US20110186441A1 - Electrolytic recovery of retained carbon dioxide - Google Patents

Electrolytic recovery of retained carbon dioxide Download PDF

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Publication number
US20110186441A1
US20110186441A1 US13/012,319 US201113012319A US2011186441A1 US 20110186441 A1 US20110186441 A1 US 20110186441A1 US 201113012319 A US201113012319 A US 201113012319A US 2011186441 A1 US2011186441 A1 US 2011186441A1
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Prior art keywords
aqueous solution
carbon dioxide
amine
metal ions
electric potential
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Abandoned
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US13/012,319
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English (en)
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Christopher J. Lafrancois
Steven M. Schlasner
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Phillips 66 Co
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ConocoPhillips Co
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Priority to US13/012,319 priority Critical patent/US20110186441A1/en
Assigned to CONOCOPHILLIPS COMPANY reassignment CONOCOPHILLIPS COMPANY ASSIGNMENT OF ASSIGNORS INTEREST (SEE DOCUMENT FOR DETAILS). Assignors: SCHLASNER, STEVEN M., LAFRANCOIS, CHRISTOPHER J.
Publication of US20110186441A1 publication Critical patent/US20110186441A1/en
Assigned to PHILLIPS 66 COMPANY reassignment PHILLIPS 66 COMPANY ASSIGNMENT OF ASSIGNORS INTEREST (SEE DOCUMENT FOR DETAILS). Assignors: CONOCOPHILLIPS COMPANY
Abandoned legal-status Critical Current

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    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M8/00—Fuel cells; Manufacture thereof
    • H01M8/06—Combination of fuel cells with means for production of reactants or for treatment of residues
    • H01M8/0662—Treatment of gaseous reactants or gaseous residues, e.g. cleaning
    • H01M8/0668—Removal of carbon monoxide or carbon dioxide
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D53/00—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols
    • B01D53/14—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols by absorption
    • B01D53/1425—Regeneration of liquid absorbents
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D53/00—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols
    • B01D53/14—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols by absorption
    • B01D53/1456—Removing acid components
    • B01D53/1475—Removing carbon dioxide
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D53/00—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols
    • B01D53/34—Chemical or biological purification of waste gases
    • B01D53/96—Regeneration, reactivation or recycling of reactants
    • B01D53/965—Regeneration, reactivation or recycling of reactants including an electrochemical process step
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02A—TECHNOLOGIES FOR ADAPTATION TO CLIMATE CHANGE
    • Y02A50/00—TECHNOLOGIES FOR ADAPTATION TO CLIMATE CHANGE in human health protection, e.g. against extreme weather
    • Y02A50/20—Air quality improvement or preservation, e.g. vehicle emission control or emission reduction by using catalytic converters
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02C—CAPTURE, STORAGE, SEQUESTRATION OR DISPOSAL OF GREENHOUSE GASES [GHG]
    • Y02C20/00—Capture or disposal of greenhouse gases
    • Y02C20/40—Capture or disposal of greenhouse gases of CO2
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
    • Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
    • Y02E60/30—Hydrogen technology
    • Y02E60/50—Fuel cells

