Experiments on the ocean sequestration of fossil fuel CO2: pH measurements and hydrate formation

We have carried out a series of in situ experiments to investigate the formation of a CO₂ hydrate (CO₂:5.75 H₂O) for the purpose of evaluating scenarios for ocean fossil fuel CO₂ disposal with a solid hydrate as the sequestered form. The experiments were carried out with a remotely operated vehicle in Monterey Bay at a depth of 619 m. pH measurements made in close proximity to the hydrate–seawater interface showed a wide range of values, depending upon the method of injection and the surface area of the hydrate formed. Rapid injection of liquid CO₂ into an inverted beaker to form a flocculant mass of hydrate resulted in pH initially as low as 4.5 within a few centimeters of the interface, decaying slowly over 1–2 h towards normal seawater values as dense CO₂ rich brine drained from the hydrate mass. In a second experiment, slower injection of the liquid CO₂ to produce a simple two-layer system with a near planar interface of liquid CO₂ with a thin hydrate film yielded pH values indistinguishable from the in situ ocean background level of 7.6. Both field and laboratory results now show that the dissolution rate of a mass of CO₂ hydrate in seawater is slow but finite.     

日本大沼湖沉积物碳氮比值、有机碳同位素特征及其近400年的古气候环境意义

通过对日本大沼湖沉积物样品总有机碳含量(TOC)及其稳定同位素、总氮含量(TN)和C/N值的测定,结合沉积岩芯火山灰和1℃年代,分析了大沼湖沉积物中有机质的来源,探讨了沉积物有机碳同位素的主要影响因素.结果表明:大沼湖沉积物中有机质主要来源于自生藻类,受陆源输入的影响较小;沉积物δ13C值指示了夏季温度的变化.过去400年来,大沼湖地区存在1660～ 1730年和1780～ 1860年两个明显的冷期,与邻近地区冰芯、树轮和湖泊沉积物记录的冷期基本一致,分别对应于Maunder和Dalton太阳黑子极小期.     

Redistribution of REE, Pb and U by supergene weathering studied from in-situ isotopic analyses of the Bangombé natural reactor, Gabon

The isotopic analyses of rare earth elements (REE), Pb and U in several kinds of minerals from the clay and black shale layers above the Bangombé natural reactor, Gabon, were performed using a sensitive high-resolution microprobe (SHRIMP) to investigate the migration and retardation processes of fission products released from the reactor. REE isotopic data of the secondary minerals found in clays and black shales show that most of fission products were effectively trapped in the clays and not distributed into the black shales over the clays, which reveals that the clays play an important role in preventing fission products from spreading.Zircon crystals in the clays heterogeneously contain high-U regions (up to 28.3 wt%) with normal ²³⁵U/²³⁸U ratios (=0.00725) and significant amounts of fissiogenic REE, which suggest the occurrence of significant chemical fractionation between REE and U during the dissolution of reactor uraninite and the recrystallization of secondary U minerals. The Pb data suggest that galena grains in the clays were also formed by the mixing of the two components during a recent alteration event, and that a significant amount of Pb was derived from 2.05-Ga-old original uraninite rather than reactor uraninite. The U-Pb systematics of zircon provide chronological information on the old igneous activity associated with the basement rock formation at 2.8 Ga and geochemical evidence of the incomplete mixing of independent Pb and U sources. This result is consistent with previous chronological results in this area.     

Rapid Identification of Water-Conducting Fractures Using a Trace Methane Gas Measurement

Identification of water-conducting fractures is important for the safety assessment of underground projects in crystalline rocks at geological disposal sites. We applied a portable methane gas analyzer by wavelength-scanned cavity ring-down spectroscopy to detect the water-conducting fractures in the underground tunnel of the Mizunami Underground Research Laboratory, central Japan. The tunnel is excavated in granite with CH₄-rich groundwater. Two approaches were taken to obtain the profile of CH₄ concentration along the gallery walls: (1) “Scan by walking” at the speed of 0.5 m/s and (2) monitoring for 30 s at 0.5 or 1 m intervals. In the Scan by walking approach, the peaks of the CH₄ concentration corresponded well with the occurrence of high water flow rate fractures. Thus, this method is useful for rapid identification of major water-conducting fractures. Monitoring at constant intervals takes more time than the Scan by walking approach; however, this method can largely detect occurrences of fractures with low fluid fluxes.     

Trans-boundary and in-country transport of air pollutants observed in Kobe,Japan by high frequent filter pack sampling method

The seasonal intensive sampling of gases and particulate matter in ambient air was conducted at the site established in urban area of Japan to study the seasonal difference of the temporal variation of gases and particulate matter concentrations in urban atmosphere as well as to illustrate the different transport regimes that impacts air pollutants. The sample was collected by the four-stage filter-pack method with 6-h interval for one week in four seasons (spring, summer, autumn and winter). The trans-boundary transport of air pollutants with high concentration was characteristically observed in the spring sampling. On the other hand, we could successfully detect the in-country transports of air pollutants in the summer sampling. Four-season’s intensive survey considered, we could show the characteristic transport of air pollutants to provide the episodic high concentration for ambient air in the urban area of Japan, and successfully illustrate the seasonal-dependent transport regimes to impact on air pollutants.     

