, 2020]

C1-C3
C 2-

/,

C3

#$b&1980,
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Fuzzi et al., 2001; Whiteaker and Prather, 2003; Collett<C6

et al., 2008; Ehrenhauser et al., 2012; LeClair et al.,[Grosjean and Wright, 1983; Igawa et

2012; Pratt et al., 2013; Herckes et al., 2013; Boone etal., 1989]

al., 2015][Igawa et al., 1989][Kawamura and Kaplan,

FT-ICR mass spectrometry

1984; Munger et al., 1989]

700 Da(hydroxymethanesulfonate) [Munger et al.,
1986]

CHNOS

[Richartz et al., 1990]

Zhao et al., 2013]

2

CHO, CHNO, CHOS,[  42  (2020)

CHO

1

CHNO

>50%
O/C

∼0.6
[Zhao et al., 2013]u2000

Blando andTurpin [2000][

Gelencsér and Varga, 2005;

Ervens et al., 2008]
SOA
1980

Chang and Hill [1980]

1-

1-decene, C10H20

O3

4-30 µm
 .& mj}xio~+>0 

11-nonanal, C8H17CHO

1-

b!

1-

a\^d 72+

/

&


['Z(k|q|f|swu'Y(& 2+gipy~q~'X(& k|q|& C;ETELHWENE& HT& EM,*& .432D[ 7PQWRKIJT&

nonanol, C9H19OH.432&5NHRKGEO&7JHNKGEM&?PGKHTW,&&

11-Ervens et al. [2004]
CH2
Hatakeyama et al. [1985]

O3

OH
2

glutaraldehyde, HCO(CH2)3CHO
adipaldehyde, HCO(CH2)4CHO
2
5-

5-

OH

(n+2)
C6→C5→C4→C3→C2

oxopentanoic acid, HCO(CH2)3COOH
glutaric acid, HOOC(CH2)3COOH
6-

6-Enami et al. [2015]

oxohexanoic acid, HCO(CH2)4COOH
adipic acid, HOOC(CH2)4COOH

3  42  (2020)[Kawamura andBikkina, 2016]
anthropogenic volatile organic compounds,
AVOC

VOC

biogenic volatileorganic compounds, BVOC
glyoxal, GLY
methyl glyoxal, MGLY& /& a\^d'O)0(nh|z~]cwu}imnh|z~

&

HMWC

ltnh|z~e_d'O)/(nh|z~b[Carlton et al., 2007]

[C9RVHOS&HT&EM,*&/--1D.

GLYOH
glyoxylic acid, HC(O)-COOH(oxalic acid, HOOC-COOH)(HO)2CH-

COOH

C3-C6

[Tan et al., 2009]

HCO-CHO (aq) + H2O

CHO-CH(OH)2(1)

CHO-CH(OH)2 + H2O(HO)2CH-CH(OH)2(2)

OH(HO)2CH-CH(OH)2 + OH + O2 → (HO)2CH-C(OH)2OO + H2O(3)(HO)2CH-C(OH)2OO → (HO)2CH-COOH + HO2(4)(HO)2CH-COOH + OH + O2 → OO(HO)2C-COOH + H2O(5)

OO(HO)2C-COOH → HOOC-COOH + HO2

(6)

GLY

<1

mM

Ca

Zn

HMWC
>0.1 M

HMWC[Lim et al., 2010][Furukawa and
Takahashi, 2011]

HMWC

NH3

H2SO4
[Xu and
Zhang, 2012; Ortiz-Montalvo et al., 2014; Drozd et al.,2014; Peng et al., 2016]4  42  (2020)

ammonium sulfate, AS

sulfuric acid,

SA
SOA

3

SOA

YSOA
Mom

liquid water content,

LWC

Volkamer

et al.[2009]
WSOC
Daumit et al.[2014]
OH

SOA
SOA
 0& r{~v%a\^d ?>5 'B?>5(`mu'=PN('5*&7*&9(` <A7&'6*&8*&:(`b"C@PMLENHR&HT&EM,*&/--4D[7PQWRKIJT& /--4& 7RHETKVH& 7PNNPOS& 5TTRKFUTKPO& 0,-&<KGHOSH,&&

