Publication Date:
2023-09-12
Description:
〈title xmlns:mml="http://www.w3.org/1998/Math/MathML"〉Abstract〈/title〉〈p xmlns:mml="http://www.w3.org/1998/Math/MathML" xml:lang="en"〉Chloromethane (CH〈sub〉3〈/sub〉Cl) is the most abundant natural chlorinated organic compound in the atmosphere playing an important role in catalyzing stratospheric ozone loss. Vegetation emits the largest amounts of CH〈sub〉3〈/sub〉Cl to the atmosphere but its source strength is highly uncertain leading also to large uncertainties in the global budget of CH〈sub〉3〈/sub〉Cl. Triple‐element stable isotope analysis may help to reduce uncertainties because it provides additional process‐level information compared to conventional quantification methods. In this study we performed experiments to obtain a first triple‐elemental isotopic fingerprint (〈sup〉2〈/sup〉H, 〈sup〉13〈/sup〉C, 〈sup〉37〈/sup〉Cl) of CH〈sub〉3〈/sub〉Cl emitted by a relevant plant species (royal fern, 〈italic〉Osmunda regalis〈/italic〉). Isotopic values of all three elements showed considerable differences compared to isotopic values of industrially manufactured CH〈sub〉3〈/sub〉Cl which bodes well for future applications to distinguish individual sources. Isotopic analysis of potential precursors (rain, methoxy groups) of CH〈sub〉3〈/sub〉Cl in plants revealed no measurable change of hydrogen and chlorine isotopic ratios during formation which may provide a simpler route to estimate the isotopic composition of CH〈sub〉3〈/sub〉Cl emissions. Plant degradation experiments of CH〈sub〉3〈/sub〉Cl were carried out with club moss (〈italic〉Selaginella kraussiana〈/italic〉) revealing significant isotopic fractionation for all three elements. The fractionation pattern characterized by epsilon and lambda is inconsistent with known biotic dechlorination reactions indicating a yet unreported biotic degradation mechanism for CH〈sub〉3〈/sub〉Cl. Overall, this study provides first insights into the triple‐elemental isotopic fingerprint of plant emissions and degradation. The results may represent important input data for future isotope‐based models to improve global budget estimates of CH〈sub〉3〈/sub〉Cl and to explore the yet unknown degradation pathways.〈/p〉
Description:
Plain Language Summary: Chloromethane is the most abundant chlorinated organic compound in the atmosphere. It contributes to the destruction of the ozone layer that protects us from skin cancer and genetic damage. Currently, we do not have a good understanding of the sources and removal processes of chloromethane in the atmosphere. In this paper, we use a technique that takes advantage of the different varieties of a chemical element. These so‐called isotopes behave differently during chemical reactions that lead to individual isotopic fingerprints depending on the source or removal process. We used isotopic fingerprints of all three chemical elements in chloromethane and showed that chloromethane produced by a plant (royal fern) differs substantially from chloromethane manufactured by industry. Other plant species such as club moss are able to remove chloromethane from the atmosphere but it is often not clear how this occurs. Isotopic analysis revealed that the studied club moss uses a unique, thus far unknown, way to break down chloromethane. This study demonstrates how information extracted from isotopic fingerprints will help to improve our understanding of sources and removal processes of chloromethane in the atmosphere. It can help to better predict how ozone destruction in the stratosphere affects us in the future.〈/p〉
Description:
Key Points: First triple‐element isotopic characterization of plant CH〈sub〉3〈/sub〉Cl emission and degradation.
Plant degradation experiments suggest another yet unknown transformation pathway. Important input data for future isotope based models to improve understanding of global CH〈sub〉3〈/sub〉Cl budget.
Description:
Helmholtz Association
http://dx.doi.org/10.13039/501100009318
Description:
Deutsche Forschungsgemeinschaft
http://dx.doi.org/10.13039/501100001659
Description:
https://doi.org/10.48758/ufz.13388
Keywords:
ddc:551.9
;
CH3Cl
;
ozone depletion
;
isotopes
;
plant emissions
;
halogens
Language:
English
Type:
doc-type:article
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