WO2007041872B1 - Continuous co-current electrochemical reduction of carbon dioxide - Google Patents

Continuous co-current electrochemical reduction of carbon dioxide

Info

Publication number
WO2007041872B1
WO2007041872B1 PCT/CA2006/001743 CA2006001743W WO2007041872B1 WO 2007041872 B1 WO2007041872 B1 WO 2007041872B1 CA 2006001743 W CA2006001743 W CA 2006001743W WO 2007041872 B1 WO2007041872 B1 WO 2007041872B1
Authority
WO
WIPO (PCT)
Prior art keywords
anolyte
cathode
catholyte
recycling
carbon dioxide
Prior art date
Application number
PCT/CA2006/001743
Other languages
French (fr)
Other versions
WO2007041872A1 (en
Inventor
Colin Oloman
Hui Li
Original Assignee
Colin Oloman
Hui Li
Priority date (The priority date is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the date listed.)
Filing date
Publication date
Application filed by Colin Oloman, Hui Li filed Critical Colin Oloman
Priority to AU2006301857A priority Critical patent/AU2006301857A1/en
Priority to US12/090,052 priority patent/US20080223727A1/en
Priority to CN2006800378108A priority patent/CN101657568B/en
Priority to CA2625656A priority patent/CA2625656C/en
Priority to EP06804642A priority patent/EP1951933A4/en
Priority to JP2008534843A priority patent/JP2009511740A/en
Publication of WO2007041872A1 publication Critical patent/WO2007041872A1/en
Publication of WO2007041872B1 publication Critical patent/WO2007041872B1/en
Priority to US14/244,869 priority patent/US20140299482A1/en
Priority to US14/851,745 priority patent/US20160068974A1/en