Definitions

  • Embodiments of the invention relate to methods and systems for electrolytic recovery of retained gasses from absorption liquid to regenerate the absorption liquid.
  • One approach to reducing emissions of carbon dioxide gas includes recovery of the carbon dioxide from power plants and other point sources. Such recovery depends on ability to remove or capture the carbon dioxide from other gasses. By example, sequestration of the carbon dioxide once captured provides ability to dispose of the carbon dioxide without creating atmospheric environmental issues.
  • a prior technique that enables the recovery of the carbon dioxide utilizes an amine solution that absorbs the carbon dioxide and is then regenerated by steam stripping.
  • generating steam by burning fossil fuels in order to release the carbon dioxide from the amine solution produces more carbon dioxide and contributes to operational costs making the recovery expensive.
  • Other problems associated with such prior systems include need to further purify an overhead containing the carbon dioxide released during the steam stripping to remove water and need to compress the carbon dioxide via inefficient as compression. Size of vessels required for the steam stripping can also limit ability to locate the prior systems where desired. Further, raising temperature of the amine solution with the steam stripping results in undesired increasing corrosiveness of the amine solution in contact with components of the system.
  • a method of capturing carbon dioxide from a gas mixture includes contacting an aqueous solution formed from amine and metal ions with the gas mixture thereby forming metallocarbamate complexes from the amine, the metal ions and the carbon dioxide. Separating the aqueous solution from unabsorbed constituents of the gas mixture occurs after the contacting. Applying an electric potential to the aqueous solution recovered by the separating causes dissociation of the metallocarbamate complexes in order to liberate the carbon dioxide for capture.
  • a method of capturing carbon dioxide from a gas mixture includes forming an aqueous solution by mixing monoethanolamine and copper ions from copper sulfate. Contacting the aqueous solution with the gas mixture forms metallocarbamate complexes from the monoethanolamine, the copper ions and the carbon dioxide. The method further includes separating the aqueous solution from unabsorbed constituents of the gas mixture after the contacting. Pumping the aqueous solution recovered by the separating increases pressure of the aqueous solution to above a first pressure associated with the contacting prior to applying an electric potential to the aqueous solution to liberate from the aqueous solution the carbon dioxide at a second pressure above the first pressure.
  • a method of capturing carbon dioxide from a gas mixture includes forming an aqueous solution by mixing amine and metal ions with less of the metal ions added on a mole basis than the amine. Contacting the aqueous solution with the gas mixture causes the aqueous solution to absorb the carbon dioxide. Separating the aqueous solution from unabsorbed constituents of the gas mixture occurs after the contacting.
  • the method includes applying an electric potential to the aqueous solution recovered by the separating such that throughout the applying of the electric potential one of the metal ions reacts with more than one molecule to facilitate liberation of the carbon dioxide and regeneration of the aqueous solution.
  • FIG. 1 is a schematic of a system for carbon dioxide capture, according to one embodiment.
  • FIG. 2 is an exemplary reaction pathway to enable capturing carbon dioxide, according to one embodiment.
  • FIG. 3 is a plot of carbon dioxide released by electrolysis from an aqueous solution, according to one embodiment.
  • Embodiments of the invention relate to capturing carbon dioxide.
  • a solution formed from metal ions combined with an amine reagent absorbs carbon dioxide from gas introduced into the solution.
  • Subsequent electrolysis of the solution results in dissociation of complexes formed upon the carbon dioxide being absorbed. The electrolysis thus liberates the carbon dioxide for capture and regenerates the solution for reuse.
