1 Bubbles attenuate elastic waves at seismic frequencies: first experimental 2 evidence 3 4 Nicola Tisato1*, Beatriz Quintal2, Samuel Chapman2, Yury Podladchikov2, and Jean-Pierre Burg3 5 6 Supporting Information. Methods: 7 8 Laboratory experiments 9 The Broad Band Attenuation Vessel (BBAV) was employed to measure seismic attenuation, in 10 extensional-mode, in water- (Fig. 2a) and water-glycerin- (Fig. 2b) saturated Berea sandstone 11 (BS) samples. The solid frame of the samples can be considered homogeneous at the sample 12 scale and isotropic [Madonna et al., 2013]. The specimens were named: BS4, BS5 and BS3, with 13 a permeability of 200, 100 and 1000 mD, and porosity: 0.2, 0.18 and 0.21, respectively. The 14 samples were sealed with an aluminum foil glued onto their curved surface and a plastic shrink- 15 tube (jacket). Such device impeded a free-flow boundary condition that might bias the 16 measurements [Dunn, 1986; Yin et al, 1992]. The sample was confined with oil up to 23.7 MPa, 17 and an additional vertical stress, ranging between 1 and 2 MPa, was applied on the top of the 18 specimen to ensure the good coupling between the specimen and the sample holders. 19 Attenuation measurements were performed utilizing the force-oscillation (i.e sub-resonance) 20 method [McKavanagh and Stacey, 1974]. A piezoelectric motor served to cyclically vary the 21 vertical stress causing a strain of ~1.5×10-6. The analyzed frequencies were logarithmically 22 spaced between 0.1 and 100 Hz. The attenuation ( 1 Q E ) was calculated as: 23 1 QE tan (7) 24 where is the phase shift between vertical stress and strain. The Young’s modulus (E) equals: 25 E 26 where pp and pp are the vertical peak-to-peak stress and strain, respectively. 27 Stress-induced fluid pressure measurements were performed with the sample BS4 saturated with 28 water and air (Fig. 1b). Confining pressure was varied with a rate of 0.82±0.2 MPa s-1 and fluid 29 pressure was measured by means of a manometer connected to the top of the specimen. Both 30 confining and fluid pressure were recorder at 1000 Hz sampling rate with an accuracy of 31 ±0.01 MPa. 32 The BBAV was also equipped to measure transient fluid pressure caused by the oscillatory 33 differential stress applied on top of the sample (Fig. 1a) [Tisato and Quintal, 2013]. Up to 5 34 pressure sensors, able to sense pressure variations in less than 50 µs, were laterally introduced 35 into the sample BS3 saturated with 97% water. Sensors were 200 kPa full scale and vertically 36 spaced of ~4.2 cm. The 5 mm diameter sensor holes were sealed to reduce the free space 37 between the sensor and the inner wall of the hole limiting the artificial porosity introduced by the 38 presence of the sensors. More details on the methods employed to measure attenuation and 39 transient fluid pressure are reported in the literature [Tisato and Madonna, 2012; Tisato and 40 Quintal, 2013]. pp cos pp (8) 41 42 Numerical experiments 43 The deformation caused by an external sinusoidal hydrostatic pressure applied on a water 44 volume (198×198×198 μm) containing a micrometric spherical CO2 bubble (18 μm diameter) 45 (i.e. water-bubble-volume) was calculated solving three differential equations with an explicit 46 finite difference Eulerian-time-marching scheme. The equations consider i) the elastic 47 deformation of the bubble, ii) the dynamic dissolution of the gas in the surrounding liquid and 48 iii) the diffusion of the gas in the surrounding water. The bubble dissolution rate ( dn dt ) and the 49 rate of change of the bubble radius ( dr dt ) are calculated according eqs. 1 and 2. The diffusion 50 of the gas in the surrounding water is calculated according to the Fick’s law [Cussler, 1997], 51 which was solved in spherical coordinates. 52 The external pressure exerted on the system was given as Pf : 53 Pf Pfi Pf sin(2 f t ) cW k Hpc 2 / r Pf sin(2 f t ) 54 where Pfi is the initial fluid pressure (i.e. equilibrium or injection pressure), ΔPf the amplitude of 55 the sinusoidal fluid pressure (Fig. 1a) and f the frequency. To numerically solve eq. 1, 2 and the 56 diffusion of the gas in the liquid we considered time (t) between 0 and 2/f and frequency (f) 57 between 0.1 and 100 Hz. Time and f were discretized in 1024 and 32 steps, respectively. 58 At t=0 the code calculated the equilibrium conditions and in particular the initial concentration of 59 gas in the water (cW(t=0)) imposing dn dt 0 . At each subsequent time step the code calculates 60 the bubble radius, the new concentration of gas in the water (cW(t>0)), and the volume of the 61 water whose deformation is considered proportional to its bulk modulus (KH2O). The total 62 volume (V) is given by the sum of the bubble and the water volume, and the volumetric strain 63 (εV) is calculated as: 64 V 65 where Vi is the initial volume (Vi=V(t=0)). Then the real and imaginary part of the bulk modulus 66 of the water-bubble-volume are calculated as: V Vi Vi (9) (10) Pˆf cos V ˆV (11) Pˆf sin V ˆV (12) 67 Re K f 68 Im K f 69 where P̂f and ˆV are the peak-to-peak amplitude of Pf and εV, respectively. V is the phase shift 70 between V and Pf, and it is calculated with a best fit procedure [Bourbié et al., 1987] 71 The complex effective Young’s modulus of the saturated Berea sandstone (E) and the related 72 attenuation (1/QE) are obtained using Kf and some petrophysical properties of the dry Berea 73 sandstone. In particular, the P-wave modulus was calculated as: 74 H 75 and the P-wave velocity as: 76 VP 77 where is the density of the saturated rock [Bourbié et al., 1987]. 