A method for measuring methane oxidation rates using low levels of 14C-labeled methane and accelerator mass spectrometry

Mary A. Pack, Monica B. Heintz, William S. Reeburgh, Susan E. Trumbore, David L. Valentine, Xiaomei Xu, Ellen R. M. Druffel

Limnol. Oceanogr. Methods 9:245-260 (2011) | DOI: 10.4319/lom.2011.9.245

ABSTRACT: We report a new method for methane oxidation rate measurements that uses 103-105 times less 14C-CH4 than existing measurements by taking advantage of the high sensitivity of accelerator mass spectrometry. Methane oxidation in the marine environment is a microbial process of global importance because it prevents methane released from underlying reservoirs from reaching the ocean and atmosphere. Rate measurements provide a crucial tool for assessing the efficacy of this process across a range of environments, but the current methods use high amounts of radioactive elements (3H- or 14C-CH4), tend to increase methane concentrations in a sample markedly over in situ levels, and are limited by strict health and safety regulations. The low-level method presented here uses levels of 14C-CH4 that are below transportation regulations, produce samples that do not require treatment as radioactive waste, and allow for tracer level rate measurements in low methane environments. Moreover, the low-level method lays the analytical foundation for a below-regulation rate measurement that could be used broadly and in-situ. Parallel rate measurements with the low-level 14C-CH4 and existing 3H-CH4 methods are generally consistent with a correlation coefficient of 0.77. However, the low-level method in most cases yields slower rates than the 3H method possibly due to temperature, priming, and detection limit effects.