SOA[Perri et al., 2010]
SOA

gasSOA

SOA[Nozière et al., 2009]

SOA aqSOAcloud

SOA

aqSOAaerosol

brown carbon[Shapiro etal., 2009]
OH
LWC
−3

1-10 µm, 0.1-1 g m ,HMWC[Chang and Thompson,
0.1-1

2010]

GLY MGLYµm, ∼10−-6-10−5 gm−3,α[Zarzana et al., 2012]∼0.1-1 mM∼1-10 M

4-5

SOA

SOA

IEPOX

[Ervens et al.,isoprene

epoxydiol

2014; Herrmann et al., 2015]

2-

2-methyltetrol[Surratt et al.,5  42  (2020)

2010]

4

β-IEPOX
HMWC[Surratt et al., 2007]
WSOC
aqSOAcloud[Ervens et al., 2014]
SO42−

LWC

SO42−

(

MO

i

a

;

t

10438

[

dle

6

el

[Crahan et al., 2004; Yu

nl

;EE

et al., 2005; Sorooshian et al., 2006]

E

(

o

MO

cl

63.
SOA
OH
NO3−

Fe(II)/H2O2
H 2O 2

SOA

2010

OH

Kaul et al. [2011]
KanpurOH

SOA[Arakaki et al., 2013
]

1

SOA

SOA

OH

Li et al.[2013]

OH
Herrmann et al.[2010]

FresnoGe et al.[2012]

Ervens et al.[2014]
sulfate, nitrate, ammonium(

63.

oxygenated organic aerosol
SOA

O/C

SOA gasSOA

SOA
aqSOA

[Ervens, 2015]6  42  (2020)

AMS

O/C

Mt. Whistler

Lee et al.

O/C[2012]AMS

Kanpur[Chakraborty
et al., 2015; 2016]
SOA

OH

Volkamer et al.[2007]

SOA

BVOC

GLY

cisGLYmissing sink
GLY
SOA

RES

INT

SOA

INT

GLY
hydrocarbon-like OA, HOA

70-95

SOA

15%

µg m−3RES
low volatile-oxygenated OA, LV-OOA

Hennigan et al.[2008]

SOA

SOA
[Hao et al., 2013]

Gilardoni et al.[2014](Fp)

Po Valley

SOA-

140 nmHersey et al.[2011]

1.2 µmO:C

WSOC

LV-OOAINTWIOC/WSOC

0.2-0.3

WSOC

SOA

SO42−

OOA

0.6-0.8

LV-OOA

Gilardoni et al.[2016]high resolution mass spectrometry, HR-MS
SOA

SOA

O’Brien et al.[2013]
Bakersfield

SOA

HR-MS
CHON
urban-rural

O/C

7

CHO
40-52%

CHON

  42  (2020)

SOA
aqSOA

[Pratt et al.,2013]
Ervens et al.

[2011]

SOA

)

l

WSOA
SOA
[

(

Heald et al., 2005; Volkamer et al., 2006]
SOA

63.

VBS

volatile basis set[Donahue et al., 2006]
SOA

primary organic aerosol, POA

Sorooshian et al.[2006]

SOA

Pratt etal.[2013]

HMWC
ESI-MSElectrospray

WSOC

aqSOA

ionization mass spectrometer

IEPOX

aqSOA

C5H12O7S

aqSOA

SOA

SOA

O/C

Boone et al.[2015]

RH

HRMS

[Myriokefalitakis et al., 2011;
Carlton et al., 2008; Lin et al., 2012; Liu et al., 2012]

4

CHON

CHON
N:C

0.14

N:C

aqSOA

0.3

McNeill et al.[2015]

