期刊
ANALYTICAL CHEMISTRY
卷 93, 期 26, 页码 9139-9148出版社
AMER CHEMICAL SOC
DOI: 10.1021/acs.analchem.1c00944
关键词
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资金
- National Science Foundation [2041539]
- Hanse-Wissenschaftskolleg (HWK) Institute for Advanced Study
- U.S. Geological Survey Water Mission Area and Environmental Health Mission Area
- Division Of Ocean Sciences
- Directorate For Geosciences [2041539] Funding Source: National Science Foundation
This study introduces a new method using electrospray ionization Orbitrap to measure multidimensional isotope signatures of intact polar compounds and establishes performance metrics for comparisons with conventional mass spectrometers. Additionally, a framework for converting isotopolog intensities to delta values commonly used in isotope geochemistry was developed, providing a new pathway for measuring new isotopic signatures in diverse organic and inorganic solutes.
Widely used isotope ratio mass spectrometers have limited capabilities to measure metabolites, drugs, or small polyatomic ions without the loss of structural isotopic information. A new approach has recently been introduced that uses electrospray ionization Orbitrap to measure multidimensional isotope signatures of intact polar compounds. Using nitrate as a model compound, this study aims to establish performance metrics for comparisons with conventional IRMS at the natural abundance level. We present a framework on how to convert isotopolog intensities to delta values that are commonly used in the isotope geochemistry community. The quantification of seven nitrate isotopologs provides multiple pathways for obtaining the primary N and O delta values including non-mass-dependent O isotope variations, as well as opportunities to explore nonrandom isotopic distributions (i.e., clumping effects) within molecular nitrate. Using automation and the adaptation of measurement principles that are specific to isotope ratio analysis, nitrate delta N-15(AIR), delta O-18(VSMOW), and delta O-17(VSMOV) were measured with a long-term precision of 0.4 parts per thousand or better for isotopic reference materials and purified nitrate from environmental samples. In addition, we demonstrate promising results for unpurified environmental samples in liquid form. With these new developments, this study connects the two largely disparate mass spectrometry fields of bioanalytical MS and isotope ratio MS, thus providing a route to measure new isotopic signatures in diverse organic and inorganic solutes.
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