Growth in stratospheric chlorine from short-lived chemicals not controlled by the Montreal Protocol

R. Hossaini; M. P. Chipperfield; A. Saiz-Lopez; J. J. Harrison; R. Von Glasow; R. Sommariva; E. Atlas; M. Navarro; S. A. Montzka; W. Feng; S. Dhomse; C. Harth; J. Mühle; C. Lunder; S. O'Doherty; D. Young; S. Reimann; M. K. Vollmer; P. B. Krummel; P. F. Bernath

doi:10.1002/2015GL063783

Growth in stratospheric chlorine from short-lived chemicals not controlled by the Montreal Protocol

R. Hossaini^*, M. P. Chipperfield, A. Saiz-Lopez, J. J. Harrison, R. Von Glasow, R. Sommariva, E. Atlas, M. Navarro, S. A. Montzka, W. Feng, S. Dhomse, C. Harth, J. Mühle, C. Lunder, S. O'Doherty, D. Young, S. Reimann, M. K. Vollmer, P. B. Krummel, P. F. Bernath

^*Corresponding author for this work

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Abstract

We have developed a chemical mechanism describing the tropospheric degradation of chlorine containing very short-lived substances (VSLS). The scheme was included in a global atmospheric model and used to quantify the stratospheric injection of chlorine from anthropogenic VSLS (ClyVSLS) between 2005 and 2013. By constraining the model with surface measurements of chloroform (CHCl<inf>3</inf>), dichloromethane (CH<inf>2</inf>Cl<inf>2</inf>), tetrachloroethene (C<inf>2</inf>Cl<inf>4</inf>), trichloroethene (C<inf>2</inf>HCl<inf>3</inf>), and 1,2-dichloroethane (CH<inf>2</inf>ClCH<inf>2</inf>Cl), we infer a 2013 ClyVSLS mixing ratio of 123 parts per trillion (ppt). Stratospheric injection of source gases dominates this supply, accounting for ∼83% of the total. The remainder comes from VSLS-derived organic products, phosgene (COCl<inf>2</inf>, 7%) and formyl chloride (CHClO, 2%), and also hydrogen chloride (HCl, 8%). Stratospheric ClyVSLS increased by ∼52% between 2005 and 2013, with a mean growth rate of 3.7 ppt Cl/yr. This increase is due to recent and ongoing growth in anthropogenic CH<inf>2</inf>Cl<inf>2</inf> - the most abundant chlorinated VSLS not controlled by the Montreal Protocol.

Original language	English
Pages (from-to)	4573-4580
Number of pages	8
Journal	Geophysical Research Letters
Volume	42
Issue number	11
DOIs	https://doi.org/10.1002/2015GL063783
Publication status	Published - 16 Jun 2015

Keywords

dichloromethane
Montreal Protocol
ozone
phosgene
stratosphere
VSLS

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Hossaini, R., Chipperfield, M. P., Saiz-Lopez, A., Harrison, J. J., Von Glasow, R., Sommariva, R., Atlas, E., Navarro, M., Montzka, S. A., Feng, W., Dhomse, S., Harth, C., Mühle, J., Lunder, C., O'Doherty, S., Young, D., Reimann, S., Vollmer, M. K., Krummel, P. B., & Bernath, P. F. (2015). Growth in stratospheric chlorine from short-lived chemicals not controlled by the Montreal Protocol. Geophysical Research Letters, 42(11), 4573-4580. https://doi.org/10.1002/2015GL063783

@article{10067d692cf2499eb9474324d8f0c9e2,

title = "Growth in stratospheric chlorine from short-lived chemicals not controlled by the Montreal Protocol",

abstract = "We have developed a chemical mechanism describing the tropospheric degradation of chlorine containing very short-lived substances (VSLS). The scheme was included in a global atmospheric model and used to quantify the stratospheric injection of chlorine from anthropogenic VSLS (ClyVSLS) between 2005 and 2013. By constraining the model with surface measurements of chloroform (CHCl3), dichloromethane (CH2Cl2), tetrachloroethene (C2Cl4), trichloroethene (C2HCl3), and 1,2-dichloroethane (CH2ClCH2Cl), we infer a 2013 ClyVSLS mixing ratio of 123 parts per trillion (ppt). Stratospheric injection of source gases dominates this supply, accounting for ∼83% of the total. The remainder comes from VSLS-derived organic products, phosgene (COCl2, 7%) and formyl chloride (CHClO, 2%), and also hydrogen chloride (HCl, 8%). Stratospheric ClyVSLS increased by ∼52% between 2005 and 2013, with a mean growth rate of 3.7 ppt Cl/yr. This increase is due to recent and ongoing growth in anthropogenic CH2Cl2 - the most abundant chlorinated VSLS not controlled by the Montreal Protocol.",

keywords = "dichloromethane, Montreal Protocol, ozone, phosgene, stratosphere, VSLS",

