Enhancing surface methane fluxes from an oligotrophic lake: exploring the microbubble hypothesis.

Exchange of the greenhouse gases carbon dioxide (CO2) and methane (CH4) across inland water surfaces is an important component of the terrestrial carbon (C) balance. We investigated the fluxes of these two gases across the surface of oligotrophic Lake Stechlin using a floating chamber approach. The normalized gas transfer rate for CH4 (k600,CH4) was on average 2.5 times higher than that for CO2 (k600,CO2) and consequently higher than Fickian transport. Because of its low solubility relative to CO2, the enhanced CH4 flux is possibly explained by the presence of microbubbles in the lake’s surface layer. These microbubbles may originate from atmospheric bubble entrainment or gas supersaturation (i.e., O2) or both. Irrespective of the source, we determined that an average of 145 L m(–2) d(–1) of gas is required to exit the surface layer via microbubbles to produce the observed elevated k600,CH4. As k600 values are used to estimate CH4 pathways in aquatic systems, the presence of microbubbles could alter the resulting CH4 and perhaps C balances. These microbubbles will also affect the surface fluxes of other sparingly soluble gases in inland waters, including O2 and N2.

[1]  John C Little,et al.  Predicting diffused-bubble oxygen transfer rate using the discrete-bubble model. , 2002, Water research.

[2]  H. Laudon,et al.  Variability of groundwater levels and total organic carbon in the riparian zone of a boreal catchment , 2011 .

[3]  Y. Prairie,et al.  A new pathway of freshwater methane emissions and the putative importance of microbubbles , 2013 .

[4]  Christian Steinberg,et al.  Use of GC and equilibrium calculations of CO2 saturation index to indicate whether freshwater bodies in north-eastern Germany are net sources or sinks for atmospheric CO2 , 1998 .

[5]  Ira Leifer,et al.  Modelling of bubble-mediated gas transfer: Fundamental principles and a laboratory test , 2007 .

[6]  I. Mammarella,et al.  Effects of cooling and internal wave motions on gas transfer coefficients in a boreal lake , 2014 .

[7]  M. Pace,et al.  Multiple approaches to estimating air‐water gas exchange in small lakes , 2010 .

[8]  Patrick M. Crill,et al.  Freshwater Methane Emissions Offset the Continental Carbon Sink , 2011, Science.

[9]  J. Downing,et al.  Plumbing the Global Carbon Cycle: Integrating Inland Waters into the Terrestrial Carbon Budget , 2007, Ecosystems.

[10]  J. Cole,et al.  Impact of chemically enhanced diffusion on dissolved inorganic carbon stable isotopes in a fertilized lake , 2006 .

[11]  Dieter M. Imboden,et al.  Bubble plume modeling for lake restoration , 1992 .

[12]  J. Greinert,et al.  Fate of rising methane bubbles in stratified waters: How much methane reaches the atmosphere? , 2006 .

[13]  S. Vagle,et al.  Upper ocean bubble measurements from the NE Pacific and estimates of their role in air‐sea gas transfer of the weakly soluble gases nitrogen and oxygen , 2010 .

[14]  R. Wanninkhof Relationship between wind speed and gas exchange over the ocean , 1992 .

[15]  H. Grossart,et al.  Microbial methane production in oxygenated water column of an oligotrophic lake , 2011, Proceedings of the National Academy of Sciences.

[16]  John W. Kanwisher,et al.  On the exchange of gases between the atmosphere and the sea , 1963 .

[17]  B. Jähne,et al.  On the parameters influencing air‐water gas exchange , 1987 .

[18]  D. Serça,et al.  Gas transfer velocities of CO2 and CH4 in a tropical reservoir and its river downstream , 2007 .

[19]  R. Glud Oxygen dynamics of marine sediments , 2008 .

[20]  W. Eugster,et al.  Methane emissions from a small wind shielded lake determined by eddy covariance, flux chambers, anchored funnels, and boundary model calculations: a comparison. , 2012, Environmental science & technology.

