Establishing the accuracy of position–specific carbon isotope analysis of propane by GC–pyrolysis–GC–IRMS

Liu, Changjie; Liu, Peng; Wang, Xiaofeng; Li, Xiaoqiang; Horita, Juske

doi:10.1002/rcm.9494

Establishing the accuracy of position–specific carbon isotope analysis of propane by GC–pyrolysis–GC–IRMS

Journal Article · Wed Feb 15 23:00:00 EST 2023 · Rapid Communications in Mass Spectrometry

DOI:https://doi.org/10.1002/rcm.9494· OSTI ID:2420486

^[1]; Liu, Peng ^[2]; Wang, Xiaofeng ^[3]; Li, Xiaoqiang ^[4]; Horita, Juske ^[4]

Chinese Academy of Sciences (CAS), Lanzhou (China). Northwest Institute of Eco-Environment and Resources; OSTI
Xi'an University of Science and Technology (China)
Northwest University, Xi'an (China)
Texas Tech Univ., Lubbock, TX (United States)

Rationale: Position-specific (PS) δ¹³C values of propane have proven their ability to provide valuable information on the evolution history of natural gases. Two major approaches to measure PS δ¹³C values of propane are isotopic ¹³C nuclear magnetic resonance (NMR) and gas chromatography-pyrolysis-gas chromatography-isotope ratio mass spectrometry (GC-Py-GC-IRMS). Measurement accuracy of the isotopic ¹³C NMR has been verified, but the requirements of large sample size and long experimental time limit its applications. GC-Py-GC-IRMS is a more versatile method with a small sample size, but its accuracy has not been demonstrated. Methods: We measured the PS δ¹³C values of propane from nine natural gases using both ¹³C NMR and GC-Py-GC-IRMS, then evaluated the accuracy of the GC-Py-GC-IRMS method. Results: The results show that large carbon isotope fractionations occurred for both terminal and central carbons within propane during pyrolysis. The isotope fractionations during the pyrolysis are reproducible at optimum conditions, but vary between the two GC-Py-GC-IRMS systems tested, affected by experimental conditions (e.g., pyrolysis temperature, flow rate, and reactor conditions). Conclusions: It is necessary to evaluate and calibrate each GC-Py-GC-IRMS system using propane gases with accurately determined PS δ¹³C values. Finally, this study also highlights a need for PS isotope standards for propane and other molecules (e.g., butane and acetic acid).

View Accepted Manuscript (DOE)

Research Organization:: Texas Tech Univ., Lubbock, TX (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division (CSGB); Chinese Academy of Sciences (CAS); National Natural Science Foundation of China (NSFC)

Grant/Contract Number:: SC0016271

OSTI ID:: 2420486

Alternate ID(s):: OSTI ID: 1960645

Journal Information:: Rapid Communications in Mass Spectrometry, Journal Name: Rapid Communications in Mass Spectrometry Journal Issue: 9 Vol. 37; ISSN 0951-4198

Publisher:: WileyCopyright Statement

Country of Publication:: United States

Language:: English

References (25)

