Indicators of natural and anthropogenic emission source impact · 2020. 11. 2. · Indicators of...

Indicators of natural and anthropogenicemission source impact

A. Cecinato1,2, A. Bacaloni2, P. Romagnoli1, M. Perilli1,

C. Balducci1

1 CNR IIA, Monterotondo Stazione RM

2 University «Sapienza» – Rome 1, Dept. of Chemistry

Preliminary remarks:

All pollution sources release into the environment a number of characteristic chemicals (individual substances and mixtures)

Emissions persist in the environment enough long time to accumulate and to be transferred, transported or spread

Emissions can be characterized according to physical and chemical features derived from sources

qualitative

quantitative

yes/no

what source(s)

in what proportions

Inferences are:

When the emission profile of sources is well known, thevariations in the pattern of chemicals relased allow todraw information about contour conditions (namely, theenvironmental compartment).

For instance, the oxidizing capacity of atmosphere can beindexed through the distinct decomposition rates ofindividual substances there occurring and the relatedchanges in the molecular signature.

Particulates (i.e., solid state matters accumulated in grains ranging1 nm – 1 mm in diameter) affect all compartments of environment:

atmosphere

surface waters

soils

surfaces

living organisms

dispersions

depositions

dispersions

depositions

Dusts occur in waters owing to natural phenomena (scrub,wash out, etching, rain out, precipitation)and anthropogenic emissions (industrial,agricultural and urban wastes, boats)

Chemical composition of water dustsis regulated by accumulation/dilutionof low-soluble species, solubilization,redox processes, mechanical removal

Particulate (SPM) is released into the atmosphere by naturalaccidents (eruptions, fires, etching, rains; winds; sea spray),humans (vehicles; industrial, agricultural and urban wastes;heating and power plants), and biota

Looking to size, shape and chemicalfeatures, SPM looks different fromsettled dust

Inquinamento da mercurio: aria, acqua, suolo, alimenti

SPM is also generated by gaseouspollutants degradation

Impo

rtan

tpo

rtio

nsof

susp

ende

d

part

icul

ate

(SPM

) are

gene

rate

dby

chem

ical

degr

adat

ion

ofga

sph

ase

pollu

tant

s dev

elop

ing

insit

u

RCHO

R 2CO

hnhnIm

port

ant

port

ions

ofsu

spen

ded

part

icul

ate

(SPM

) are

gene

rate

dby

chem

ical

degr

adat

ion

ofga

sph

ase

pollu

tant

sde

velo

ping

insi

tu

RCH

O

R 2CO

hn

hn

RCHO

R2CO

Impo

rtan

tpo

rtio

nsof

susp

ende

d

part

icul

ate

(SPM

) are

gene

rate

dby

chem

ical

degr

adat

ion

ofga

sph

ase

pollu

tant

s dev

elop

ing

insit

u

RCHO

R 2CO

hnhnIm

port

ant

port

ions

ofsu

spen

ded

part

icul

ate

(SPM

) are

gene

rate

dby

chem

ical

degr

adat

ion

ofga

sph

ase

pollu

tant

sde

velo

ping

insi

tu

RCH

O

R 2CO

hn

hnRCHO

R2CO

Import

antpo

rtions

ofsus

pended

particu

late(SP

M)are

genera

tedby

chemic

al degr

adatio

n of ga

s phas

e

pollut

ants d

evelop

ingin s

ituRC

HO

R 2CO

hnhnIm

porta

ntpo

rtions

ofsus

pend

ed

particu

late(SP

M)are

genera

tedby

chemi

calde

gradat

ionof

gasph

ase

pollut

ants d

evelop

ingin s

itu

RCHO

R 2CO

hnhnRCHO

R2CO

Impo

rtant

portio

nsof

suspe

nded

partic

ulate

(SPM)