78 The code was validated by fitting some results presented by Holocher et al., [2003]. We 79 simulated the “stagnant flow regime” where an air-gas-bubble is trapped in the subsurface 80 groundwater. Suddenly, the water column height and, as a consequence the pressure increases 81 causing the partial dissolution of the gas-bubble. The pressure increase is: 82 Pfval gh 83 where ρ is the water density (1000 kg m-3), h the water column increase [m], and g is the 84 gravitational acceleration (9.81 m s-2). 85 Holocher et al. [2003] considered instantaneous gas diffusion in the water surrounding the 86 bubble, thus we simulated two cases: 3K 1 1 H (13) (14) (15) 87 1) The gas diffuses instantaneously in the surrounding water; 88 2) The gas diffuses according to the Fick’s law as aforementioned. 89 Both the cases, calculated for 4 different h values (0.05, 0.35, 0.65 and 0.95 m), reach a steady 90 state after ~30 min similarly to what calculated by Holocher et al. [2003]. However, the second 91 case shows a slower dynamic (Figure S1), which is in agreement with the model as the diffusion 92 of the gas requires time to occur. 93 The simulation of wave propagation in the subsurface presenting a domain saturated with water 94 and CO2 microbubbles was performed by means of the two-dimensional (2D) numerical code 95 called Sofi2D [Bohlen, 2002]. The source function was a Ricker wavelet with center frequency 96 of 5 Hz. The viscoelasticity of the GZ was implemented as a third-order generalized standard 97 linear solid (GSLS) model with QP=25 at frequencies 2, 4 and 6 Hz. The characteristic 98 parameters for the spring stiffness and viscosity of the dashpots were assigned using the least- 99 squares optimization [Bohlen, 2002]. A fourth-order finite difference, time-explicit scheme was 100 employed to evaluate the displacement field in the nodes of the mesh. 101 102 Approximation of the critical frequency (fc) for WIGED 103 We combined equation 1, 4 and 9 obtaining: 104 dI 3RT DW r 105 . (16) 106 We calculated the time derivative of 9 and, combining it with 5, we obtained: 107 d R 2 f r Pf cos(2 f t ) 108 Finally, we equated the amplitudes of the harmonic oscillations in 16 and 17 and we obtained a 109 proxy for fc: Pf 2 / r 3RT DW cw k Hpc r Pfi Pf sin(2 f t ) 2 / r 3RT DW Pf sin(2 f t ) cw k Hpc k Hpc r (17) 110 f 3RT DW fc . 2 kHpc r 2 (18) 111 Considering the properties reported in table S1 fc ≈ 11 Hz which is less than half order of 112 magnitude higher than the attenuation peak frequency. 113 114 Supporting Information. Tables: 115 116 117 Table S1. Fluid and Berea sandstone properties utilized to calculate the attenuation caused by the 118 dynamic bubble exsolution-dissolution of CO2 in water [Hart and Wang, 1995; Cussler, 1997; 119 Tisato and Madonna, 2012; Tisato and Quintal, 2013]. 120 Supporting Information. Figures: 121 122 123 Figure S1. Validation of the numerical model: the radius (r) of the bubble as a function of time 124 has been calculated after that a step of pressure ( Pfval ) has been applied at time=0 min. The 125 “stagnant flow regime” data, presented by Holocher et al. [2003], are represented by the circles. 126 The two cases which have been modelled are shown by the continuum (case 1: no diffusion) and 127 the dashed (case 2: diffusion) line. 128 129 130 131 Figure S2. 2D model utilized to simulate wave propagation with and without the influence of the 132 WIGED mechanism. From the bottom to the top the lithologies are: i) basalt, ii) carbonates, iii) 133 anhydrites, and iv) sandstones. Velocities (VP and VS) and densities () are typical for the 134 lithologies [Jaeger et al., 2007]. We assumed that the carbonates represent a geological CO2 135 storage with injection point in the center of the model. The anhydrites are an imperfect seal and 136 the leakage creates an overlying gassy zone (GZ) saturated with water and CO2. For depth 137 <700 m we assume that the CO2 is a gas phase creating micrometric bubbles in the pores of the 138 sandstone [Span and Wagner, 1996; Cussler, 1997]. Under this circumstances the P-wave 139 attenuation of the GZ is 0.05 at 3.6 Hz (ii) and the VP dispersion is 180 m/s between 1 and 10 Hz 140 (Fig. 3e). An explosion generates a 5 HZ Ricker elastic signal at the source point and it is 141 recorder by the 6 receivers. 142 143 Supporting References 144 Dunn, K. J. (1986), Acoustic attenuation in fluid-saturated porous cylinders at low frequencies, 145 J. Acoust. Soc. Am., 79(6), 1709–1721. 146 Madonna, C., B. Quintal, M. Frehner, B. S. G. Almqvist, N. Tisato, M. Pistone, F. Marone, and 147 E. H. Saenger (2013), Synchrotron-based X-ray tomographic microscopy for rock physics 148 investigations, Geophysics, 78(1), D53–D64, doi:10.1190/geo2012-0113.1. 149 McKavanagh, B., and F. D. Stacey (1974), Mechanical hysteresis in rocks at low strain 150 amplitudes and seismic frequencies, Phys. Earth Planet. Inter., 8(3), 246–250.