2

2-

Ervens[2015]
2-methylglyceric

acid, 2-MGA)

glycolaldehyde, GLYC

BOX

l

2000
1-2
CAPRAM
Mechanism

Chemical Aqueous Phase Radical[Herrmannet

CAPRAM2.4[Ervens et al., 2003]

8

al.,

2000]

  42  (2020)

RADM2[Stockwell et al., 1990]
RACM[Stockwell et al., 1997]

Li et al.[2013]

Ervens et al.[2004]

aqSOAcloud

aqSOAaerosol

CMAQ
SOA

CAPRAM

OH

SO4

2−

OOA
Pye etal., [2013]

aqSOA

CMAQ
IEPOX

−

2-

2-

CAPRAMCAPRAM3.0i

air parcel model

SPACCIM[Tilgner et al., 2013]

SOA
Lim et al.[2005]
SOA

Ervens and Volkamer[2010]

McNeill et al.[2012]
)

763

Q

; E A

)

E ;

;

l

X

SOA

aqSOAcloud

2.5

l

6

,
I

vWS

;A

2.5- ;C63.

]v

7PQWRKIJT& /--3& 5NHRKGEO&

7JHNKGEM&?PGKHTW,&

Community
Multiscale Air Quality Model

CMAQ

Carlton and Turpin[2013]

CMAQ

Chen et al.[2007] Carlton et al.[2008, 2010]
5

SOA

Carlton et al.[2008]
(OC)

WSOC

Sullivan

LWC
SO42−

LWC

et al.[2006]
WSOC

SO2

aqSOAcloud

VOC

SOA
Knote et al.[2014]

9E  42  (2020)

et al.[2011]
WRF-CHEM

5%
21-38 Tg yr-1

SOA
total SOA

1-15%

79%

SOA

VOC

IMPACT GFDL-AM3 GEOS-Chem
CMAQ v.5.1

VOC

aqSOAcloud aqSOAaerosol(Lin et al., 2012, 2014; Liu et al., 2012; Marais et al.,

PAH

2016)

q
Pye et al.[2017]
Southern
Oxidant and Aerosol Study

SOAS

aqSOA

WSOC

2013

/
OM/OC

κorg
aqSOA

)

r

l
GLY

MGLY

-

SOA
GEOS-Chem

Fu

et al.[2009]
BVOC
WSOC

2.2

µg C m−3

0.9

aqSOA

2.0 1.1µg C m−3
SOA

aqSOA

27%
18%

AVOC

BVOC

SOA 28%

SOA 27%

WSOC

SOA

in-aerosol

WSOC
TM4-ECPL
Myriokefalitakis

10

in-cloud  42  (2020)

SOA

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Carlton, A. G. et al. (2008), CMAQ model performance

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Article No. 042A05

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Glyoxal and dicarboxylic acids in the terrestrial atmosphere
]
1/0

/

]
SOA

PM2.5

VOC

]
]
ÃÂ]PM2.5

gasSOA
PM1

aqSOA

PM2.5
1

1
PM2.5

inorganic aerosol

IAorganic aerosol OA
OA

organic aerosol

primary
POA

secondary organic aerosol SOA
SOA

water-

insoluble secondary organic aerosol WISOA
water-soluble secondaryorganic aerosol WSSOA

WSSOA

CCN
[Kanakidou et al., 2005; Mochida, 2007; Kuwata,
2012; Kulmala et al., 2014] WSOC e]yvfci £/(¢§¤»²º[¿.,7À

1

#& ' 42/ (2020)

PM2.5

organic nitrogencompounds

1
DCA

aqSOA

SOA

aqSOAcloud

total organic aerosol

SOA

TOC

1–2%

aqSOAaerosol

WSOC

20–35%
DCA[, 2020]

DCA
[

[

aqSOA

20%

Kawamura and Ikushima,1993;

Kanakidou et al., 2005]