arege

nerat

edby

chem

ical d

egrad

ation

ofgas

phase

pollu

tants

deve

loping

insit

uRC

HO

R 2CO

hnhnIm

porta

ntpo

rtion

sof

susp

ende

d

parti

culat

e (SP

M)are

gene

rated

by

chem

ical d

egrad

ation

ofga

s pha

se

pollu

tants

deve

loping

insit

u

RCHO

R 2CO

hnhn

RCHO

R2CO

Impo

rtan

tpo

rtio

nsof

susp

ende

d

part

icul

ate

(SPM

) are

gene

rate

dby

chem

ical

degr

adat

ion

ofga

sph

ase

pollu

tant

s dev

elop

ing

insit

u

RCHO

R 2CO

hnhnIm

port

ant

port

ions

ofsu

spen

ded

part

icul

ate

(SPM

) are

gene

rate

dby

chem

ical

degr

adat

ion

ofga

sph

ase

pollu

tant

sde

velo

ping

insi

tu

RCH

O

R 2CO

hn

hn

Impo

rtan

tpo

rtio

nsof

susp

ende

d

part

icul

ate

(SPM

) are

gene

rate

dby

chem

ical

degr

adat

ion

ofga

sph

ase

pollu

tant

s dev

elop

ing

insit

u

RCHO

R 2CO

hnhnIm

port

ant

port

ions

ofsu

spen

ded

part

icul

ate

(SPM

) are

gene

rate

dby

chem

ical

degr

adat

ion

ofga

sph

ase

pollu

tant

sde

velo

ping

insi

tu

RCH

O

R 2CO

hn

hn

RCHO

R2CO

Impo

rtan

tpo

rtio

nsof

susp

ende

d

part

icul

ate

(SPM

) are

gene

rate

dby

chem

ical

degr

adat

ion

ofga

sph

ase

pollu

tant

s dev

elop

ing

insit

u

RCHO

R 2CO

hnhnIm

port

ant

port

ions

ofsu

spen

ded

part

icul

ate

(SPM

) are

gene

rate

dby

chem

ical

degr

adat

ion

ofga

sph

ase

pollu

tant

sde

velo

ping

insi

tu

RCH

O

R 2CO

hn

hnRCHO

R2CO

Import

antpo

rtions

ofsus

pended

particu

late(SP

M)are

genera

tedby

chemic

al degr

adatio

n of ga

s phas

e

pollut

ants d

evelop

ingin s

ituRC

HO

R 2CO

hnhnIm

porta

ntpo

rtions

ofsus

pend

ed

particu

late(SP

M)are

genera

tedby

chemi

calde

gradat

ionof

gasph

ase

pollut

ants d

evelop

ingin s

itu

RCHO

R 2CO

hnhnRCHO

R2CO

Impo

rtant

portio

nsof

suspe

nded

partic

ulate

(SPM)

arege

nerat

edby

chem

ical d

egrad

ation

ofgas

phase

pollu

tants

deve

loping

insit

uRC

HO

R 2CO

hnhnIm

porta

ntpo

rtion

sof

susp

ende

d

parti

culat

e (SP

M)are

gene

rated

by

chem

ical d

egrad

ation

ofga

s pha

se

pollu

tants

deve

loping

insit

u

RCHO

R 2CO

hnhn

RCHO

R2CO

Impo

rtan

tpo

rtio

nsof

susp

ende

d

part

icul

ate

(SPM

) are

gene

rate

dby

chem

ical

degr

adat

ion

ofga

sph

ase

pollu

tant

s dev

elop

ing

insit

u

RCHO

R 2CO

hnhnIm

port

ant

port

ions

ofsu

spen

ded

part

icul

ate

(SPM

) are

gene

rate

dby

chem

ical

degr

adat

ion

ofga

sph

ase

pollu

tant

sde

velo

ping

insi

tu

RCH

O

R 2CO

hn

hn

Important portions of suspended

particulate (SPM) are generated by

chemical degradation of gas phase

pollutants developing in situ

RCHO

R2 CO

hnhn





RCHO

R2 CO

hnhn

RCHO

R2 CO





RCHO

R2 CO

hnhn





RCHO

R2 CO

hnhn

RCH

O

R2 CO

Importantportions

of suspended




RCHO

R2 CO

hnhn





RCHO

R2 CO

hn

hn

RCHO

R2 CO





RCHO

R2 CO

hnhn





RCHO

R2 CO

hnhn

RCHO

R2 CO





RCHO

R2 CO

hnhn





RCHO

R2 CO

hnhn





RCHO

R2 CO

hnhn





RCHO

R2 CO

hnhn

RCHO

R2 CO





RCHO

R2 CO

hnhn





RCHO

R2 CO

hnhn

RCH

O

R2 CO

Importantportions

of suspended




RCHO

R2 CO

hnhn





RCHO

R2 CO

hn

hn

RCHO

R2 CO





RCHO

R2 CO

hnhn





RCHO

R2 CO

hnhn

RCHO

R2 CO





RCHO

R2 CO

hnhn





RCHO

R2 CO

hnhn

RCHO

R2CO

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Secondary aerosol occurs in two major forms different withregards to origin and nature:

«Acidic smog», associated to SO2 oxidationto H2SO4. H2SO4 aggregates C particles andoxidize organic species to elemental C.

