Methane cycling in the carbonate critical zone.
Sci Total Environ
; 899: 165645, 2023 Nov 15.
Article
em En
| MEDLINE
| ID: mdl-37474066
ABSTRACT
The carbonate critical zone (CZ) is characterized by extensive groundwater-surface water exchange that leads to highly variable redox states of groundwater. Changes in redox condition may cause either production or consumption of methane (CH4), thereby providing an atmospheric source or sink of this important greenhouse gas. To assess how groundwater-surface water exchange affects redox state and CH4 cycling in the carbonate CZ, we measured CH4 concentrations and 13C isotopes in water from streams, spring systems, and wells in north-central Florida. Sampled groundwater has subsurface residence times ranging from hours at a stream sink-rise system, to months following a flood recharge event into a spring vent, to decades at springs with limited point recharge. Concentrations of CH4 ranged from 0.002 to 89 µM, with an inverse relationship in springs between subsurface residence time and CH4 concentration. Where residence time is short, low CH4 concentrations result from methanotrophy linked to elevated dissolved oxygen (DO) concentrations. Following flooding, methanotrophy occurs soon after recharge and is followed by methanogenesis as groundwater becomes increasingly reducing. Groundwater extracted from wells had CH4 concentrations greater than spring water indicating CH4 is lost during flow to spring vents. CH4 concentrations covary with δ13C-CH4 values, which supports both methanogenesis and methanotrophy with changing residence times. Mean fluxes of CH4 ranged from -0.05 to 1.0 mg m-2 d-1 at spring vents, with negative values caused by CH4 uptake in water undersaturated with respect to atmospheric concentration. Most springs are dominated by methanotrophy, limiting atmospheric evasion of CH4 produced in the carbonate CZ. We estimate CH4 emissions to be 12.6 × 10-6 Tg a-1 across all Florida springs or about two orders of magnitude less than emissions from Floridan aquifer groundwater abstraction (3041 × 10-6 Tg a-1). Although CH4 is produced in the carbonate CZ, natural attenuation limits its effects on the global carbon cycle.
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MEDLINE
Idioma:
En
Ano de publicação:
2023
Tipo de documento:
Article