author = "R. Hossaini and Chipperfield, {M. P.} and A. Saiz-Lopez and Harrison, {J. J.} and {Von Glasow}, R. and R. Sommariva and E. Atlas and M. Navarro and Montzka, {S. A.} and W. Feng and S. Dhomse and C. Harth and J. M{\"u}hle and C. Lunder and S. O'Doherty and D. Young and S. Reimann and Vollmer, {M. K.} and Krummel, {P. B.} and Bernath, {P. F.}",

year = "2015",

month = jun,

day = "16",

doi = "10.1002/2015GL063783",

language = "English",

volume = "42",

pages = "4573--4580",

journal = "Geophysical Research Letters",

issn = "0094-8276",

publisher = "American Geophysical Union",

number = "11",

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Hossaini, R, Chipperfield, MP, Saiz-Lopez, A, Harrison, JJ, Von Glasow, R, Sommariva, R, Atlas, E, Navarro, M, Montzka, SA, Feng, W, Dhomse, S, Harth, C, Mühle, J, Lunder, C, O'Doherty, S, Young, D, Reimann, S, Vollmer, MK, Krummel, PB & Bernath, PF 2015, 'Growth in stratospheric chlorine from short-lived chemicals not controlled by the Montreal Protocol', Geophysical Research Letters, vol. 42, no. 11, pp. 4573-4580. https://doi.org/10.1002/2015GL063783

TY - JOUR

T1 - Growth in stratospheric chlorine from short-lived chemicals not controlled by the Montreal Protocol

AU - Hossaini, R.

AU - Chipperfield, M. P.

AU - Saiz-Lopez, A.

AU - Harrison, J. J.

AU - Von Glasow, R.

AU - Sommariva, R.

AU - Atlas, E.

AU - Navarro, M.

AU - Montzka, S. A.

AU - Feng, W.

AU - Dhomse, S.

AU - Harth, C.

AU - Mühle, J.

AU - Lunder, C.

AU - O'Doherty, S.

AU - Young, D.

AU - Reimann, S.

AU - Vollmer, M. K.

AU - Krummel, P. B.

AU - Bernath, P. F.

PY - 2015/6/16

Y1 - 2015/6/16

N2 - We have developed a chemical mechanism describing the tropospheric degradation of chlorine containing very short-lived substances (VSLS). The scheme was included in a global atmospheric model and used to quantify the stratospheric injection of chlorine from anthropogenic VSLS (ClyVSLS) between 2005 and 2013. By constraining the model with surface measurements of chloroform (CHCl3), dichloromethane (CH2Cl2), tetrachloroethene (C2Cl4), trichloroethene (C2HCl3), and 1,2-dichloroethane (CH2ClCH2Cl), we infer a 2013 ClyVSLS mixing ratio of 123 parts per trillion (ppt). Stratospheric injection of source gases dominates this supply, accounting for ∼83% of the total. The remainder comes from VSLS-derived organic products, phosgene (COCl2, 7%) and formyl chloride (CHClO, 2%), and also hydrogen chloride (HCl, 8%). Stratospheric ClyVSLS increased by ∼52% between 2005 and 2013, with a mean growth rate of 3.7 ppt Cl/yr. This increase is due to recent and ongoing growth in anthropogenic CH2Cl2 - the most abundant chlorinated VSLS not controlled by the Montreal Protocol.

AB - We have developed a chemical mechanism describing the tropospheric degradation of chlorine containing very short-lived substances (VSLS). The scheme was included in a global atmospheric model and used to quantify the stratospheric injection of chlorine from anthropogenic VSLS (ClyVSLS) between 2005 and 2013. By constraining the model with surface measurements of chloroform (CHCl3), dichloromethane (CH2Cl2), tetrachloroethene (C2Cl4), trichloroethene (C2HCl3), and 1,2-dichloroethane (CH2ClCH2Cl), we infer a 2013 ClyVSLS mixing ratio of 123 parts per trillion (ppt). Stratospheric injection of source gases dominates this supply, accounting for ∼83% of the total. The remainder comes from VSLS-derived organic products, phosgene (COCl2, 7%) and formyl chloride (CHClO, 2%), and also hydrogen chloride (HCl, 8%). Stratospheric ClyVSLS increased by ∼52% between 2005 and 2013, with a mean growth rate of 3.7 ppt Cl/yr. This increase is due to recent and ongoing growth in anthropogenic CH2Cl2 - the most abundant chlorinated VSLS not controlled by the Montreal Protocol.

KW - dichloromethane

KW - Montreal Protocol

KW - ozone

KW - phosgene

KW - stratosphere

KW - VSLS

UR - http://www.scopus.com/inward/record.url?scp=84934440324&partnerID=8YFLogxK

U2 - 10.1002/2015GL063783

DO - 10.1002/2015GL063783

M3 - Article (Academic Journal)

C2 - 27570318

AN - SCOPUS:84934440324

SN - 0094-8276

VL - 42

SP - 4573

EP - 4580

JO - Geophysical Research Letters

JF - Geophysical Research Letters

IS - 11

ER -

Growth in stratospheric chlorine from short-lived chemicals not controlled by the Montreal Protocol

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Professor Simon O'Doherty

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Growth in stratospheric chlorine from short-lived chemicals not controlled by the Montreal Protocol

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Professor Simon O'Doherty

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