technical note: an inverse method to relate organic carbon reactivity to isotope composition from serial oxidation
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2017
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Abstract
Serial oxidation coupled with stable carbon and radiocarbon analysis of
sequentially evolved CO2 is a promising method to characterize the
relationship between organic carbon (OC) chemical composition, source, and
residence time in the environment. However, observed decay profiles depend on
experimental conditions and oxidation pathway. It is therefore necessary to
properly assess serial oxidation kinetics before utilizing decay profiles as
a measure of OC reactivity. We present a regularized inverse method to
estimate the distribution of OC activation energy (E), a proxy for bond
strength, using serial oxidation. Here, we apply this method to ramped
temperature pyrolysis or oxidation (RPO) analysis but note
that this approach is broadly applicable to any serial oxidation technique.
RPO analysis directly compares thermal reactivity to isotope composition by
determining the E range for OC decaying within each temperature interval
over which CO2 is collected. By analyzing a decarbonated test sample
at multiple masses and oven ramp rates, we show that OC decay during RPO
analysis follows a superposition of parallel first-order kinetics and that
resulting E distributions are independent of experimental conditions. We
therefore propose the E distribution as a novel proxy to describe OC
thermal reactivity and suggest that E vs. isotope relationships can provide
new insight into the compositional controls on OC source and residence time.
| Reference Key |
hemingway2017biogeosciencestechnical
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|---|---|
| Authors | ;J. D. Hemingway;J. D. Hemingway;J. D. Hemingway;D. H. Rothman;S. Z. Rosengard;S. Z. Rosengard;S. Z. Rosengard;V. V. Galy |
| Journal | tetrahedron letters |
| Year | 2017 |
| DOI |
10.5194/bg-14-5099-2017
|
| URL | |
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