«Photochemical smog» coming from gaseoushydrocarbon decomposition induced by OH,NO3, O3, NO2.

Piogge acide

Tenuta di san Rossore

corrosione di monumenti e materialidistruzione dei boschi

tutta colpa dello zolfo…...

.

Full chemical characterization of dusts (mass balance or closure)is limited to macro-components (elemental and organic carbon,sea spray, crustal matter, nitrates, sulphates, metal oxides andsalts)

Though extensive, chemical investigations of dusts deal witha few groups and tens of chemicals.Mass closure is unrealistic; nevertheless, it does not belongto purposes of researches.

Particulate organic matter (POM) is comprised of thousandsof substances displaying wide variety of

relative concentration

acidity

polarity

hydrophylic/hydrophobic ability

vapour pressure

short/long-term toxicity

Usually no peculiar chemicals occur in the emissions,

however «typical» organic mixtures characterize the sources

Distribution patterns are identified within groups and withregard to gross POM composition (e.g., polarity and watersolubility fractions), which provide insights about sourcesand/or contour conditions of the release

Diossina

Chernobyl

26 aprile 1986: esplosione del reattore nucleare n°4. Contaminata un’area di 150000 km2, persone colpite

7 milioni

Three Mile Island

28 marzo 1976. Fusione parziale d’un reattorenucleare. Rilascio di iodio e kripton radioattivinell’ambiente. Migliaia di persone colpite.

Tokaimura

30 settembre 1999: Incidente all’impianto di produzione di combustibile nucleare: rilasciodi uranio, raggi gamma e neutroni. Centinaiadi residenti colpiti dalle radiazioni.

Fukushima

11 marzo 2011: il maremoto del Tohokucolpisce l’impianto. 4 incidenti fondono 3reattori. Contaminati aria, acqua e suolo(20000 km2), colpiti fauna e popolazione.

INCIDENTI NUCLEARI

CASALE MONFERRATO1907-1984: la fabbrica d’Eternit.1200 casi di mesotelioma

POMEZIA5 maggio 2017: incendio nella Eco-X (impianto trattamento e smaltimento rifiuti industriali

PALERMO1998-2000: 37 operai Fincantieri deceduti

AMIANTO ed ETERNIT

IPA monitorati nelle polveri sospese per il Progetto EXPAH

DBahAIP

BaA BjFBbFBkF

BaP

CH BPEBeP PE

1. PAH cancerogeni

2. PAH mutageni 3. PAH addizionali

DBahAIP

BaA BjFBbFBkF

BaP

CH BPEBeP PE

1. PAH cancerogeni


DBahAIP

BaA BjFBbFBkF

BaP

CH BPEBeP PE

1. PAH cancerogeni


Idrocarburi policiclici aromatici

Radiazioni

Asbesto

Petrolio

Policlorodibenzo-p-diossine (PCDD: 75 congeneri)

Policlorobifenili(PCB: 209 congeneri)

Policlorodibenzofurani(PCDF: 135 congeneri)

Policloronaftaleni(PCN: 75 congeneri)

Polibromodifenileteri(PBDE: 209 congeneri)









































Gravi episodi d’inquinamento e rispettive cause

chlorodioxins

2,3,7,8-tetrachloro-para-dibenzodioxin

Distribution patterns of organic substances in the particulate emissions (1)

To assess the organic emission sources, three cathegories oftracers are adopted, i.e.:

important/predominant occurrence of an individual/a handful of component(s)

concentration ratios between pairsof components (diagnostic ratios)

molecular fingerprints of group homologuesor congeners (percentage distribution)

Non-polar fraction (normal and branched alkanes, alkenes, alicyclics)

n-Alkanes

Distinct profiles for biogenic and fossil fuels emissions.

