Pressure dependence of vibrational Raman scattering of narrow-band, 248-nm, laser light by H2, N2, O2, CO2, CH4, C2H6, and C3H8 as high as 97 bar

Gu, Yixin; Zhou, Yanhua; Tang, Hua; Rothe, Erhard W.; Reck, Gene P.

doi:10.1007/s003400000412

Cited by 28 publications

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“…We previously measured (Gu et al, 2000) Raman signals I j with the same apparatus from a number of high-pressure gaseous species j (up to 60 atm) and from SC-CO 2 (up to 97 atm). For a fixed apparatus geometry, I j increased linearly with the density q j , and with I 0 .…”

Section: Calibrationsmentioning

confidence: 99%

“…The KrF excimer laser is described elsewhere (Grü nefeld et al, 1996;Gu et al, 2000). The laser light has %1 cm À1 bandwidth, a % 13 ns pulse length, a % 1 mrad divergence, and was operated near 248.3 nm.…”

Section: Apparatusmentioning

confidence: 99%

“…In particular, this applied to CO 2 up to 97 bar. Figure 1 is a schematic of our apparatus, which was adapted from those previously described (Gu et al, 2000(Gu et al, , 2002Tang et al, 2001). It includes a tunable narrowband excimer laser, a beam energy detector, a high-pressure cell with optical access, an intensified imaging spectrometer, and appropriate control units.…”

mentioning

confidence: 99%

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Determination of Concentrations of Solutes in Gaseous, Liquid, and Supercritical Co₂by Means of UV Raman Spectroscopy

Tang

Gulari

Rothe

2005

Chemical Engineering Communications

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We measured compositions of high-pressure CO 2 solutions in vapor, liquid, and supercritical phases by means of UV-Raman spectra. Our goal was to investigate whether excimer-based Raman could quantitatively determine compositions of such solutions under high-pressure conditions. Some potential problems include (a) species that can absorb much, or all, of the UV-laser light, (b) fluorescence that might overwhelm the Raman signal, and (c) density gradients that would bend the laser beam. We studied two binary systems that were chosen to avoid such problems and that yielded quantitative composition analyses. These were (a) two-phase mixtures of CO 2 and n-pentane and (b) solutions of 1,1,1,2,3,4,4,5,5,5-decafluoropentane in CO 2 . We suggest some changes that could increase the usefulness of the method for future applications.

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Section: Calibrationsmentioning

confidence: 99%

Section: Apparatusmentioning

confidence: 99%

mentioning

confidence: 99%

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Determination of Concentrations of Solutes in Gaseous, Liquid, and Supercritical Co₂by Means of UV Raman Spectroscopy

Tang

Gulari

Rothe

2005

Chemical Engineering Communications

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“…The ability to monitor changes in these fundamental parameters with the DORISS is important in experiments that test the feasibility of sequestering CO 2 on the ocean floor. The Raman spectrum of CO 2 , in turn, is a moderately accurate monitor of its density, [22][23][24][25][26][27][28][29][30] and Raman spectroscopy can be used to determine the concentration and speciation (e.g., into CO 3 2Ϫ and HCO 3 Ϫ ) of CO 2 dissolved in water. [31][32][33] Our laboratory work 22 and that of others has shown that, as CO 2 density increases, the Raman band positions of both bands of the Fermi diad 34 downshift, whereas the spectral separation increases between these two bands.…”

Section: Fig 6 Comparison Of the Raman Spectra Of Deionized Water (mentioning

confidence: 99%

Feasibility of Large-Scale Ocean Co2 Sequestration

Brewer¹,

Barry²

2004

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ABSTRACT:The past year has been one of continued high productivity and technical innovation for research conducted under support of this contract. We report here on the successful completion of development of a deep-ocean laser Raman spectrometer, and the use of this novel system for direct in situ measurement of the dissolution rate of CO 2 from a N 2 /CO 2 gas mixture at 300m ocean depth. We have carried out the deepest ever ocean CO 2 injection experiment at 3960m depth, and have observed the behavior of the plume of low pH/high CO 2 water emanating from this source. This was made possible by the design, construction, and operation of a novel flume to contain the liquid CO 2 and to force flow in a controlled manner over the liquid CO 2 surface. In carrying out this experiment we observed for the first time the extraordinarily rapid hydration kinetics of CO 2 with water at high pressure. This initial observation was later confirmed in a carefully controlled series of acid and CO 2 injection studies at varying depths. In carrying out this research we are aware of the environmental concerns, and we have been in the forefront of identifying the challenges resulting from the far greater quantities of CO 2 being passively absorbed from the atmosphere. This quantity now is approximately 1 million metric tons CO 2 per hour, and reasonable projections for the 21 st century project ocean pH changes of 0.3 or more by mid-century. The PIs have played a key role in organizing a major international meeting on this topic, and on reporting the results. We are now engaged in developing the novel techniques required to investigate this problem. INTRODUCTIONThe primary mechanism preventing very fast accumulation of CO 2 in the atmosphere is ocean absorption through the sea surface. This absorption, driven by the accumulated mean pCO 2 difference between air and sea, now proceeds at a rate of about 1 million metric tons CO 2 per hour. Thus ocean passive "disposal" of fossil fuel CO 2 is the primary greenhouse gas control technique used by all nations at all times, and the accumulated oceanic fossil fuel burden is now ≅ 500 billion tons CO 2 . In the few years that CO 2 is resident in the atmosphere it affects the planetary radiation balance and contributes to global warming. Thus some 25 years ago it was first suggested that direct injection of CO 2 into the deep ocean, thus bypassing the atmospheric disposal step with its attendant global warming, would be a useful greenhouse gas control technology. We have investigated this process in a series of studies carried out in part through the support of this award. These have involved creation of advanced experimental techniques for injection of CO 2 into the deep ocean, the measurement of the fate and behavior of the injected liquid, the formation and dissolution of a solid hydrate, and the environmental consequences of both direct and indirect CO 2 injection into the ocean. EXECUTIVE SUMMARYIn this report we detail research carried out in the period October 1, 2003 through Septemb...

