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Title: Efficient collection and preparation of methane from low concentration waters for natural abundance radiocarbon analysis

Journal Article · · Limnology and Oceanography Methods
DOI:https://doi.org/10.1002/lom3.10184· OSTI ID:1533187

Freshwater and marine environments constitute the largest global reservoirs of the greenhouse gas methane (CH4) and natural abundance radiocarbon measurements (14C-CH4) can allow for high confidence interpretations about CH4 dynamics operating in these environments. Collecting sufficient amounts of CH4 sample for a standard, high precision 14C-accelerator mass spectrometry (AMS) analysis (~ 200 μg carbon (C)) was previously unfeasible when sampling from low CH4 concentration waters, such as much of the surface ocean (~ 2 nM), which would require collecting the CH4 from 8500 L of seawater. The method described here involves pumping 20,000–40,000 L of seawater up from depth through a dissolved gas extraction system, which enables the collection of a sample composed of 100s of L of gas in less than 4 h on station. The large volume extracted gas sample is compressed into a 1.7 L cylinder for transport from the ship to the home laboratory. The home laboratory preparation of each sample to a CH4-derived carbon dioxide aliquot for 14C-AMS analysis is carried out in 3 h on a flow-through vacuum line that simultaneously prepares aliquots for stable isotope analyses (δ13C-CH4 and δ2H-CH4). The total process blank of the method is small (5.0 μg CH4-C) and composes 1.2% of the average collected and prepared sample (424 ± 163 μg, from a recent campaign; n = 16). Finally, the 14C-CH4 blanks prepared on the vacuum line have acceptably low 14C content (0.23 ± 0.07 percent Modern Carbon (pMC); n = 7) relative to the 14C-dead (0 pMC) CH4 from which they are prepared.

Research Organization:
Univ. of Rochester, NY (United States)
Sponsoring Organization:
USDOE Office of Fossil Energy (FE); National Science Foundation (NSF)
Grant/Contract Number:
FE0028980; PLR-1417149
OSTI ID:
1533187
Journal Information:
Limnology and Oceanography Methods, Vol. 15, Issue 7; ISSN 1541-5856
Publisher:
Association for the Sciences of Limnology and Oceanography (ASLO)Copyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 11 works
Citation information provided by
Web of Science

References (33)

Fossil methane source dominates Cariaco Basin water column methane geochemistry: FOSSIL METHANE SOURCE IN CARIACO BASIN journal June 2005
Magnesium Perchlorate as an Alternative Water Trap in AMS Graphite Sample Preparation: A Report On Sample Preparation at Kccams at the University of California, Irvine journal January 2004
Oceanic Methane Biogeochemistry journal February 2007
A New Method for Analyzing 14 C of Methane in Ancient Air Extracted from Glacial Ice journal January 2008
Continuous-flow isotope ratio mass spectrometry method for carbon and hydrogen isotope measurements on atmospheric methane journal January 2010
Basin-wide estimates of the input of methane from seeps and clathrates to the Black Sea journal March 2006
Recommendations for autonomous underway pCO2 measuring systems and data-reduction routines journal April 2009
Rapid rates of aerobic methane oxidation at the feather edge of gas hydrate stability in the waters of Hudson Canyon, US Atlantic Margin journal May 2017
Performance of catalytically condensed carbon for use in accelerator mass spectrometry journal November 1984
Methane sources in gas hydrate-bearing cold seeps: Evidence from radiocarbon and stable isotopes journal June 2009
Determination of the isotopic composition of atmospheric methane and its application in the Antarctic journal January 1991
The global methane budget 2000–2012 journal January 2016
Preparation of natural methane samples for stable isotope and radiocarbon analysis: Methane isotope analysis journal September 2005
Methane fluxes from the sea to the atmosphere across the Siberian shelf seas: CH journal June 2016
Diverse origins of Arctic and Subarctic methane point source emissions identified with multiply-substituted isotopologues journal September 2016
Determining the flux of methane into Hudson Canyon at the edge of methane clathrate hydrate stability: METHANE FLUX INTO HUDSON CANYON journal October 2016
The interaction of climate change and methane hydrates: Climate-Hydrates Interactions journal February 2017
Methane fluxes to the atmosphere from deepwater hydrocarbon seeps in the northern Gulf of Mexico: AIR-SEA FLUX OF CH journal January 2012
Are the Fractionation Corrections Correct: Are the Isotopic Shifts for 14 C/ 12 C Ratios in Physical Processes and Chemical Reactions Really Twice Those for 13 C/ 12 C? journal January 2011
Geologic methane seeps along boundaries of Arctic permafrost thaw and melting glaciers journal May 2012
A survey of methane isotope abundance ( 14 C, 13 C, 2 H) from five nearshore marine basins that reveals unusual radiocarbon levels in subsurface waters : UNUSUAL CH journal December 2008
Regional and seasonal variations in the flux of oceanic carbon monoxide to the atmosphere journal January 1995
Evaluation of a seawater equilibrator for shipboard analysis of dissolved oceanic trace gases journal August 1999
Equilibrium solubilities of methane, carbon monoxide, and hydrogen in water and sea water journal October 1979
A Preliminary Determination of the Absolute 14 C/ 12 C Ratio of OX-I journal January 2007
Dissolved methane and carbon dioxide fluxes in Subarctic and Arctic regions: Assessing measurement techniques and spatial gradients journal February 2016
Centennial evolution of the atmospheric methane budget: what do the carbon isotopes tell us? journal January 2007
A rapid method for preparing low volume CH 4 and CO 2 gas samples for 14 C AMS analysis journal January 2015
Rising atmospheric methane: 2007-2014 growth and isotopic shift: RISING METHANE 2007-2014 journal September 2016
Discussion Reporting of 14 C Data journal January 1977
The isotopic composition of atmospheric methane journal June 1999
Lithium Contamination in AMS Measurements of 14 C journal January 1991
High Resolution Measurements of Methane and Carbon Dioxide in Surface Waters over a Natural Seep Reveal Dynamics of Dissolved Phase Air–Sea Flux journal August 2014

Cited By (6)

Methane Sources in the Waters of Lake Michigan and Lake Superior as Revealed by Natural Radiocarbon Measurements journal May 2019
Greenhouse gas emissions from diverse Arctic Alaskan lakes are dominated by young carbon journal January 2018
Limited contribution of ancient methane to surface waters of the U.S. Beaufort Sea shelf journal January 2018
Comment on “The origin of methane in the East Siberian Arctic Shelf unraveled with triple isotope analysis” by Sapart et al. (2017) journal January 2018
Carbon isotopes (13C and 14C) and concentrations of dissolved methane (CH4) in surface waters sampled in June 2019 at the Coal Oil Point seep field of the Santa Barbara Basin dataset January 2020
Radiocarbon in methane from waters of the US Atlantic and Pacific margins as collected on R/V Hugh Sharp cruise HRS1713 and R/V Rachel Carson cruise RC0026 in 2017 and 2019 dataset January 2021