Various indicators have been formulated, e.g.:

Carbon Preference Indexes (Cn ranging C12÷C36)

n-Alkanes vs. non-linear HCs (hump)

Natural wax percentage

Distribution patterns of organic substances in particulate emissions (2)

n-Alkanes


fuelslubricating oils

biogenic HCs

high trees

city center

rural area

n-Alkanes: CPI indexes


CmaxC29, C31

C21, C23

C16÷C21

high trees

petroleum

bacteria, algae

NW% =S12 [C2n+1 - 0.5*(C2n + C2n+2)]

S12 [C2n+1]

17

17

Branched and alicyclic hydrocarbons

A list of indexes and markers has been drawn, including:

pristane/phytane ratio

hopanes and steranes

squalane and squalene

sitosterol, stigmasterol, cholesterol, amyrins


20 24 28 32 36 40time (min)

0

20

40

60

80

100

Rel

ativ

e A

bu

nd

ance

26.25

26.07

32.87

34.4420.08

30.27

29.44 36.6038.65

31.32

21.4222.04 30.4827.23

26.07

22.53

24.09

20.24 33.18

m/z = 191

m/z = 217

hopanes

steranes

20 24 28 32 36 40time (min)

0

20

40

60

80

100

Rel

ativ

e A

bu

nd

ance

26.25

26.07

32.87

34.4420.08

30.27

29.44 36.6038.65

31.32

21.4222.04 30.4827.23

26.07

22.53

24.09

20.24 33.18

m/z = 191

m/z = 217

hopanes

steranes

Branched and alicyclic hydrocarbons

iso- e anteiso-alkanes (C27-C36 range): typical profile of tobacco smoke


odd iso-alkanes and even anteiso-alkanes in the tobacco smoke and in tobacco leaf wax

odd iso-ALK (a) and even anteiso-ALK (b) in the tobacco smoke and in tobacco leaf wax

Polycyclic Aromatic Hydrocarbons (PAHs)

Several PAH fingeprints have been identified based on:

retene

(1-methyl,7-isopropylphenanthrene)

benzo[ghi]fluoranthene

abietane


A. Individual compounds

B. Diagnostic ratios (DRPAH) between pair of compounds


benz[a]anthracene/chrysene

benzo[b]fluoranthene/benzo[k]fluoranthene

fluoranthene/pyrene

chrysene/benzo[a]pyrene

indeno[1,2,3-cd]pyrene/benzo[ghi]perylene

phenanthrene/S(methylphenantrenes)

phenanthrene/anthracene

CP(PAHs)/S(PAHs)

benzo[ghi]perylene/benzo[a]pyrene

B. Diagnostic ratios (DRPAH) between pair of compounds


FA/PY BA/CH IP/BPE BaP/BPE BaP/BeP

mixed 0.60 0.55

gasoline 0.54 0.8~1.3 0.20~0.35 0.35 0.95

diesel 0.8~1.1 0.38 0.65~1.1 0.8~1.1 0.50

coal 0.65 0.9~1.3 1.57

wood, pine 0.78 0.64 1.1~1.6 1.94 2.1

wood, oak 0.75 0.70 1.2~1.6 1.77 1.77

syntetic fuel 1.19 0.78 1.1 1.91

heavy oil 0.83 1.01 1.61 0.81 0.52

coke (coal) 0.30 1.9 1.21 0.78 1.65

power plant (coal) 0.66 0.56 2.01 0.88 2.57

tobacco smoke particulate 0.96 1.3 0.18 0.23 0.38

landfill 1.3 0.84 0.76 0.70 0.55

urban incinerator ~17. 0.71 0.92 ~0.12 0.01waste fumes

domestic heating

iron/steel plant

source

vehicles


dimethylphenanthrenes:

distinct profiles are assoc-

iated with oil fuels and

with biomass burning

retene: typical marker of

wood combustion13.0 14.0 15.0 16.0

time (min)