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    • 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
    • B01D53/32—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 electrical effects other than those provided for in group B01D61/00
    • B01D53/326—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 electrical effects other than those provided for in group B01D61/00 in electrochemical cells
    • C—CHEMISTRY; METALLURGY
    • C25—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES; APPARATUS THEREFOR
    • C25B—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES FOR THE PRODUCTION OF COMPOUNDS OR NON-METALS; APPARATUS THEREFOR
    • C25B11/00—Electrodes; Manufacture thereof not otherwise provided for
    • C25B11/02—Electrodes; Manufacture thereof not otherwise provided for characterised by shape or form
    • C25B11/03—Electrodes; Manufacture thereof not otherwise provided for characterised by shape or form perforated or foraminous
    • C25B11/031—Porous electrodes
    • C—CHEMISTRY; METALLURGY
    • C25—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES; APPARATUS THEREFOR
    • C25B—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES FOR THE PRODUCTION OF COMPOUNDS OR NON-METALS; APPARATUS THEREFOR
    • C25B11/00—Electrodes; Manufacture thereof not otherwise provided for
    • C25B11/04—Electrodes; Manufacture thereof not otherwise provided for characterised by the material
    • C—CHEMISTRY; METALLURGY
    • C25—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES; APPARATUS THEREFOR
    • C25B—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES FOR THE PRODUCTION OF COMPOUNDS OR NON-METALS; APPARATUS THEREFOR
    • C25B11/00—Electrodes; Manufacture thereof not otherwise provided for
    • C25B11/04—Electrodes; Manufacture thereof not otherwise provided for characterised by the material
    • C25B11/042—Electrodes formed of a single material
    • C25B11/043—Carbon, e.g. diamond or graphene
    • C25B11/044—Impregnation of carbon
    • C—CHEMISTRY; METALLURGY
    • C25—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES; APPARATUS THEREFOR
    • C25B—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES FOR THE PRODUCTION OF COMPOUNDS OR NON-METALS; APPARATUS THEREFOR
    • C25B11/00—Electrodes; Manufacture thereof not otherwise provided for
    • C25B11/04—Electrodes; Manufacture thereof not otherwise provided for characterised by the material
    • C25B11/051—Electrodes formed of electrocatalysts on a substrate or carrier
    • C—CHEMISTRY; METALLURGY
    • C25—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES; APPARATUS THEREFOR
    • C25B—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES FOR THE PRODUCTION OF COMPOUNDS OR NON-METALS; APPARATUS THEREFOR
    • C25B11/00—Electrodes; Manufacture thereof not otherwise provided for
    • C25B11/04—Electrodes; Manufacture thereof not otherwise provided for characterised by the material
    • C25B11/051—Electrodes formed of electrocatalysts on a substrate or carrier
    • C25B11/073—Electrodes formed of electrocatalysts on a substrate or carrier characterised by the electrocatalyst material
    • C25B11/075—Electrodes formed of electrocatalysts on a substrate or carrier characterised by the electrocatalyst material consisting of a single catalytic element or catalytic compound
    • C—CHEMISTRY; METALLURGY
    • C25—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES; APPARATUS THEREFOR
    • C25B—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES FOR THE PRODUCTION OF COMPOUNDS OR NON-METALS; APPARATUS THEREFOR
    • C25B11/00—Electrodes; Manufacture thereof not otherwise provided for
    • C25B11/04—Electrodes; Manufacture thereof not otherwise provided for characterised by the material
    • C25B11/051—Electrodes formed of electrocatalysts on a substrate or carrier
    • C25B11/073—Electrodes formed of electrocatalysts on a substrate or carrier characterised by the electrocatalyst material
    • C25B11/091—Electrodes formed of electrocatalysts on a substrate or carrier characterised by the electrocatalyst material consisting of at least one catalytic element and at least one catalytic compound; consisting of two or more catalytic elements or catalytic compounds
    • C—CHEMISTRY; METALLURGY
    • C25—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES; APPARATUS THEREFOR
    • C25B—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES FOR THE PRODUCTION OF COMPOUNDS OR NON-METALS; APPARATUS THEREFOR
    • C25B13/00—Diaphragms; Spacing elements
    • C25B13/04—Diaphragms; Spacing elements characterised by the material
    • C25B13/08—Diaphragms; Spacing elements characterised by the material based on organic materials
    • C—CHEMISTRY; METALLURGY
    • C25—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES; APPARATUS THEREFOR
    • C25B—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES FOR THE PRODUCTION OF COMPOUNDS OR NON-METALS; APPARATUS THEREFOR
    • C25B15/00—Operating or servicing cells
    • C25B15/02—Process control or regulation
    • C—CHEMISTRY; METALLURGY
    • C25—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES; APPARATUS THEREFOR
    • C25B—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES FOR THE PRODUCTION OF COMPOUNDS OR NON-METALS; APPARATUS THEREFOR
    • C25B15/00—Operating or servicing cells
    • C25B15/08—Supplying or removing reactants or electrolytes; Regeneration of electrolytes
    • C—CHEMISTRY; METALLURGY
    • C25—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES; APPARATUS THEREFOR
    • C25B—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES FOR THE PRODUCTION OF COMPOUNDS OR NON-METALS; APPARATUS THEREFOR
    • C25B3/00—Electrolytic production of organic compounds
    • C25B3/20—Processes
    • C25B3/25—Reduction
    • C—CHEMISTRY; METALLURGY
    • C25—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES; APPARATUS THEREFOR
    • C25B—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES FOR THE PRODUCTION OF COMPOUNDS OR NON-METALS; APPARATUS THEREFOR
    • C25B9/00—Cells or assemblies of cells; Constructional parts of cells; Assemblies of constructional parts, e.g. electrode-diaphragm assemblies; Process-related cell features
    • C25B9/17—Cells comprising dimensionally-stable non-movable electrodes; Assemblies of constructional parts thereof
    • C25B9/19—Cells comprising dimensionally-stable non-movable electrodes; Assemblies of constructional parts thereof with diaphragms
    • C—CHEMISTRY; METALLURGY
    • C25—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES; APPARATUS THEREFOR
    • C25B—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES FOR THE PRODUCTION OF COMPOUNDS OR NON-METALS; APPARATUS THEREFOR
    • C25B9/00—Cells or assemblies of cells; Constructional parts of cells; Assemblies of constructional parts, e.g. electrode-diaphragm assemblies; Process-related cell features
    • C25B9/40—Cells or assemblies of cells comprising electrodes made of particles; Assemblies of constructional parts thereof
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D2257/00—Components to be removed
    • B01D2257/50—Carbon oxides
    • B01D2257/504—Carbon dioxide
    • 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
    • Y02P—CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
    • Y02P20/00—Technologies relating to chemical industry
    • Y02P20/151—Reduction of greenhouse gas [GHG] emissions, e.g. CO2