Kawamura andBikkina, 2016] aqSOA

TOC

DCA

1

anthropogenic volatileorganic compounds AVOC biogenic volatile organic

PM2.5 PM1

compounds BVOC

high molecular weightcompounds, HMWC

DCA
[

WSOC

, 2020

PM2.5] aqSOA
tetrols
SOA

organic sulfate
browncarbon f]V¯©º¶¼UWS8N?/R$]

2



[

#& ' 42/ (2020), 2020][Hatakeyama et al.,2

1985; Kalberer et al., 2000; Ziemann, 2002]
VOC
90%

O3

[Baboukas et al., 2000; Yao et al.,

O3

2002]

primary ozonide
O-O[Sullivan and Prather, 2007; Furukawa

CHO

-

-COOH

2

and Takahashi, 2011]

SOA
O3

fÂ¯©º¶¼U1+fce] 1+ ]1<(]

3[Kalberer et al., 2000]
adipaldehyde 1,6-hexanedial c

DCA

6-

6-oxohexanoic acid d[Yamasoe et al., 2000]

glutaraldehyde[Kawamura and Kaplan, 1987][Rogge etgal., 1991]

1,5-pentanedialSOA
5-5-oxopentanoic acidadipic acid ehglutaric[Huang and Yu, 2007; Stone et al., 2010]
DCA[Kundu et al., 2010][Kawamura et al., 2013]
DCA

60%

C2
C3

malonic acidwC2

C4 succinic acidglyoxylic acid
³C4

,

10%

DCA

[Rogge et al.,

1991; Zhao et al., 2007]

fcf] 2=&]
SOA
[
2020

,

]

 g] 2=½& ¢®«»´ª°¼b¨²¼
 &   & 0 / ~t] ] ca] fddd ¡ * D q ]emli]p]q]zc]3acid i#& ' 42/ (2020)

DCA[, 2020]–

Enami et al.[2015]
3

g
h

d h

DCA

e i
DCA
Ox

AVOC BVOC

Hatakeyama et al.[1985]

glyoxal GLY
methylglyoxal MGLYO3OH
[Sorooshian et al., 2006]
SOA
5-

Volkamer

et al.[2007]
6-

GLY

[

, 2020]Kalberer et al.[2000]

GLY

O3
,

sink

missing
GLY

,

C2-C4

GLY MGLY

Ox

high molecular weightcompounds HMWC
Carlton etal.[2007]

DCA

GLY

Tan

et al.[2009](HO)2CH-CH(OH)2
w-C2

DCA

OH
(HO)2CH-COOH[Sato et al., 2007,[

Kautzman et al., 2009, Praplan et al., 2014]2020]

fcg] 3=&]fch] ¬¹¨ª­¾º<(CP]


C2-C6

GLY

DCA

GLY

OH
C6®C5®C4®C3®C2DCA

GLY
Ervens et al.[2004]
4

AVOC

,

#& ' 42



BVOC

OH

/ (2020)

2001]

2-1,6-

CH

CH + OH (+ M) ® HOCH=CH (+ M)

(q1)

-2,4-

MHDD

[Klotz et al.,1999; Baltaretu et al., 2009]

HOCH=CH + O2 (+M) ® HOCH=CHO2 (+M) (q2)
HOCH=CHO2 + NO ® HOCH=CHO + NO2(q3)

HOCH=CHO + O2 ® OHC-CHO + HO2(q4)[Galano et al., 2008;, 2014]
NOx
OH

GLY

AVOC

BVOC
NOx

OH
OH

4

GLY MGLY2--1,4

2-butene-1,4-dial[Paulot et al., 2009;

GLY
GLY

Galloway et al., 2011]

O3

2-

-1,4
[Volkamer etal., 2001][Zhang et al., 2002]
OH

GLY

OH

O3
[Volkamer et al.,OH

 h] 2=¢ wx µ¼±¼ xs KOU&0/~u]]ca]emmjo]r ]]{a]emmm


5



GLY MGLY#& ' 42/ (2020)[Paulot et al., 2009]
GLY 
VOC

DCA

2

GLY
AVOC

BVOC

[Kawamura and Bikkina, 2016] DCA(C2

oxalic acid)