0

50

1000

50

1000

50

100

Rela

tive

Ab

un

da

nce

0

50

1000

50

10013.86

13.9913.4312.95

13.22 14.4114.68

13.85 14.1913.43

14.6813.19

14.0613.80

13.43 14.2013.20

13.79

13.3612.76

16.31

Selva, winter_3

Selva, winter_1

M/Z = 206

M/Z = 206

M/Z = 206

M/Z = 206

M/Z = 234

Leonessa, winter_1

Leonessa, winter_3

Leonessa, summer_1

Rome dust

C2-phenanthrenes and retene

As for reactivity of the atmosphere («particle ageing») the PAH-relatedindicators are:

benzo[a]pyrene/benzo[e]pyrene

ciclopenta[cd]pyrene/chrysene

benzo[b]anthracene (naphthacene)

anthanthrene


Polycyclic Aromatic Hydrocarbons (PAH)

Nitro-PAHs originate from parent PAH nitration, according to two major mechanisms:

emission sources and atmospheric photochemistrygive rise to distinct Nitro-PAHs


Nitrated Polycyclic Aromatic Hydrocarbons (Nitro-PAHs)

acid attackfree radical attack

in emissionsfrom in-situ reactions

Nitro-fluoranthenes

gaseousfluoranthene 2-nitrofluoranthene

dark

light

gaseousfluoranthene 2-nitrofluoranthene

dark

light

particulatefluoranthene

directemission

directemission

main products

other products

3-nitrofluoranthene

8-nitrofluoranthene

1-nitrofluoranthene7-nitrofluo ranthene

nitrating agents (HNO3)

3-nitrofluoranthene


directemission

directemission

main products

other products

3-nitrofluoranthene

8-nitrofluoranthene



3-nitrofluoranthene


directemission

directemission

main products

other products

3-nitrofluoranthene

8-nitrofluoranthene



3-nitrofluoranthene


directemission

directemission

main products

other products

3-nitrofluoranthene

8-nitrofluoranthene



3-nitrofluoranthene


directemission

directemission

main products

other products

3-nitrofluoranthene

8-nitrofluoranthene



3-nitrofluoranthene


Nitropyrenes


chemical reactions(photochemical)

dark

light

dark

light

dark

light

gaseous pyrene

directemission


particulatepyrene

2-nitropyrene

4-nitropyrene

1-nitropyrene

1-nitropyrene


Nitro-PAHs occurring in air

RN = nighttime formation; RD = daytime formation; ED = direct emission

2-nitrofluoranthene (RD, RN)-

1-nitropyrene (ED)4-nitropyrene (RN)

2-nitropyrene(RD)


Nitro-PAHs occurring in air and emissions

A, B: atmospheric PM;

C, D: diesel soot

NPY: nitropyrene;

NFL: nitrofluoranthene;

NAN: nitroanthracene;

NFE: nitrophenanthrene.

m/z = 223

m/z = 247

even C-number homologuesare predominant (CPI ≥5)

distinct distributions in emissions fromland/sea vegetation, high trunk plants,micro-organisms, bacteria,…


FAs and OLs originate from biogenicsources though they are present infuels and vehicle emissions

Fatty acids (linear mono/di-carboxylic, saturated/unsaturated) and Alkanols

for nC ≥7, predominance of even-C homologues (CPI ≥10)

Dicarboxylic fatty acids (DAs)

important exception: azelaic acid C7H14(COOH)2, arising fromphotochemical decomposition of oleic acid C17COOH

1=

for nC

Emission sources in interiors

Several emission sources are typical of interiors or overall affect indoorenvironments

Todays, investigations deal with emerging contaminants(endocrine disruptors, mutagens, allergenes, sensitizers,irritants, epigenetics), rather than on carcinogens

CH3

SiO

CH3

Si

SiO

CH3

CH3

CH3

CH3

CH3

CH3

SiCH

3

Si OO

CH3

O

CH3 Si

O

CH3

Si

Si

O

CH3

CH3

CH3

CH3

CH3

CH3

L3

D5

Emission sources in interiors (2)

Gaseous and particulate fractions are overall comprised of the sameorganics, partitioned between the two phases according to vapourpressure, concentration and environmental contour

Instead, dust and suspended particulates look as two distinct worlds.Both must be characterized to picture the ambient quality

