TY - JOUR
T1 - Stable carbon isotopic composition of biomass burning emissions – implications for estimating the contribution of C3 and C4 plants
AU - Vernooij, Roland
AU - Dusek, Ulrike
AU - Popa, Maria Elena
AU - Yao, Peng
AU - Shaikat, Anupam
AU - Qiu, Chenxi
AU - Winiger, Patrik
AU - van der Veen, Carina
AU - Eames, Thomas Callum
AU - Ribeiro, Natasha
AU - van der Werf, Guido R.
N1 - Funding Information:
Acknowledgements. This research was supported by the Dutch Research Council (NWO) (Vici scheme research programme, no. 016.160.324) and a KNAW Ammodo grant. The CO and CO2 isotope measurements were supported by the NWO project number 824.14.015. We owe great thanks to Natasha Ribeiro (Ed-uardo Mondlane University, Mozambique) and Franziska Stein-bruch (Wildlife Conservation Society Mozambique) for making the field measurements possible. We are also grateful to Hans Cornelis-sen and Richard van Logtestijn for their help and allowing us to use the FLARE facilities and to Cameron Yates and Jeremy Russel-Smith (Charles Darwin University, Australia) for their invaluable help with the shrub biomass calculations.
Funding Information:
Financial support. This work was funded by grants from KNAW Ammodo and the Dutch Research Council (NWO) (grant nos. 016.160.324 and 824.14.015).
Publisher Copyright:
© Author(s) 2022.
PY - 2022/3/3
Y1 - 2022/3/3
N2 - Landscape fires are a significant contributor to atmospheric burdens of greenhouse gases and aerosols. Although many studies have looked at biomass burning products and their fate in the atmosphere, estimating and tracing atmospheric pollution from landscape fires based on atmospheric measurements are challenging due to the large variability in fuel composition and burning conditions. Stable carbon isotopes in biomass burning (BB) emissions can be used to trace the contribution of C3 plants (e.g. trees or shrubs) and C4 plants (e.g. savanna grasses) to various combustion products. However, there are still many uncertainties regarding changes in isotopic composition (also known as fractionation) of the emitted carbon compared to the burnt fuel during the pyrolysis and combustion processes. To study BB isotope fractionation, we performed a series of laboratory fire experiments in which we burned pure C3 and C4 plants as well as mixtures of the two. Using isotope ratio mass spectrometry (IRMS), we measured stable carbon isotope signatures in the pre-fire fuels and post-fire residual char, as well as in the CO2, CO, CH4, organic carbon (OC), and elemental carbon (EC) emissions, which together constitute over 98 % of the post-fire carbon. Our laboratory tests indicated substantial isotopic fractionation in combustion products compared to the fuel, which varied between the measured fire products. CO2, EC, and residual char were the most reliable tracers of the fuel 13C signature. CO in particular showed a distinct dependence on burning conditions; flaming emissions were enriched in 13C compared to smouldering combustion emissions. For CH4 and OC, the fractionation was the other way round for C3 emissions (13C-enriched) and C4 emissions (13C-depleted). This indicates that while it is possible to distinguish between fires that were dominated by either C3 or C4 fuels using these tracers, it is more complicated to quantify their relative contribution to a mixed-fuel fire based on the δ13C signature of emissions. Besides laboratory experiments, we sampled gases and carbonaceous aerosols from prescribed fires in the Niassa Special Reserve (NSR) in Mozambique, using an unmanned aerial system (UAS)-mounted sampling set-up. We also provided a range of C3 : C4 contributions to the fuel and measured the fuel isotopic signatures. While both OC and EC were useful tracers of the C3-to-C4 fuel ratio in mixed fires in the lab, we found particularly OC to be depleted compared to the calculated fuel signal in the field experiments. This suggests that either our fuel measurements were incomprehensive and underestimated the C3 : C4 ratio in the field or other processes caused this depletion. Although additional field measurements are needed, our results indicate that C3-vs.-C4 source ratio estimation is possible with most BB products, albeit with varying uncertainty ranges.
AB - Landscape fires are a significant contributor to atmospheric burdens of greenhouse gases and aerosols. Although many studies have looked at biomass burning products and their fate in the atmosphere, estimating and tracing atmospheric pollution from landscape fires based on atmospheric measurements are challenging due to the large variability in fuel composition and burning conditions. Stable carbon isotopes in biomass burning (BB) emissions can be used to trace the contribution of C3 plants (e.g. trees or shrubs) and C4 plants (e.g. savanna grasses) to various combustion products. However, there are still many uncertainties regarding changes in isotopic composition (also known as fractionation) of the emitted carbon compared to the burnt fuel during the pyrolysis and combustion processes. To study BB isotope fractionation, we performed a series of laboratory fire experiments in which we burned pure C3 and C4 plants as well as mixtures of the two. Using isotope ratio mass spectrometry (IRMS), we measured stable carbon isotope signatures in the pre-fire fuels and post-fire residual char, as well as in the CO2, CO, CH4, organic carbon (OC), and elemental carbon (EC) emissions, which together constitute over 98 % of the post-fire carbon. Our laboratory tests indicated substantial isotopic fractionation in combustion products compared to the fuel, which varied between the measured fire products. CO2, EC, and residual char were the most reliable tracers of the fuel 13C signature. CO in particular showed a distinct dependence on burning conditions; flaming emissions were enriched in 13C compared to smouldering combustion emissions. For CH4 and OC, the fractionation was the other way round for C3 emissions (13C-enriched) and C4 emissions (13C-depleted). This indicates that while it is possible to distinguish between fires that were dominated by either C3 or C4 fuels using these tracers, it is more complicated to quantify their relative contribution to a mixed-fuel fire based on the δ13C signature of emissions. Besides laboratory experiments, we sampled gases and carbonaceous aerosols from prescribed fires in the Niassa Special Reserve (NSR) in Mozambique, using an unmanned aerial system (UAS)-mounted sampling set-up. We also provided a range of C3 : C4 contributions to the fuel and measured the fuel isotopic signatures. While both OC and EC were useful tracers of the C3-to-C4 fuel ratio in mixed fires in the lab, we found particularly OC to be depleted compared to the calculated fuel signal in the field experiments. This suggests that either our fuel measurements were incomprehensive and underestimated the C3 : C4 ratio in the field or other processes caused this depletion. Although additional field measurements are needed, our results indicate that C3-vs.-C4 source ratio estimation is possible with most BB products, albeit with varying uncertainty ranges.
UR - http://www.scopus.com/inward/record.url?scp=85131580747&partnerID=8YFLogxK
U2 - 10.5194/acp-22-2871-2022
DO - 10.5194/acp-22-2871-2022
M3 - Article
AN - SCOPUS:85131580747
SN - 1680-7316
VL - 22
SP - 2871
EP - 2890
JO - Atmospheric chemistry and physics
JF - Atmospheric chemistry and physics
IS - 4
ER -