DCA

C3

C4
Volkamer et al.[2007]

acid

C5

glutaric

C6 adipic acid

GLY

[Fu et al., 2013; Kawamura andBikkina, 2016]

DCA

50–70%

C2

I e] T!Á-¢B®¸¦U ¯©º¶¼U"6#
Sampling Site Month, Year [Oxalic Acid](ng m-3)
Tokyo
Aug. 2003
260[Total DCA]
(ng m-3)580[Oxalic Acid]/[Total DCA]
0.45

[WSOC](µg m-3)---[Total DCA]/[TWSOC]---

Reference
Takegawa et al., 2007

Tokyo

May 2003

261

430

0.61

---

---

Kawamura and Watanabe 2004

Saitama(suburb)
MaebashiJul. 2007

473

734

0.64

---

---

Bao et al., 2012

May 2007
Jul.-Aug.
2008
Gosan,
Annual
S. Korea
2001-02
Beijing, China Aug. 2007

435
472

542
656

0.80
0.72

2.69
4.35

0.20
0.15

Kumagai et al., 2010

473

660

0.72

---

---

Kawamura et al., 2004

435

1010

0.43

5.59

0.18

Ho et al., 2015

Beijing, China Jul.-Aug.
2002
Xi'an, China Jul.-Aug.
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Wuhan, China Jul. 2012

412

630

0.65

---

---

Huang et al., 2005

767

1259

0.61

9.6

0.13

Cheng et al., 2013

571

1477

0.39

---

---

Guo et al., 2015

Chengdu,
China
Guangzhou,
China
Hong Kong,
China
Mt. Hua,
China
Mt. Tai, China

Winter
2011, Day
Jul.-Aug.
2007
Jun. 2003

686

1532

0.45

20

0.08

Cheng et al., 2015

216

523

0.41

1.42

0.37

Ho et al., 2011

268

526

0.51

---

---

Ho et al., 2006

Jul.-Aug.
2009
May-Jun.
2006
Inland China Spring 2004
(aircraft)
Summer2003
Chennai, India May 2007

522

744

0.70

2.2

0.34

Meng et al., 2014

1046

1702

0.61

10.4

0.16

Kawamura et al., 2013

285
183

507
653

0.56
0.28

-----

-----

Zhang et al., 2016

241

503

0.48

4.1

0.12

Pavuluri et al., 2010

1223

2107

0.58

23.3

0.09

Decesari et al., 2006

50

---

---

---

---

Laongsri and Harrison, 2013

68

140

0.49

---

---

Limbeck et al., 2005

Rondônia,
Sep.-Nov.
Brazil2002
Birmingham, Nov. 2008UK
Apr. 2011
Vienna,Feb. 1999
Austria6#& ' 42

C3 C4C3/ (2020)

Total DCA
C4

[Ho et10–30%

20%

al., 2006; Kawamura and Bikkina, 2016] DCA
1

hÂT!2®¸¦U9%]hce] A9']

AVOC

BVOC

DCA

DCA
2000

[Kawamura and
DCA

Ikushima 1993; Rogge et al., 1993; Röhrl and Lammel,
2001; Meng et al., 2014]
1

DCA

C2-C6

AVOC BVOC

Total DCA

TDCA

BVOC

WSOC

DCA

WSOC

Total DCA
DCA
0.1–0.2 µg m-3

0.01–0.05 µg m

-3

9

6

[Laongri

DCA[Kundu et al., 2010; Kawamura et al.,and Harrison, 2013]

2013]
AVOC BVOC

1 µg m-3

Total DCA
40–60%
Gosan

80%

Mt.
70–

Hua

DCA

2000 m[Meng et al., 2014] Mt. Hua

AVOC

C6
C5-C7 DCA

C2-C4 DCA

Ph

2
C2-C4 DCA

~40%

MGLY

2

GLY
1
DCA

Mt. Tai[Kawamura et al., 2013]
al., 2014]
2006]