[21]  P. Claus,et al.  Characterization of methanogenic Archaea and stable isotope fractionation during methane production in the profundal sediment of an oligotrophic lake (Lake Stechlin, Germany) , 2007 .

[22]  R. Conrad,et al.  Hydrogen, carbon monoxide, and methane dynamics in Lake Constance , 1993 .

[23]  Jonathan J. Cole,et al.  Atmospheric exchange of carbon dioxide in a low‐wind oligotrophic lake measured by the addition of SF6 , 1998 .

[24]  H. Grossart,et al.  Paradox reconsidered: Methane oversaturation in well‐oxygenated lake waters , 2014 .

[25]  R. Wanninkhof,et al.  Chemical enhancement of CO2 exchange in natural waters , 1996 .

[26]  W. Shuster,et al.  Controls on gas transfer velocities in a large river , 2012 .

[27]  S. Doney,et al.  Riverine coupling of biogeochemical cycles between land, oceans, and atmosphere , 2011 .

[28]  John M. Melack,et al.  Photosynthetic rates of phytoplankton in East African alkaline, saline lakes1 , 1974 .

[29]  E. D’Asaro,et al.  The Kolmogorov constant for the Lagrangian velocity spectrum and structure function , 2002 .

[30]  R. Betts,et al.  Changes in Atmospheric Constituents and in Radiative Forcing. Chapter 2 , 2007 .

[31]  D. Bastviken,et al.  Determination of the piston velocity for water‐air interfaces using flux chambers, acoustic Doppler velocimetry, and IR imaging of the water surface , 2013 .

[32]  D. Farmer,et al.  Bubble Clouds and Langmuir Circulation: Observations and Models , 2003 .

[33]  Mark Schmidt,et al.  Discovery of a natural CO2 seep in the German North Sea: Implications for shallow dissolved gas and seep detection , 2011 .

[34]  Andreas Richter,et al.  The boundless carbon cycle , 2009 .

[35]  W. R. Turner Microbubble Persistence in Fresh Water , 1960 .

[36]  J. Cole,et al.  The relationship between near‐surface turbulence and gas transfer velocity in freshwater systems and its implications for floating chamber measurements of gas exchange , 2010 .

[37]  R. Wanninkhof,et al.  � 2003, by the American Society of Limnology and Oceanography, Inc. Gas transfer velocities measured at low wind speed over a lake , 2022 .

[38]  G. Nützmann,et al.  Net groundwater inflow in an enclosed lake: from synoptic variations to climatic projections , 2013 .

[39]  S. MacIntyre,et al.  Buoyancy flux, turbulence, and the gas transfer coefficient in a stratified lake , 2010 .

[40]  John M. Melack,et al.  Lakes and reservoirs as regulators of carbon cycling and climate , 2009 .

[41]  J. Simpson,et al.  A novel technique for measuring the rate of turbulent dissipation in the marine environment , 2006 .

[42]  Tobias Steinhoff,et al.  In situ Quality Assessment of a Novel Underwater pCO2 Sensor Based on Membrane Equilibration and NDIR Spectrometry , 2014 .

[43]  D. D. Adams,et al.  An approach to understanding a temperate oligotrophic lowland lake (Lake Stechlin, Germany) , 2003 .

[44]  Jin Wu,et al.  Bubble populations and spectra in near‐surface ocean: Summary and review of field measurements , 1981 .

[45]  L. Merlivat,et al.  Gas exchange across an air‐water interface: Experimental results and modeling of bubble contribution to transfer , 1983 .

[46]  P. Crill,et al.  Automated flux chamber for investigating gas flux at water-air interfaces. , 2013, Environmental science & technology.

[47]  F. Chapin,et al.  CO2 exchange between air and water in an Arctic Alaskan and midlatitude Swiss lake: Importance of convective mixing , 2003 .

[48]  F. Peeters,et al.  Importance of the autumn overturn and anoxic conditions in the hypolimnion for the annual methane emissions from a temperate lake. , 2014, Environmental science & technology.