Direct numerical simulation of gas transfer at the air-water interface in a buoyant-convective flow environment

Abstract

The gas transfer process across the air-water interface in a buoyant-convective environment has been investigated by Direct Numerical Simulation (DNS) to gain improved understanding of the mechanisms that control the process. The process is controlled by a combination of molecular diffusion and turbulent transport by natural convection. The convection when a water surface is cooled is combination of the Rayleigh-B´enard convection and the Rayleigh-Taylor instability. It is therefore necessary to accurately resolve the flow field as well as the molecular diffusion and the turbulent transport which contribute to the total flux. One of the challenges from a numerical point of view is to handle the very different levels of diffusion when solving the convection-diffusion equation. The temperature diffusion in water is relatively high whereas the molecular diffusion for most environmentally important gases is very low. This low molecular diffusion leads to steep gradients in the gas concentration, especially near the interface. Resolving the steep gradients is the limiting factor for an accurate resolution of the gas concentration field. Therefore a detailed study has been carried out to find the limits of an accurate resolution of the transport for a low diffusivity scalar. This problem of diffusive scalar transport was studied in numerous 1D, 2D and 3D numerical simulations. A fifth-order weighted non-oscillatory scheme (WENO) was deployed to solve the convection of the scalars, in this case gas concentration and temperature. The WENO-scheme was modified and tested in 1D scalar transport to work on non-uniform meshes. To solve the 2D and 3D velocity field the incompressible Navier-Stokes equations were solved on a staggered mesh. The convective terms were solved using a fourth-order accurate kinetic energy conserving discretization while the diffusive terms were solved using a fourth-order central method. The diffusive terms were discretized using a fourth-order central finite difference method for the second derivative. For the time-integration of the velocity field a second-order Adams-Bashworth method was employed. The Boussinesq approximation was employed to model the buoyancy due to temperature differences in the water. A linear relationship between temperature and density was assumed. A mesh sensitivity study found that the velocity field is fully resolved on a relatively coarse mesh as the level of turbulence is relatively low. However a finer mesh for the gas concentration field is required to fully capture the steep gradients that occur because of its low diffusivity. A combined dual meshing approach was used where the velocity field was solved on a coarser mesh and the scalar field (gas concentration and temperature) was solved on an overlaying finer submesh. The velocities were interpolated by a second-order method onto the finer sub-mesh. A mesh sensitivity study identified a minimum mesh size required for an accurate solution of the scalar field for a range of Schmidt numbers from Sc = 20 to Sc = 500. Initially the Rayleigh-B´enard convection leads to very fine plumes of cold liquid of high gas concentration that penetrate the deeper regions. High concentration areas remain in fine tubes that are fed from the surface. The temperature however diffuses much stronger and faster over time and the results show that temperature alone is not a good identifier for detailed high concentration areas when the gas transfer is investigated experimentally. For large timescales the temperature field becomes much more homogeneous whereas the concentration field stays more heterogeneous. However, the temperature can be used to estimate the overall transfer velocity KL. If the temperature behaves like a passive scalar a relation between Schmidt or Prandtl number and KL is evident. A qualitative comparison of the numerical results from this work to existing experiments was also carried out. Laser Induced Fluorescence (LIF) images of the oxygen concentration field and Schlieren photography has been compared to the results from the 3D simulations, which were found to be in good agreement. A detailed quantitative analysis of the process was carried out. A study of the horizontally averaged convective and diffusive mass flux enabled the calculation of transfer velocity KL at the interface. With KL known the renewal rate r for the so called surface renewal model could be determined. It was found that the renewal rates are higher than in experiments in a grid stirred tank. The horizontally averaged mean and fluctuating concentration profiles were analysed and from that the boundary layer thickness could be accurately monitored over time. A lot of this new DNS data obtained in this research might be inaccessible in experiments and reveal previously unknown details of the gas transfer at the air water interface.