  • FIG. 1 shows a system for carbon dioxide (CO 2 or “CO2”) capture that includes an absorber vessel 100 in which a gas mixture containing carbon dioxide enters via gas input 102 .
  • the gas mixture passes through the absorber vessel 100 and contacts a liquid solution formed from amine and metal “M” ions prior to exiting the absorber vessel 100 via gas output 104 as treated gas. Unabsorbed constituents of the gas mixture thus separate in the absorber vessel 100 from the solution after the contacting to provide the treated gas.
  • CO 2 carbon dioxide
  • the solution absorbs the carbon dioxide from the gas mixture such that the treated gas contains a lower concentration of the carbon dioxide than present in the gas mixture as introduced into the absorber vessel 100 at the gas input 102 .
  • flue gas defines the gas mixture, which thus may include between about 3% and about 30% carbon dioxide by volume and other exhaust gasses, such as about 70% to about 95% nitrogen.
  • passage of the gas mixture through the absorber 100 removes at least about 70%, at least about 80% or at least about 90% of the carbon dioxide from the gas mixture.
  • a rich liquid conduit 106 from the absorber vessel 100 couples the absorber vessel 100 with an optional pump 107 and an electrolysis cell 108 , which is used to regenerate the solution by releasing the carbon dioxide from complexes formed from the amine, the carbon dioxide and the metal ions.
  • the electrolysis cell 108 includes a counter electrode 110 and a working electrode 112 that supply an electric potential to the solution in the electrolysis cell 108 .
  • the working electrode 112 reduces metal in the complex resulting in release of the carbon dioxide.
  • a liquid-gas phase selective membrane may facilitate separation of the carbon dioxide from the solution upon the carbon dioxide being liberated from the complexes.
  • a carbon dioxide recovery outlet 114 of the electrolysis cell 108 captures the carbon dioxide liberated within the electrolysis cell 108 .
  • Controlling voltage applied during the electrolysis and selection of the counter and working electrodes 110 , 112 can avoid competing reactions and decomposition of water concurrent with the release of the carbon dioxide from the solution in the electrolysis cell 108 . While the voltage depends on reactant concentrations in the solution and composition of the electrodes 110 , 112 , the voltage in some embodiments cycles between about ⁇ 3 volts to about +3 volts. Alternating between positive and negative potentials about each minute, for example, ensures that the metal ions are not depleted from the solution as a result of precipitation or plating on the working electrode 112 .
  • the pump 107 in fluid communication with the solution inside the absorber vessel 100 and inside the electrolysis cell 108 functions to increase pressure of the solution that is fed to the electrolysis cell 108 to above a first pressure, such as ambient pressure, associated with the contacting inside the absorber vessel 100 .
  • a first pressure such as ambient pressure
  • the pump 107 maintains the solution inside the electrolysis cell 108 at sufficient elevated pressure such that the carbon dioxide is released at a second pressure, such as above about 6750 kilopascal, higher than the first pressure.
  • the carbon dioxide output through the recovery outlet 114 may not require further compression for transport or sequestration purposes due to use of the pump 107 .
  • a lean liquid line 116 couples the electrolysis cell 108 to the absorber vessel 100 to resupply the solution for more carbon dioxide absorption.
  • the lean liquid line 116 contains the solution formed from the amine and the metal ions with the carbon dioxide removed upon the solution being regenerated in the electrolysis cell 108 .
  • the solution thus cycles through the absorber vessel 100 and the electrolysis cell 108 for treating a stream of the gas mixture fed into the gas input 102 .
  • the amine used to form the solution includes a linear or noncyclical amine in water such that the solution is aqueous.
  • R 1 being C x H 2x OH and R 2 being one of hydrogen and C y H 2y OH, given x and y are from 1 to 8, or 2 to 4.
