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A New Method for Analyzing 14C of Methane in Ancient Air Extracted from Glacial Ice

Published online by Cambridge University Press:  18 July 2016

Vasilii V Petrenko ,
Andrew M Smith ,
Gordon Brailsford ,
Katja Riedel ,
Quan Hua ,
Dave Lowe ,
Jeffrey P Severinghaus ,
Vladimir Levchenko ,
Tony Bromley  and
Rowena Moss
...Show all authors
Vasilii V Petrenko*
Affiliation:
Scripps Institution of Oceanography, University of California, San Diego, Mail Code 0244, 9500 Gilman Dr., La Jolla, California 92093, USA
Andrew M Smith
Affiliation:
Australian Nuclear Science and Technology Organisation (ANSTO), PMB 1, Menai, NSW 2234, Australia
Gordon Brailsford
Affiliation:
National Institute of Water and Atmospheric Research, Private Bag 14901, Wellington, New Zealand
Katja Riedel
Affiliation:
National Institute of Water and Atmospheric Research, Private Bag 14901, Wellington, New Zealand
Quan Hua
Affiliation:
Australian Nuclear Science and Technology Organisation (ANSTO), PMB 1, Menai, NSW 2234, Australia
Dave Lowe
Affiliation:
National Institute of Water and Atmospheric Research, Private Bag 14901, Wellington, New Zealand
Jeffrey P Severinghaus
Affiliation:
Scripps Institution of Oceanography, University of California, San Diego, Mail Code 0244, 9500 Gilman Dr., La Jolla, California 92093, USA
Vladimir Levchenko
Affiliation:
Australian Nuclear Science and Technology Organisation (ANSTO), PMB 1, Menai, NSW 2234, Australia
Tony Bromley
Affiliation:
National Institute of Water and Atmospheric Research, Private Bag 14901, Wellington, New Zealand
Rowena Moss
Affiliation:
National Institute of Water and Atmospheric Research, Private Bag 14901, Wellington, New Zealand
Jens Mühle
Affiliation:
Scripps Institution of Oceanography, University of California, San Diego, Mail Code 0244, 9500 Gilman Dr., La Jolla, California 92093, USA
Edward J Brook
Affiliation:
Department of Geosciences, Oregon State University, Corvallis, Oregon 97331, USA
*
Corresponding author. Email: vpetrenko@ucsd.edu
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Abstract

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We present a new method developed for measuring radiocarbon of methane (14CH4) in ancient air samples extracted from glacial ice and dating 11,000–15,000 calendar years before present. The small size (∼20 μg CH4 carbon), low CH4 concentrations ([CH4], 400–800 parts per billion [ppb]), high carbon monoxide concentrations ([CO]), and low 14C activity of the samples created unusually high risks of contamination by extraneous carbon. Up to 2500 ppb CO in the air samples was quantitatively removed using the Sofnocat reagent. 14C procedural blanks were greatly reduced through the construction of a new CH4 conversion line utilizing platinized quartz wool for CH4 combustion and the use of an ultra-high-purity iron catalyst for graphitization. The amount and 14C activity of extraneous carbon added in the new CH4 conversion line were determined to be 0.23 ± 0.16 μg and 23.57 ± 16.22 pMC, respectively. The amount of modern (100 pMC) carbon added during the graphitization step has been reduced to 0.03 μg. The overall procedural blank for all stages of sample handling was 0.75 ± 0.38 pMC for ∼20-μg, 14C-free air samples with [CH4] of 500 ppb. Duration of the graphitization reactions for small (<25 μg C) samples was greatly reduced and reaction yields improved through more efficient water vapor trapping and the use of a new iron catalyst with higher surface area. 14C corrections for each step of sample handling have been determined. The resulting overall 14CH4 uncertainties for the ancient air samples are ∼1.0 pMC.

Type
Articles
Information
Radiocarbon , Volume 50 , Issue 1 , 2008 , pp. 53 - 73
Copyright
Copyright © 2008 by the Arizona Board of Regents on behalf of the University of Arizona 

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