Snow ripples and their contribution to the mass transport in drifting snow

Morphological characteristics of snow ripples formed by drifting snow were investigated as functions of wind velocity in a cold wind tunnel at -15 °C. Wave-length, wave height and migration rate of snow ripples increased from 5 to 20 cm, 3 to 5 mm and 1 to 8 cm/min, respectively, with increasing wind velocity from 5 to 7 m/s. Measured size distributions of snow particles in snow ripples showed sorting of large particles in ridges, suggesting that the snow ripple migration is caused by creeping of large particles. The snow drift rate caused by creep, that is, by the ripple migration, was estimated to amount, at least, to 6% of the total snow drift rate.     

Use of tsunami waveforms for earthquake source study

Tsunami waveforms recorded on tide gauges, like seismic waves recorded on seismograms, can be used to study earthquake source processes. The tsunami propagation can be accurately evaluated, since bathymetry is much better known than seismic velocity structure in the Earth. Using waveform inversion techniques, we can estimate the spatial distribution of coseismic slip on the fault plane from tsunami waveforms. This method has been applied to several earthquakes around Japan. Two recent earthquakes, the 1968 Tokachi-oki and 1983 Japan Sea earthquakes, are examined for calibration purposes. Both events show nonuniform slip distributions very similar to those obtained from seismic wave analyses. The use of tsunami waveforms is more useful for the study of unusual or old earthquakes. The 1984 Torishima earthquake caused unusually large tsunamis for its earthquake size. Waveform modeling of this event shows that part of the abnormal size of this tsunami is due to the propagation effect along the shallow ridge system. For old earthquakes, many tide gauge records exist with quality comparable to modern records, while there are only a few good quality seismic records. The 1944 Tonankai and 1946 Nankaido earthquakes are examined as examples of old events, and slip distributions are obtained. Such estimates are possible only using tsunami records. Since tide-gauge records are available as far back as the 1850s, use of them will provide unique and important information on long-term global seismicity.     

The correlation of whistler occurrence rate at a low latitude with thunderstorm activity at its conjugate region and with solar activity

The correlations of occurrence rate of whistlers in January during one solar cycle (1977–1987) at a low latitude station (Yamaoka, geomag. lat. 25°, L=1.26) with thunderstorm activity near its conjugate region and also with solar activity have been investigated, and it is found that the occurrence rate has no correlation with the lightning flashes near the conjugate point, while it is negatively correlated with solar activity. On the basis of these findings it is suggested that the ionospheric absorption is of major importance in the long-term variation of whistler occurrence rate, with the duct formation being of secondary effect, while the lightning activity is only a necessary condition for whistler occurrence.     

Measurements of wave normal direction of whistler mode signals in the ionosphere by means of the Rocket-Doppler technique

Wave normal directions of VLF signals propagating through the ionosphere can be determined by measuring Doppler frequency shift of the signals by means of rocket borne receivers. Two rockets were launched to detect the NWC signal of 22.3 kHz which was transmitted from Australia and propagated on two completely different paths, one being propagated through the Earth-ionosphere waveguide and up to the rocket, the other propagated down to the rocket by the whistler mode directly from the source in the opposite hemisphere. The wave normal directions of the latter mode were almost vertically downward in the ionosphere in the northern hemisphere, although substantial error was involved in the determination of the wave normal direction for a part of the upgoing flight of the rockets, due to the relative geometry of the directions of the rocket flight and the geomagnetic field. The effect of the horizontal gradients of the ionosphere on the above results were found to be not significant. From the experimental results it is concluded that field aligned ducts stretching down to the rocket altitudes did not exist, at least, during the rocket flights.     

Small Scale Field Study of an Ocean CO<Subscript>2</Subscript> Plume

We have carried out a small-scale (∼20 l) CO₂ sequestration experiment off northern California (684 m depth, ∼5°C, background ocean pH ∼7.7) designed as an initial investigation of the effects of physical forcing of the fluid, and the problem of sensing the formation of a low pH plume. The buoyant CO₂ was contained in a square frame 1.2 m high, exposing 0.21 m² to ocean flow. Two pH electrodes attached to the frame recorded the signal; a second frame placed 1.9 m south of the CO₂ pool was also equipped with two recording pH electrodes. An additional pH electrode was held in the ROV robotic arm to probe the fluid interface. Local water velocities of up to 40 cm sec⁻¹ were encountered, creating significant eddies within the CO₂ box, and forcing wavelets at the fluid interface. This resulted in rapid CO₂ dissolution, with all CO₂ being depleted in a little more than 2 days. The pH record from the sensor closest (∼10 cm) to the CO₂ showed many spikes of low pH water, the extreme value being ∼5.9. The sensor 1 m immediately below this showed no detectable response. The electrodes placed 1.9 m distant from the source also recorded very small perturbations. The results provide important clues for the design of future experiments for CO₂ disposal and biogeochemical impact studies. These include the need for dealing with the slow CO₂ hydration kinetics, better understanding of the fluid dynamics of the CO₂-water interface, and non-point source release designs to provide more constant, controlled local CO₂ enrichments within the experimental area. This revised version was published online in July 2006 with corrections to the Cover Date.