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“…The ability to monitor changes in these fundamental parameters with the DORISS is important in experiments that test the feasibility of sequestering CO 2 on the ocean floor. The Raman spectrum of CO 2 , in turn, is a moderately accurate monitor of its density, [22][23][24][25][26][27][28][29][30] and Raman spectroscopy can be used to determine the concentration and speciation (e.g., into CO 3 2-and H 2 CO 3 2-) of CO 2 dissolved in water. [31][32][33] Our laboratory work 22 and that of others has shown that, as CO 2 density increases, the Raman band positions of both the v 1 and 2v 2 bands of the Fermi diad 34 downshift, whereas the spectral separation increases between these two bands.…”

Section: Raman Spectra Of Carbon Dioxide Introduced Into the Deep Ocementioning

confidence: 99%

Final Progress Report: Direct Experiments on the Ocean Disposal of Fossil Fuel CO2.

Barry¹,

Brewer²

2004

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IntroductionFrom 2001 to early 2004, we performed field and laboratory experiments, and developed technology to investigate the feasibility and biological consequences of direct ocean CO2 injection as a sequestration strategy to mitigate rising levels of CO2 in the atmosphere. These activities were performed using support from the Monterey Bay Aquarium Research Institute (MBARI) and DoE, through the combined efforts of MBARI ships, ROVs, and science, engineering and operations personnel. DoE support included funding from NETL (Award DE-FC26-00NT40929 :Feasibility of large-scale ocean CO2 sequestration -Drs. Brewer and Barry) and DoE Office of Science Award DE-FG03-01DF63065 (Direct Experiments on the Ocean Disposal of Fossil Fuel CO 2 -Drs. Barry and Brewer). Activities supported by the Office of Science award were intertwined closely with those funded by NETL and MBARI, but were associated most closely studies by postdoctoral fellows. The major results of activities supported by the NETL award are listed in the attached technical progress report which includes several scholarly publications related to this research. Field ExperimentsSeveral deep-sea field experiments were performed off the California coast during 2001 to 2003. Each of these experiments involved a logistically complicated process of pressurizing and transporting small quantities (~20 to 150 l) of liquid CO2 to the seafloor using the ROV Tiburon, launched from the R/V Western Flyer, operated by MBARI. Five of these small-scale CO2 release experiments were used to evaluate the response of deep-sea organisms to changes in seawater chemistry caused by the addition of CO2 to the ocean. During each experiment, small pools of liquid CO2 were created on the seafloor, after which the CO2 would dissolve slowly into seawater, carrying a CO2-rich dissolution plume downstream over sediments inhabited by infaunal organisms and past small cages holding experimental animals. Changes in seawater chemistry were detected mainly by pH meters; the addition of CO2 to seawater elevates its CO2 levels, and reduces its pH (i.e. increases the acidity of seawater). We assessed the survival of various organisms (microbes, meiofauna [nematodes, amoebae, flagellates], macrofauna [sediment-dwelling worms and crustaceans], and megafauna [snails, sea urchins, sea cucumbers, octopus, fish] during month-long exposure to elevated CO2 levels in the dissolution plumes.The major results of these field experiments indicates that direct ocean injection of CO2 in the deep-sea will have variable, but generally negative effects on deep-sea ecosystems. Elevated CO2 levels cause physiological stress in many marine organisms, including respiratory stress, acidosis of intra-and inter-cellular spaces, and narcosis. The severity of effects on individual physiology vary among taxa, with echinoderms as the most sensitive taxon studies. The potential consequences for population and species level effects remain unknown. Effects will be most pronounced near sites of CO2 release, and the severity and...

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Pressure dependence of vibrational Raman scattering of narrow-band, 248-nm, laser light by H2, N2, O2, CO2, CH4, C2H6, and C3H8 as high as 97 bar

Cited by 28 publications

References 0 publications

Determination of Concentrations of Solutes in Gaseous, Liquid, and Supercritical Co₂by Means of UV Raman Spectroscopy

Determination of Concentrations of Solutes in Gaseous, Liquid, and Supercritical Co₂by Means of UV Raman Spectroscopy

Feasibility of Large-Scale Ocean Co2 Sequestration

Final Progress Report: Direct Experiments on the Ocean Disposal of Fossil Fuel CO2.

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Pressure dependence of vibrational Raman scattering of narrow-band, 248-nm, laser light by H2, N2, O2, CO2, CH4, C2H6, and C3H8 as high as 97 bar

Cited by 28 publications

References 0 publications

Determination of Concentrations of Solutes in Gaseous, Liquid, and Supercritical Co2by Means of UV Raman Spectroscopy

Determination of Concentrations of Solutes in Gaseous, Liquid, and Supercritical Co2by Means of UV Raman Spectroscopy

Feasibility of Large-Scale Ocean Co2 Sequestration

Final Progress Report: Direct Experiments on the Ocean Disposal of Fossil Fuel CO2.

Contact Info

Product

Resources

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Determination of Concentrations of Solutes in Gaseous, Liquid, and Supercritical Co₂by Means of UV Raman Spectroscopy

Determination of Concentrations of Solutes in Gaseous, Liquid, and Supercritical Co₂by Means of UV Raman Spectroscopy