Ftalati negli ambienti interni: uno studio condotto in Algeria

dust

PM10

0

10

20

30

40

50

% o

f th

e t

ota

l

dust

vapours

Me2P Et2P iBu2P nBu2P BuBzP (EH)2P

µg/m2 Me2P Et2P iBu2P nBu2P BuBzP (EH)2P NoP

UNI 0.41 4.3 23 5.7 0.61 18.2 2.7

HOS 0.09 0.11 0.05 0.06 0.02 0.19 0.26

SCH 0.53 2.6 66 22 0.36 39 4.3

DWE 0.08 1.23 1.86 7.1 0.07 21 0.71

µg/m3 Me2P Et2P iBu2P nBu2P BuBzP (EH)2P NoP

UNI 0.18 1.35 1.71 4.05 0.09 0.01 1.25

HOS 0.05 2.00 1.09 1.82 0.04 0.01 0.69

SCH 0.14 0.50 2.94 1.82 0.09 0.02 0.37

Phthalate estersin Algerian schools

Source molecular markers in indoor environments

Indoor environments are rich of chemicals released by livingorganisms (bio-aerosols, bio-dusts, bio-VOCs)

Among them three main cathegories can be recognized:

Animals (including parassites) and plants

Humans (dwellings, workplaces, public buildings, vehicles,hospitals, schools,…)

Micro-organisms (moulds, bacteria, spores, viruses…)

Source molecular markers in indoor environments (2)

Principal sources of indoor pollution

Heating plants

Foods and cooking

Dust back suspension

Intrusion from outside

Dresses, tapestries, blankets, covers

Tobacco smoking

Personal care House care (cleaning, scents, candles)

Furniture and furnishings

Living organisms and manTools and products of work

Interiors characterize for the occurrence of emission sourcesthat are peculiar or much more important than outdoors

Source molecular markers in indoor environments (3) Source molecular markers in indoor environments (3)

nicotine

myosmine

cotinine

2,3’-bipyridine

N-formylnornicotine

PM and dust hold markers of living organisms(man in particular) and of their activities

new markers of tobacco smoking


kitchen

living room

bedroom 1

bedroom 2

bedroom 2

personal care products (1)


personal care products (2)

12.5 13.5 14.5 15.5 16.5time (min)

0

20

40

60

80

100

Rel

ativ

e A

bu

nd

ance

13.89

14.11

13.30

14.5912.86

12.76

13.21

16.03

16.24

m/z = 212

m/z = 153+156

m/z = 243+258

diisopropylnaphthalenes

methyl dihydrojasmonate

galaxolide a b

12.5 13.5 14.5 15.5 16.5time (min)

0

20

40

60

80

100

Rel

ativ

e A

bu

nd

ance

13.89

14.11

13.30

14.5912.86

12.76

13.21

16.03

16.24

m/z = 212

m/z = 153+156

m/z = 243+258



galaxolide a b12.5 13.5 14.5 15.5 16.5time (min)

0

20

40

60

80

100

Rel

ativ

e A

bu

nd

ance

13.89

14.11

13.30

14.5912.86

12.76

13.21

16.03

16.24

m/z = 212

m/z = 153+156

m/z = 243+258



galaxolide a b

0.0

0.4

0.8

1.2

1.6

H_hall H_tick H_bar H_off H_chu

con

c., µ

g/g

DEET TON

GLX

Drug concentrations in three schools

0

10

20

30

Nov 28 - Dec 02 Dec 12-16 Dec 19-22

ng

/m3

NICOTINE IVIIDR

IAM

32

0

2

4

6

Nov 28 - Dec 02 Dec 12-16 Dec 19-22

ng

/m3

CAFFEINE

IVI IDR IAM

7.8

0.0

0.2

0.4

0.6

Nov 28 - Dec 02 Dec 12-16 Dec 19-22n

g/m

3

COCAINE

IVI IDR IAM

0.0

1.0

2.0

3.0

Nov 28 - Dec 02 Dec 12-16 Dec 19-22

ng/

m3

CBs

IVI IDR IAM

55

0

1

2

3

4

schools houses office

R(i

n/o

ut)

winterNIC CAF

COC CBs

5.0

in/out conc. ratio


Conclusions

The source assessment of ambient toxicants is gainingimportance and reliability thanks to two main factors:

the characterization of environments(overall interiors) with regards to ECs

the approach of chemometrics

thanks for Your attention!

If You are interested in, You can contact

Dr. Catia Balducci ([email protected])

Indicators of natural and anthropogenic emission source impact · 2020. 11. 2. · Indicators of...

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