On quantifying global carbon emission from oil contaminated lands over centuries.

Petroleum releases into the subsurface contribute to global soil carbon emissions. Quantifying releases and changes in releases of carbon from soils over the lifetime of a spill is complex. Natural source zone depletion (NSZD) of light non-aqueous phase liquids (LNAPLs) embodies all key mechanisms for transformation to carbon gases and their release from soils including partitioning, transport and degradation of petroleum components. Quantification of the interconnected behaviours of the soil microbiome, fluid flow, multi-component transport, partitioning, and biodegradation is crucial for understanding NSZD. Volatilization from LNAPL, aerobic biodegradation, methanogenesis, and heat production all lead to release of greenhouse gases to the atmosphere. To estimate carbon emissions, using a validated computational platform, we modelled the long term NSZD of four petroleum hydrocarbon types; crude oil, diesel, jet fuel and gasoline, to span the major products used globally. For two soil types, we estimated 150 years of carbon emissions from annual minor and 25 mostly major petroleum hydrocarbon land release incidents since 1950 - with an estimated released mass of ~9 million tonnes across the circumstances considered. Up to 2100 the mass of carbon emitted to the atmosphere is estimated to range from 4 to 6 Teragrams, with nearly 60 % currently released. Nomographs generated help predict the fate of LNAPL plumes and carbon emissions due to NSZD, which is crucially important to management of soil and groundwater contamination. The method provides a basis to include additionally identified and future petroleum releases. It is noted that the petroleum mixture composition, degradation rates, volatilization, and subsurface characteristics all can influence carbon emission estimations.