Combining ionic liquids and supercritical fluids: in situ ATR-IR study of CO2 dissolved in two ionic liquids at high pressures

Kazarian, Sergei G.; Briscoe, B.J.; Welton, Tom

doi:10.1039/b005514j

Cited by 422 publications

(379 citation statements)

References 13 publications

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“…As a first step we systematically computed the vibrational spectra of a H 2 O, CO 2 , and HCO 3 -in the gas phase as well as in a solvation shell corresponding to water at STP. The results are compatible with experiment: for water we find a downward shift of ~ 30cm -1 in the asymmetric stretch mode, while for CO 2 we find that solvation induces a splitting in the degenerate symmetric bend mode, just as observed experimentally [16]. For species like HCO 3 -the situation is more complicated, and our calculations predict that solvation induced shifts can be both positive and negative.…”

Section: Solvation Effects On the Vibrational Spectra Of Carbonatioussupporting

confidence: 79%

Enhancing the Atomic-Level Understanding of Co2 Mineral Sequestration Mechanisms via Advanced Computational Modeling

Chizmeshya¹

2003

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Fossil fuels currently provide 85% of the world's energy needs, with the majority coming from coal, due to its low cost, wide availability, and high energy content. The extensive use of coal-fired power assumes that the resulting CO 2 emissions can be vented to the atmosphere. However, exponentially increasing atmospheric CO 2 levels have brought this assumption under critical review. Over the last decade, this discussion has evolved from whether exponentially increasing anthropogenic CO 2 emissions will adversely affect the global environment, to the timing and magnitude of their impact. A variety of sequestration technologies are being explored to mitigate CO 2 emissions. These technologies must be both environmentally benign and economically viable. Mineral carbonation is an attractive candidate technology as it disposes of CO 2 as geologically stable, environmentally benign mineral carbonates, clearly satisfying the first criteria. The primary challenge for mineral carbonation is cost-competitive process development. CO 2 mineral sequestration − the conversion of stationary-source CO 2 emissions into mineral carbonates (e.g., magnesium and calcium carbonate, MgCO 3 and CaCO 3 ) − has recently emerged as one of the most promising sequestration options, providing permanent CO 2 disposal, rather than storage. In this approach a magnesium-bearing feedstock mineral (typically serpentine or olivine; available in vast quantities globally) is specially processed and allowed to react with CO 2 under controlled conditions. This produces a mineral carbonate which (i) is environmentally benign, (ii) already exists in nature in quantities far exceeding those that could result from carbonating the world's known fossil fuel reserves, and (iii) is stable on a geological time scale. Minimizing the process cost via optimization of the reaction rate and degree of completion is the remaining challenge.As members of the DOE/NETL managed National Mineral Sequestration Working Group we have already significantly improved our understanding of mineral carbonation. Group members at the Albany Research Center have recently shown that carbonation of olivine and serpentine, which naturally occurs over geological time (i.e., 100,000s of years), can be accelerated to near completion in hours. Further process refinement will require a synergetic science/engineering approach that emphasizes simultaneous investigation of both thermodynamic processes and the detailed microscopic, atomic-level mechanisms that govern carbonation kinetics.Our previously funded Phase I Innovative Concepts project demonstrated the value of advanced quantum-mechanical modeling as a complementary tool in bridging important gaps in our understanding of the atomic/molecular structure and reaction mechanisms that govern CO 2 mineral sequestration reaction processes for the model Mg-rich lamellar hydroxide feedstock material Mg(OH) 2 . In the present simulation project, improved techniques and more efficient computational schemes have allowed us to expand and au...

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Section: Solvation Effects On the Vibrational Spectra Of Carbonatioussupporting

confidence: 79%

Enhancing the Atomic-Level Understanding of Co2 Mineral Sequestration Mechanisms via Advanced Computational Modeling

Chizmeshya¹

2003

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“…The effect of the anion of the IL on the phase behavior can be explored by comparing two pairs of ILs that share common cations: [C 8 17 found no evidence of specific interactions of CO 2 with the cation. Thus, we do not attribute the high solubility of CO 2 in ILs to interaction with the acidic hydrogen in the 2-position of the imidazolium cation or with the nitrogens in the imidazolium or pyridinium rings.…”

Section: Discussionmentioning

confidence: 99%

High-Pressure Phase Behavior of Ionic Liquid/CO₂ Systems

2001

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This work presents the high-pressure phase behavior of CO 2 with six ionic liquids: 1-n-butyl-3-methylimidazolium hexafluorophosphate ([bmim] ]). We explored the effect of systematically changing the anionic and cationic components of the ionic liquid on the CO 2 -ionic liquid phase behavior. For all of the ionic liquids tested, large quantities of CO 2 dissolved in the ionic liquid phase, but no appreciable amount of ionic liquid solubilized in the CO 2 phase. In addition, the liquid phase volume expansion with the introduction of even large amounts of CO 2 is negligible, in dramatic contrast to the large volume expansion observed for neutral organic liquids. Our results seek to elucidate the underlying physical mechanisms of this highly unusual phase behavior.

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“…The solubility of CO2 in various RTILs has been extensively studied [2][3][4][5][6][7][8][9][10][11][12][13][14][15][16][17] and the structure of the binary mixture has been studied experimentally and theoretically. [18][19][20][21][22] On the other hand, reports on transport properties of these systems such as viscosity and diffusion are still limited in spite of their importance in designing chemical processes. How the dynamic properties of the mixture will change due to the dissolution of CO2 is also academically an interesting issue.…”

Section: Introductionmentioning

confidence: 99%

Transport Properties of Binary Mixtures of Carbon Dioxide and 1-Butyl-3-methylimidazolium Hexafluorophosphate Studied by Transient Grating Spectroscopy

2008

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Combining ionic liquids and supercritical fluids: in situ ATR-IR study of CO2 dissolved in two ionic liquids at high pressures

Abstract: An in situ ATR (attenuated total reflectance)-IR study of CO 2 dissolved in two ionic liquids at high pressures has demonstrated the effects of the anionic species of the ionic liquids on the molecular state of the dissolved CO 2 .

Cited by 422 publications

References 13 publications

Enhancing the Atomic-Level Understanding of Co2 Mineral Sequestration Mechanisms via Advanced Computational Modeling

Enhancing the Atomic-Level Understanding of Co2 Mineral Sequestration Mechanisms via Advanced Computational Modeling

High-Pressure Phase Behavior of Ionic Liquid/CO₂ Systems

Transport Properties of Binary Mixtures of Carbon Dioxide and 1-Butyl-3-methylimidazolium Hexafluorophosphate Studied by Transient Grating Spectroscopy

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Combining ionic liquids and supercritical fluids: in situ ATR-IR study of CO2 dissolved in two ionic liquids at high pressures

Abstract: An in situ ATR (attenuated total reflectance)-IR study of CO 2 dissolved in two ionic liquids at high pressures has demonstrated the effects of the anionic species of the ionic liquids on the molecular state of the dissolved CO 2 .

Cited by 422 publications

References 13 publications

Enhancing the Atomic-Level Understanding of Co2 Mineral Sequestration Mechanisms via Advanced Computational Modeling

Enhancing the Atomic-Level Understanding of Co2 Mineral Sequestration Mechanisms via Advanced Computational Modeling

High-Pressure Phase Behavior of Ionic Liquid/CO2 Systems

Transport Properties of Binary Mixtures of Carbon Dioxide and 1-Butyl-3-methylimidazolium Hexafluorophosphate Studied by Transient Grating Spectroscopy

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High-Pressure Phase Behavior of Ionic Liquid/CO₂ Systems