  • Specific alcohol amines that were tested and demonstrated suitability include monoethanolamine (MEA), diethanolamine (DEA), diisopropanolamine (DIPA) and diglycolamine (DGA).
  • linearity of the amine and the amine having at least one hydrogen atom bound to nitrogen of the amine helps ensure that the nitrogen remains sterically free and available for carbamate formation.
  • noncyclical formulas of the amine lack sites where the metal ion complexes for carbonate formation preferential to the carbamate formation during the carbon dioxide absorption. In operation, complexes formed by absorption of the carbon dioxide may thus not include carbonate groups.
  • the metal ions used to form the solution include at least one of copper, zinc, cobalt, nickel, aluminum and magnesium and may be di-cationic species.
  • the complexes formed from the amine, the metal ions and the carbon dioxide provide ionic charged species that are influenced by the electrical potential such that reduction is achieved at the working electrode 112 of the electrolysis cell 108 .
  • amine such as MEA
  • the metal ion proved inability for electrolytic release from the amine of the carbon dioxide absorbed. While possible to separate conductive mixtures like sodium hydroxide, the amine alone cannot achieve recovery of the carbon dioxide using electrolysis.
  • adding a metal salt to a reagent containing the amine forms the solution with the metal ions from the metal salt.
  • Selection of the metal salt depends on solubility of the metal salt and avoidance of anion interference with electrochemistry.
  • the metal salt include copper sulfate (CuSO 4 ) or copper perchlorate (Cu(ClO 4 ) 2 ).
  • a metal electrode such as the counter electrode 110 or a different disposable anode, within a reagent containing the amine supplies a source of the metal ions to form the solution upon electric current dissolving the metal electrode. Copper ions can for example come from use of the working electrode 110 if made from copper.
  • the solution is formed on a mole basis from less of the metal ions than the amine such that there is not a 1:1 stoichiometric quantity of the metal ions to the amine.
  • Each of the metal ions thus reacts with different molecules containing the amine throughout regeneration of the solution while applying the electric potential.
  • the forming of the solution includes mixing reagent of between about 10 percent and about 20 percent MEA in water with copper sulfate such that copper ions added are between about 1 mole percent and about 5 mole percent relative to the MEA.
  • FIG. 2 illustrates an exemplary reaction cycle 200 employed such as described with the system in FIG. 1 .
  • MEA copper ions and carbon dioxide react to form metallocarbamate complexes. Reduction of copper within the metallocarbamate complexes by electrolysis liberates the carbon dioxide, which is separated from the solution. Reversing electric potential oxidizes metallic copper or reduced copper ions for further formation of the metallocarbamate complexes upon reaction with additional carbon dioxide.
  • a solution for absorbing carbon dioxide was prepared by adding copper sulfate to a 15 percent aqueous solution of MEA such that copper was 3 mole percent relative to the MEA.
  • the solution was enriched with carbon dioxide through sparging.
  • An electric potential was then applied to the solution utilizing a carbon working electrode and a stainless steel counter electrode. Effluent gasses from the solution during application of the electric potential were collected and passed through a mass spectrometer for analysis.
  • FIG. 3 shows the carbon dioxide released based on a plot of ion current detected with the mass spectrometer as a function of time.
  • Data 300 corresponds to the carbon dioxide released from the solution increasing as voltage decreased from ⁇ 1 volts to ⁇ 5 volts prior to stopping application of the electric potential, at which point residual amounts of the carbon dioxide liberated were detected as the effluent gasses diminished to zero.
  • the effluent gas was also monitored with the mass spectrometer for hydrogen, which was not detected in the effluent gas throughout the time plotted.