Development of an advanced on-line position-specific stable carbon isotope system and application to methyl tert -butyl ether Gauchotte, Caroline; O'Sullivan, Gwen; Davis, Simon Rapid Communications in Mass Spectrometry, Vol. 23, Issue 19 https://doi.org/10.1002/rcm.4222	journal	September 2009
On-line measurement of intramolecular carbon isotope distribution of acetic acid by continuous-flow isotope ratio mass spectrometry Yamada, Keita; Tanaka, Misato; Nakagawa, Fumiko Rapid Communications in Mass Spectrometry, Vol. 16, Issue 11 https://doi.org/10.1002/rcm.678	journal	January 2002
SNIF-NMR—Part 4: Applications in an Economic Context: The Example of Wines, Spirits, and Juices Jamin, Eric; Martin, Gérard J. Modern Magnetic Resonance https://doi.org/10.1007/1-4020-3910-7_188	book	January 2006
Site-specific 13C content by quantitative isotopic 13C Nuclear Magnetic Resonance spectrometry: A pilot inter-laboratory study Chaintreau, Alain; Fieber, Wolfgang; Sommer, Horst Analytica Chimica Acta, Vol. 788 https://doi.org/10.1016/j.aca.2013.06.004	journal	July 2013
Conditions to obtain precise and true measurements of the intramolecular 13C distribution in organic molecules by isotopic 13C nuclear magnetic resonance spectrometry Bayle, Kevin; Gilbert, Alexis; Julien, Maxime Analytica Chimica Acta, Vol. 846 https://doi.org/10.1016/j.aca.2014.07.018	journal	October 2014
Determination of position-specific carbon isotope ratios in propane from hydrocarbon gas mixtures Gao, Li; He, Panqing; Jin, Yongbin Chemical Geology, Vol. 435 https://doi.org/10.1016/j.chemgeo.2016.04.019	journal	October 2016
Position-specific carbon and hydrogen isotopic compositions of propane from natural gases with quantitative NMR Liu, Changjie; McGovern, Gregory P.; Liu, Peng Chemical Geology, Vol. 491 https://doi.org/10.1016/j.chemgeo.2018.05.011	journal	July 2018
Intramolecular 13C isotope distributions of butane from natural gases Julien, Maxime; Goldman, Mark J.; Liu, Changjie Chemical Geology, Vol. 541 https://doi.org/10.1016/j.chemgeo.2020.119571	journal	May 2020
Measurement of position-specific 13C isotopic composition of propane at the nanomole level Gilbert, Alexis; Yamada, Keita; Suda, Konomi Geochimica et Cosmochimica Acta, Vol. 177 https://doi.org/10.1016/j.gca.2016.01.017	journal	March 2016
Analysis of the site-specific carbon isotope composition of propane by gas source isotope ratio mass spectrometer Piasecki, Alison; Sessions, Alex; Lawson, Michael Geochimica et Cosmochimica Acta, Vol. 188 https://doi.org/10.1016/j.gca.2016.04.048	journal	September 2016
Compound– and position–specific carbon isotopic signatures of abiogenic hydrocarbons from on–land serpentinite–hosted Hakuba Happo hot spring in Japan Suda, Konomi; Gilbert, Alexis; Yamada, Keita Geochimica et Cosmochimica Acta, Vol. 206 https://doi.org/10.1016/j.gca.2017.03.008	journal	June 2017
Position-specific 13C distributions within propane from experiments and natural gas samples Piasecki, Alison; Sessions, Alex; Lawson, Michael Geochimica et Cosmochimica Acta, Vol. 220 https://doi.org/10.1016/j.gca.2017.09.042	journal	January 2018
Position-specific hydrogen isotope equilibrium in propane Xie, Hao; Ponton, Camilo; Formolo, Michael J. Geochimica et Cosmochimica Acta, Vol. 238 https://doi.org/10.1016/j.gca.2018.06.025	journal	October 2018
Molecular and intramolecular isotope geochemistry of natural gases from the Woodford Shale, Arkoma Basin, Oklahoma Liu, Changjie; Liu, Peng; McGovern, Gregory P. Geochimica et Cosmochimica Acta, Vol. 255 https://doi.org/10.1016/j.gca.2019.04.020	journal	June 2019
Kinetic and equilibrium reactions on natural and laboratory generation of thermogenic gases from Type II marine shale Li, Xiaoqiang; Horita, Juske Geochimica et Cosmochimica Acta, Vol. 333 https://doi.org/10.1016/j.gca.2022.07.020	journal	September 2022
Isotopic 13C NMR spectrometry to assess counterfeiting of active pharmaceutical ingredients: Site-specific 13C content of aspirin and paracetamol Silvestre, Virginie; Mboula, Vanessa Maroga; Jouitteau, Catherine Journal of Pharmaceutical and Biomedical Analysis, Vol. 50, Issue 3 https://doi.org/10.1016/j.jpba.2009.04.030	journal	October 2009
Bulk and position-specific isotope geochemistry of natural gases from the Late Cretaceous Eagle Ford Shale, south Texas Zhao, Heng; Liu, Changjie; Larson, Toti E. Marine and Petroleum Geology, Vol. 122 https://doi.org/10.1016/j.marpetgeo.2020.104659	journal	December 2020
Determination of position-specific carbon isotope ratios of propane from natural gas Li, Yun; Zhang, Lin; Xiong, Yongqiang Organic Geochemistry, Vol. 119 https://doi.org/10.1016/j.orggeochem.2018.02.007	journal	May 2018
Kinetics of propane cracking and position-specific isotope fractionation: Insights into the origins of natural gases Li, Xiaoqiang; McGovern, Gregory P.; Horita, Juske Organic Geochemistry, Vol. 155 https://doi.org/10.1016/j.orggeochem.2021.104234	journal	May 2021
Position-specific carbon isotopic composition of thermogenic propane: Insights from pyrolysis experiments Zhang, Lin; Li, Yun; Jiang, Wenmin Organic Geochemistry, Vol. 166 https://doi.org/10.1016/j.orggeochem.2022.104379	journal	April 2022
NMR-based isotopic and isotopomic analysis Akoka, Serge; Remaud, Gérald S. Progress in Nuclear Magnetic Resonance Spectroscopy, Vol. 120-121 https://doi.org/10.1016/j.pnmrs.2020.07.001	journal	October 2020
Comparison of IRMS and NMR spectrometry for the determination of intramolecular 13C isotope composition: Application to ethanol Gilbert, Alexis; Hattori, Ryota; Silvestre, Virginie Talanta, Vol. 99 https://doi.org/10.1016/j.talanta.2012.05.023	journal	September 2012
Constraining the atmospheric N2O budget from intramolecular site preference in N2O isotopomers Yoshida, Naohiro; Toyoda, Sakae Nature, Vol. 405, Issue 6784 https://doi.org/10.1038/35012558	journal	May 2000
Intramolecular isotopic evidence for bacterial oxidation of propane in subsurface natural gas reservoirs Gilbert, Alexis; Sherwood Lollar, Barbara; Musat, Florin Proceedings of the National Academy of Sciences, Vol. 116, Issue 14 https://doi.org/10.1073/pnas.1817784116	journal	March 2019
Carbon Isotope Fractionation In Formation Of Amino Acids By Photosynthetic Organisms Abelson, P. H.; Hoering, T. C. Proceedings of the National Academy of Sciences, Vol. 47, Issue 5, p. 623-632 https://doi.org/10.1073/pnas.47.5.623	journal	May 1961

Similar Records

Kinetic and equilibrium reactions on natural and laboratory generation of thermogenic gases from Type II marine shale

Journal Article · Mon Jul 25 00:00:00 EDT 2022 · Geochimica et Cosmochimica Acta · OSTI ID:1977159

Gas generation and intramolecular isotope study in laboratory pyrolysis of the Springfield coal from the Illinois Basin

Journal Article · Sat Jul 16 00:00:00 EDT 2022 · Organic Geochemistry · OSTI ID:1977526

Related Subjects

03 NATURAL GAS
Biochemistry & Molecular Biology
Calibration
Chemistry
GC-Py-GC-IRMS
Isotopic 13C NMR
Position-specific isotope
Propane
Spectroscopy

Establishing the accuracy of position–specific carbon isotope analysis of propane by GC–pyrolysis–GC–IRMS

Citation Formats

References (25)

Similar Records

Related Subjects