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  • Chemical & Material Sciences (AREA)
  • Engineering & Computer Science (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Electrochemistry (AREA)
  • Organic Chemistry (AREA)
  • Materials Engineering (AREA)
  • Metallurgy (AREA)
  • Automation & Control Theory (AREA)
  • Analytical Chemistry (AREA)
  • General Chemical & Material Sciences (AREA)
  • Oil, Petroleum & Natural Gas (AREA)
  • Electrolytic Production Of Non-Metals, Compounds, Apparatuses Therefor (AREA)

Abstract

In various embodiments, the invention provides electro-chemical processes for reduction of carbon dioxide, for example converting carbon dioxide to formate salts or formic acid. In selected embodiments, operation of a continuous reactor with a three dimensional cathode and a two-phase (gas/liquid) catholyte flow provides advantageous conditions for electro-reduction of carbon dioxide. In these embodiments, the continuous two-phase flow of catholyte solvent and carbon dioxide containing gas, in selected gas/liquid phase volume flow ratios, provides dynamic conditions that favour the electro-reduction of COs at relatively high effective superficial current densities and gas space velocities, with relatively low reactor (cell) voltages (<10 Volts). In some embodiments, relatively high internal gas hold-up in the cathode chamber (evident in an internal gas to liquid phase volume ratio > 0.1) may provide greater than equilibrium CO2 concentrations in the liquid phase, also facilitating relatively high effective superficial current densities. In some embodiments, these characteristics may for example be achieved at catholyte pH > 7 and relatively low CO2 partial pressures (< 10 bar). In some embodiments, these characteristics may for example be achieved under near adiabatic conditions, with catholyte outlet temperature up to about 80°C.

Claims

AMENDED CLAIMS received by the International Bureau on 13 April 2007 (13.04.2007)CLAIMS
1. An electrochemical process for reducing carbon dioxide comprising: a) continuously passing a cathoiyte mixture through a cathode chamber of an electrochemical reactor, the catholyte mixture comprising carbon dioxide gas and a liquid catholyte solvent containing dissolved carbon dioxide; b) maintaining a catholyte gas to liquid volumetric hold-up ratio, being the ratio of the volume of gas to the volume of the liquid catholyte solvent, in the cathode chamber, greater than about 0.1. c) passing an electric current between a cathode in the cathode chamber and an anode, to reduce the dissolved carbon dioxide to form a desired product.
2. The process of claim 1 , wherein the gas (corrected to STP) to liquid volumetric feed ratio to the cathode chamber is greater than about 1.
3. The process of claim 1 or 2, wherein the effective superficial current density at the cathode is greater than 1 kA/m2 .
4. The process of claim 1 , 2 or 3, wherein the carbon dioxide gas partial pressure in the cathode chamber is less than 10 Bar.
5. The process of any one of claims 1 to 4, wherein the electric current is a direct current driven by an electrochemical cell voltage.
6. The process of claim 5, wherein the electrochemical cell voltage is less than 10 Volts.
7. The process of any one of claims 1 to 6, wherein fluids in the cathode chamber are maintained at a cathode temperature above 2O0C.
8. The process of any one of claims 1 to 7, wherein the cathode chamber is maintained at a cathode pressure and the cathode pressure is in the range of 1 Bar (100 kPa(abs)) to 10 Bar (1000 kPa(abs)).
9. The process of any one of claims 1 to 8, wherein the catholyte solvent is an aqueous solvent.
10. The process of claim 9, wherein the catholyte solvent comprises: a dissolved alkali metal bicarbonate or formate; or, a dissolved cti l il l iui ilUi i i ulurtl buhcjlt; Ol luH ricdc
11. The process of claim 9, wherein the bulk pH of the catholyte solvent is in the range of 4 to 10.
12. The process of claim 9, wherein the catholyte solvent comprises ammonium cations.
13. The process of any one of claims 1 to 12, wherein the cathode is a three dimensional electrode that has a thickness in the dimension of current flow of from 0.5 to 10 mm.
14. The process of claim 13, wherein the cathode has a porosity or voidage of from about 5% to about 95%.
15. The process of any one of claims 1 to 14, wherein the cathode comprises tin or lead.
16. The process of any one of claims 1 to 15, wherein the anode is in an anode chamber, and the anode chamber is separated from the cathode chamber by an electrochemical cell membrane.
17. The process of claim 16, wherein the anode chamber comprises an anolyte.
18. The process of claim 17, wherein the anolyte is an aqueous anolyte.
19. 19. The process of claim 18, wherein the anolyte comprises: a) a dissolved alkali metal hydroxide; b) a dissolved alkali metal or ammonium salt; c) a dissolved acid, being H2SO4, HCI, or H3PO4; d) dissolved sulphuric acid and ammonium sulphate; or e) dissolved sulphuric acid and sodium sulphate
20. The process of claim 18, wherein the anolyte comprises an ammonium ions.
21. The process of claim 16, wherein the electrochemical cell membrane is a cation permeable membrane.
22. The process of claim 16, wherein the electrochemical cell membrane permits selected ions to cross the membrane to balance the process stoichiometry.
23. The process of any one of claims 17 to 22, further comprising recycling at least a portion of the anolyte, the recycling anolyte, from an anolyte chamber outlet to an anolyte chamber inlet.
24. The process of claim 23, further comprising the step of separating an anode co-product from the recycling anolyte.
25. The process of any one of claims 17 to 24, further comprising Joule heating of the anolyte to provide heated anolyte.
26. The process of claim 25, further comprising Joule heating of the anolyte to provide heated anolyte, wherein the heated anolyte is used to heat the recycling catholyte solvent to separate water or the desired product from the recycling catholyte solvent by evaporation.
27. The process of any one of claims 1 to 26, wherein the desired product comprises a formate salt or formic acid.
28. The process of claim 27, wherein the formate salt is ammonium formate.
29. The process of any one of claims 1 to 28, further comprising separating the desired product from the catholyte solvent.
30. The process of any one of claims 1 to 28, further comprising recycling at least a portion of the catholyte solvent, the recycling catholyte solvent, from a cathode chamber outlet to a cathode chamber inlet.
31. The process of claim 30, further comprising the step of separating the desired product from the recycling catholyte solvent.
32. The process of claim 30, further comprising reacting recycling catholyte, comprising formate, with the anolyte, to obtain the desired product by an acidolysis reaction.
33. The process of claim 32, further comprising recycling at least a portion of the anolyte, the recycling anolyte, from an anolyte chamber outlet to an anolyte chamber inlet, and wherein the anolyte used to obtain the desired product is a portion of the recycling anolyte.
35
PCT/CA2006/001743 2005-10-13 2006-10-13 Continuous co-current electrochemical reduction of carbon dioxide WO2007041872A1 (en)

