Skip to main content

Lund University Publications

LUND UNIVERSITY LIBRARIES

UK greenhouse gas measurements at two new tall towers for aiding emissions verification

Stavert, Ann R. ; O'Doherty, Simon ; Stanley, Kieran ; Young, Dickon ; Manning, Alistair J. ; Lunt, Mark F. ; Rennick, Christopher and Arnold, Tim LU orcid (2019) In Atmospheric Measurement Techniques 12(8). p.4495-4518
Abstract

Under the UK-focused Greenhouse gAs and Uk and Global Emissions (GAUGE) project, two new tall tower greenhouse gas (GHG) observation sites were established in the 2013/2014 Northern Hemispheric winter. These sites, located at existing telecommunications towers, utilized a combination of cavity ring-down spectroscopy (CRDS) and gas chromatography (GC) to measure key GHGs (CO2, CH4, CO, N2O and SF6). Measurements were made at multiple intake heights on each tower. CO2 and CH4 dry mole fractions were calculated from either CRDS measurements of wet air, which were post-corrected with an instrumentspecific empirical correction, or samples dried to between 0.05 % H2O... (More)

Under the UK-focused Greenhouse gAs and Uk and Global Emissions (GAUGE) project, two new tall tower greenhouse gas (GHG) observation sites were established in the 2013/2014 Northern Hemispheric winter. These sites, located at existing telecommunications towers, utilized a combination of cavity ring-down spectroscopy (CRDS) and gas chromatography (GC) to measure key GHGs (CO2, CH4, CO, N2O and SF6). Measurements were made at multiple intake heights on each tower. CO2 and CH4 dry mole fractions were calculated from either CRDS measurements of wet air, which were post-corrected with an instrumentspecific empirical correction, or samples dried to between 0.05 % H2O and 0.3 % H2O using a Nafion® dryer, with a smaller correction applied for the residual H2O. The impact of these two drying strategies was examined. Drying with a Nafion® dryer was not found to have a significant effect on the observed CH4 mole fraction; however, Nafion® drying did cause a 0.02 μmol mol-1 CO2 bias. This bias was stable for sample CO2 mole fractions between 373 and 514 μmol mol-1 and for sample H2O up to 3.5 %. As the calibration and standard gases are treated in the same manner, the 0.02 μmol mol-1 CO2 bias is mostly calibrated out with the residual error (0.01 μmol mol-1 CO2) well below the World Meteorological Organization (WMO) reproducibility requirements. Of more concern was the error associated with the empirical instrument-specific water correction algorithms. These corrections are relatively stable and reproducible for samples with H2O between 0.2 % and 2.5 %, CO2 between 345 and 449 μmol mol-1, and CH4 between 1743 and 2145 nmol mol-1. However, the residual errors in these corrections increase to > 0.05 μmol mol-1 for CO2 and > 1 nmol mol-1 for CH4 (greater than the WMO internal reproducibility guidelines) at higher humidities and for samples with very low (< 0.5 %) water content. These errors also scale with the absolute magnitude of the CO2 and CH4 mole fractions. As such, water corrections calculated in this manner are not suitable for samples with low (< 0.5 %) or high (> 2.5 %) water contents and either alternative correction methods should be used or partial drying or humidification considered prior to sample analysis.

(Less)
Please use this url to cite or link to this publication:
author
; ; ; ; ; ; and
publishing date
type
Contribution to journal
publication status
published
in
Atmospheric Measurement Techniques
volume
12
issue
8
pages
24 pages
publisher
Copernicus GmbH
external identifiers
  • scopus:85071519253
ISSN
1867-1381
DOI
10.5194/amt-12-4495-2019
language
English
LU publication?
no
additional info
Publisher Copyright: © 2019 The Author(s).
id
b8885761-443c-45b6-ba94-d4964c326273
date added to LUP
2024-10-24 09:32:06
date last changed
2025-02-13 20:21:35
@article{b8885761-443c-45b6-ba94-d4964c326273,
  abstract     = {{<p>Under the UK-focused Greenhouse gAs and Uk and Global Emissions (GAUGE) project, two new tall tower greenhouse gas (GHG) observation sites were established in the 2013/2014 Northern Hemispheric winter. These sites, located at existing telecommunications towers, utilized a combination of cavity ring-down spectroscopy (CRDS) and gas chromatography (GC) to measure key GHGs (CO<sub>2</sub>, CH<sub>4</sub>, CO, N<sub>2</sub>O and SF<sub>6</sub>). Measurements were made at multiple intake heights on each tower. CO<sub>2</sub> and CH<sub>4</sub> dry mole fractions were calculated from either CRDS measurements of wet air, which were post-corrected with an instrumentspecific empirical correction, or samples dried to between 0.05 % H<sub>2</sub>O and 0.3 % H<sub>2</sub>O using a Nafion® dryer, with a smaller correction applied for the residual H<sub>2</sub>O. The impact of these two drying strategies was examined. Drying with a Nafion® dryer was not found to have a significant effect on the observed CH<sub>4</sub> mole fraction; however, Nafion® drying did cause a 0.02 μmol mol<sup>-1</sup> CO<sub>2</sub> bias. This bias was stable for sample CO<sub>2</sub> mole fractions between 373 and 514 μmol mol-1 and for sample H<sub>2</sub>O up to 3.5 %. As the calibration and standard gases are treated in the same manner, the 0.02 μmol mol<sup>-1</sup> CO<sub>2</sub> bias is mostly calibrated out with the residual error (0.01 μmol mol<sup>-1</sup> CO<sub>2</sub>) well below the World Meteorological Organization (WMO) reproducibility requirements. Of more concern was the error associated with the empirical instrument-specific water correction algorithms. These corrections are relatively stable and reproducible for samples with H2O between 0.2 % and 2.5 %, CO<sub>2</sub> between 345 and 449 μmol mol<sup>-1</sup>, and CH<sub>4</sub> between 1743 and 2145 nmol mol<sup>-1</sup>. However, the residual errors in these corrections increase to &gt; 0.05 μmol mol-1 for CO<sub>2</sub> and &gt; 1 nmol mol<sup>-1</sup> for CH<sub>4</sub> (greater than the WMO internal reproducibility guidelines) at higher humidities and for samples with very low (&lt; 0.5 %) water content. These errors also scale with the absolute magnitude of the CO<sub>2</sub> and CH<sub>4</sub> mole fractions. As such, water corrections calculated in this manner are not suitable for samples with low (&lt; 0.5 %) or high (&gt; 2.5 %) water contents and either alternative correction methods should be used or partial drying or humidification considered prior to sample analysis.</p>}},
  author       = {{Stavert, Ann R. and O'Doherty, Simon and Stanley, Kieran and Young, Dickon and Manning, Alistair J. and Lunt, Mark F. and Rennick, Christopher and Arnold, Tim}},
  issn         = {{1867-1381}},
  language     = {{eng}},
  number       = {{8}},
  pages        = {{4495--4518}},
  publisher    = {{Copernicus GmbH}},
  series       = {{Atmospheric Measurement Techniques}},
  title        = {{UK greenhouse gas measurements at two new tall towers for aiding emissions verification}},
  url          = {{http://dx.doi.org/10.5194/amt-12-4495-2019}},
  doi          = {{10.5194/amt-12-4495-2019}},
  volume       = {{12}},
  year         = {{2019}},
}