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  • General Chemical & Material Sciences (AREA)
  • Chemical Kinetics & Catalysis (AREA)
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  • Oil, Petroleum & Natural Gas (AREA)
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US13/012,319 2010-01-29 2011-01-24 Electrolytic recovery of retained carbon dioxide Abandoned US20110186441A1 (en)

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US20130008800A1 (en) * 2011-07-06 2013-01-10 Liquid Light, Inc. Carbon dioxide capture and conversion to organic products
US20130186775A1 (en) * 2012-01-23 2013-07-25 Battelle Memorial Institute Separation and/or Sequestration Apparatus and Methods
US8500987B2 (en) 2010-03-19 2013-08-06 Liquid Light, Inc. Purification of carbon dioxide from a mixture of gases
US8524066B2 (en) 2010-07-29 2013-09-03 Liquid Light, Inc. Electrochemical production of urea from NOx and carbon dioxide
WO2013151809A1 (fr) * 2012-04-05 2013-10-10 Battelle Memorial Institute Systèmes et procédés d'élimination de composants d'un mélange de gaz
US8562811B2 (en) 2011-03-09 2013-10-22 Liquid Light, Inc. Process for making formic acid
US8568581B2 (en) 2010-11-30 2013-10-29 Liquid Light, Inc. Heterocycle catalyzed carbonylation and hydroformylation with carbon dioxide
US8592633B2 (en) 2010-07-29 2013-11-26 Liquid Light, Inc. Reduction of carbon dioxide to carboxylic acids, glycols, and carboxylates
US8641885B2 (en) 2012-07-26 2014-02-04 Liquid Light, Inc. Multiphase electrochemical reduction of CO2
US8647493B2 (en) 2012-07-26 2014-02-11 Liquid Light, Inc. Electrochemical co-production of chemicals employing the recycling of a hydrogen halide
US8663447B2 (en) 2009-01-29 2014-03-04 Princeton University Conversion of carbon dioxide to organic products
US8721866B2 (en) 2010-03-19 2014-05-13 Liquid Light, Inc. Electrochemical production of synthesis gas from carbon dioxide
US20140151240A1 (en) * 2012-11-30 2014-06-05 Alstom Technology Ltd Electroylytic reduction of carbon capture solutions
US8845878B2 (en) 2010-07-29 2014-09-30 Liquid Light, Inc. Reducing carbon dioxide to products
US8845877B2 (en) 2010-03-19 2014-09-30 Liquid Light, Inc. Heterocycle catalyzed electrochemical process
US8858777B2 (en) 2012-07-26 2014-10-14 Liquid Light, Inc. Process and high surface area electrodes for the electrochemical reduction of carbon dioxide
US8961774B2 (en) 2010-11-30 2015-02-24 Liquid Light, Inc. Electrochemical production of butanol from carbon dioxide and water
US9085827B2 (en) 2012-07-26 2015-07-21 Liquid Light, Inc. Integrated process for producing carboxylic acids from carbon dioxide
US9090976B2 (en) 2010-12-30 2015-07-28 The Trustees Of Princeton University Advanced aromatic amine heterocyclic catalysts for carbon dioxide reduction
US9267212B2 (en) 2012-07-26 2016-02-23 Liquid Light, Inc. Method and system for production of oxalic acid and oxalic acid reduction products
US9873951B2 (en) 2012-09-14 2018-01-23 Avantium Knowledge Centre B.V. High pressure electrochemical cell and process for the electrochemical reduction of carbon dioxide
WO2018031297A1 (fr) * 2016-08-09 2018-02-15 Nrgtek, Inc. Solvants et procédés de séparation de gaz à partir d'un flux gazeux
US9956522B2 (en) 2016-08-09 2018-05-01 Nrgtek, Inc. Moisture removal from wet gases
US9962656B2 (en) 2016-09-21 2018-05-08 Nrgtek, Inc. Method of using new solvents for forward osmosis
CN108701837A (zh) * 2015-12-17 2018-10-23 联邦科学与工业研究组织 酸性气体可再生电池
US10143970B2 (en) 2016-08-09 2018-12-04 Nrgtek, Inc. Power generation from low-temperature heat by hydro-osmotic processes
US10329676B2 (en) 2012-07-26 2019-06-25 Avantium Knowledge Centre B.V. Method and system for electrochemical reduction of carbon dioxide employing a gas diffusion electrode
US10384164B2 (en) 2016-11-04 2019-08-20 Nrgtek, Inc. Combined electrical and thermal renewable/conventional energy storage and on-demand hydro-osmotic power generation methods and systems
CN113578025A (zh) * 2021-08-20 2021-11-02 中南大学 一种烟气中二氧化碳的捕集方法及捕集系统

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Cited By (50)

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US8663447B2 (en) 2009-01-29 2014-03-04 Princeton University Conversion of carbon dioxide to organic products
US8986533B2 (en) 2009-01-29 2015-03-24 Princeton University Conversion of carbon dioxide to organic products
US9970117B2 (en) 2010-03-19 2018-05-15 Princeton University Heterocycle catalyzed electrochemical process
US8500987B2 (en) 2010-03-19 2013-08-06 Liquid Light, Inc. Purification of carbon dioxide from a mixture of gases
US8845877B2 (en) 2010-03-19 2014-09-30 Liquid Light, Inc. Heterocycle catalyzed electrochemical process
US20130292262A1 (en) * 2010-03-19 2013-11-07 Liquid Light, Inc. Purification of Carbon Dioxide from a Mixture of Gases
US8721866B2 (en) 2010-03-19 2014-05-13 Liquid Light, Inc. Electrochemical production of synthesis gas from carbon dioxide
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US8524066B2 (en) 2010-07-29 2013-09-03 Liquid Light, Inc. Electrochemical production of urea from NOx and carbon dioxide
US8592633B2 (en) 2010-07-29 2013-11-26 Liquid Light, Inc. Reduction of carbon dioxide to carboxylic acids, glycols, and carboxylates
US8568581B2 (en) 2010-11-30 2013-10-29 Liquid Light, Inc. Heterocycle catalyzed carbonylation and hydroformylation with carbon dioxide
US8961774B2 (en) 2010-11-30 2015-02-24 Liquid Light, Inc. Electrochemical production of butanol from carbon dioxide and water
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