Mt. Hua[Meng etRondônia [Decesari et al.,60–70%WSOC

Mt Hua7

C2-C4 DCA



C2-C4
Ph

#& ' 42/ (2020)C6VOC

aq-SOA

RH[Meng et al., 2014]hcf] 43V^u}q_ÁY=W]

DCA

AVOC BVOC

SO2

SO42-

OH
TDCA
liquid water content LWC[Wolff et al., 1979; Seinfeld and Pandis, 2016]
DCA

SOA

Cheng et al.[2015]
GLY
C2/GLY

SO42-

C2
ωC2

C2/ωC2

SO42-

LWC

LWC

GLY

[Yu et al.,ωC2

2005; Sorooshian et al., 2006; Kumagai et al., 2010;
Deshmukh et al.[2017]

Laongsri and Harrison, 2013; Cheng et al., 2017]

Bikkina et al.[2017]

5

Sorooshian et al.[2006]

Raipur
LWC

5

Sorooshian et al.[2006]
cloud particles

cloud interstitial

particles

cloud droplet residuals

 i] G@0J5 ¢§¤»²º®¸¦U¥¨¼>U¥¨¼=W~z]]ca]fddjq ]fddj]p]r]|c]

LWC[Sorooshian et al., 2007]

Deshmukh et al.[2016]

Wonaschuetz et al.[2012]8

#& ' 42

DCA C2-C5/ (2020)

ωC2 GLY

0.65–1.1 µm

SO42-

NH4+

LWC

]
hch] \=W]iÂ¬¹¨ª­¾º ¯©º¶¼U1³¹¼¬]
ice] Z·³º] ]Zhang et al.[2016]
SOA
2-methylglycoric acid 2-MGA

C5-[2020]

alkane triol cis-methyl-1,3,4-trihydroxy-1-butene, 3methyl-2-3-4-tryhydrol-1-butene

a-

·

CMAQ

b-

Chen et al.[2007] Carlton et al.[2008]

bSOA
GLY
MGLY

GLY
0.9

SOA
Waxman et al.[2013]
NOx

GLY[Volkamer et al., 2007]
O/A

NOx

Knote etisoprene epoxydiol

IEPOX

2-

methylthreitol2-

al.[2014]

GLY

2-

GLY
4 ´ 105 M atm-1[Ip et al.,2-

methylerythritol

2009; Kampf et al., 2013]

Yang et al.[2009]

GLY

single particle time-of-flight aerosol mass

SOA

semi-explicit

spectrometry SP-ATOFMS

Knote et al.[2014]
WEF–Chem
GLY

20%
OH
2 mm s-1
OH[Noziere et al., 2009]
9

NH4+



#& ' 42/ (2020)

GLY

in-cloud SOA

3728

GLY MGLY35
GLY

Fu et al.[2008]
GEOS–Chem
GLY

140 Tg yr-1,

Li et al.[2013]
CMAQ

45 Tg yr-1

MGLY

47% 79%

GLY
37

15

,

15

7

jÂE,:]

8
6(2014),

21

MGLY

BVOC

82

.

(2020),

79

,
,(

).

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ŐŞǅŁĀüȂȈɄȭȸȦäȆƀȜȚǻȓȈȂǶǤ

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Kurokawa, J. et al. (2013), Emissions of air pollutants andȒɘJAMSTEC ĆLȧɐɕȿȈŃýɘS-7 Ǉ&

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Ikeda, K. and H. Tanimoto (2015), Exceedances of air quality

Arnold, S. R. et al. (2016), Arctic air pollution: Challenges andstandard level of PM2.5 in Japan caused by Siberian

opportunities for the next decade, Elementa: Science of thewildfires, Environmental Research Letters, 10, 105001,

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