Priority Applications (8)

Application Number Priority Date Filing Date Title
AU2006301857A AU2006301857A1 (en) 2005-10-13 2006-10-13 Continuous co-current electrochemical reduction of carbon dioxide
US12/090,052 US20080223727A1 (en) 2005-10-13 2006-10-13 Continuous Co-Current Electrochemical Reduction of Carbon Dioxide
CN2006800378108A CN101657568B (en) 2005-10-13 2006-10-13 Continuous co-current electrochemical reduction of carbon dioxide
CA2625656A CA2625656C (en) 2005-10-13 2006-10-13 Continuous electro-chemical reduction of carbon dioxide
EP06804642A EP1951933A4 (en) 2005-10-13 2006-10-13 Continuous co-current electrochemical reduction of carbon dioxide
JP2008534843A JP2009511740A (en) 2005-10-13 2006-10-13 Continuous cocurrent electrochemical reduction of carbon dioxide
US14/244,869 US20140299482A1 (en) 2005-10-13 2014-04-03 Continuous co-current electrochemical reduction of carbon dioxide
US14/851,745 US20160068974A1 (en) 2005-10-13 2015-09-11 Continuous co-current electrochemical reduction of carbon dioxide

Applications Claiming Priority (2)

Application Number Priority Date Filing Date Title
US72564205P 2005-10-13 2005-10-13
US60/725,642 2005-10-13

Related Child Applications (3)

Application Number Title Priority Date Filing Date
US12/090,052 A-371-Of-International US20080223727A1 (en) 2005-10-13 2006-10-13 Continuous Co-Current Electrochemical Reduction of Carbon Dioxide
US14/244,869 Continuation US20140299482A1 (en) 2005-10-13 2014-04-03 Continuous co-current electrochemical reduction of carbon dioxide
US14/851,745 Continuation US20160068974A1 (en) 2005-10-13 2015-09-11 Continuous co-current electrochemical reduction of carbon dioxide

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WO2007041872A1 WO2007041872A1 (en) 2007-04-19
WO2007041872B1 true WO2007041872B1 (en) 2007-07-19

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US (3) US20080223727A1 (en)
EP (1) EP1951933A4 (en)
JP (1) JP2009511740A (en)
CN (1) CN101657568B (en)
AU (1) AU2006301857A1 (en)
CA (1) CA2625656C (en)
WO (1) WO2007041872A1 (en)

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