CN112546878A - Ceramic-carbonate compact two-phase inorganic membrane with ceramic material as support - Google Patents

Ceramic-carbonate compact two-phase inorganic membrane with ceramic material as support Download PDF

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CN112546878A
CN112546878A CN202110082114.5A CN202110082114A CN112546878A CN 112546878 A CN112546878 A CN 112546878A CN 202110082114 A CN202110082114 A CN 202110082114A CN 112546878 A CN112546878 A CN 112546878A
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carbonate
phase
ceramic
inorganic membrane
mixed
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CN202110082114.5A
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陈天嘉
张永锋
许艳阳
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Inner Mongolia University of Technology
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Inner Mongolia University of Technology
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    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D71/00—Semi-permeable membranes for separation processes or apparatus characterised by the material; Manufacturing processes specially adapted therefor
    • B01D71/02—Inorganic material
    • 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
    • B01D53/22—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 diffusion
    • B01D53/228—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 diffusion characterised by specific membranes
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D67/00—Processes specially adapted for manufacturing semi-permeable membranes for separation processes or apparatus
    • B01D67/0039—Inorganic membrane manufacture
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D69/00—Semi-permeable membranes for separation processes or apparatus characterised by their form, structure or properties; Manufacturing processes specially adapted therefor
    • B01D69/04—Tubular membranes
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D69/00—Semi-permeable membranes for separation processes or apparatus characterised by their form, structure or properties; Manufacturing processes specially adapted therefor
    • B01D69/06—Flat membranes
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D69/00—Semi-permeable membranes for separation processes or apparatus characterised by their form, structure or properties; Manufacturing processes specially adapted therefor
    • B01D69/08—Hollow fibre membranes
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D69/00—Semi-permeable membranes for separation processes or apparatus characterised by their form, structure or properties; Manufacturing processes specially adapted therefor
    • B01D69/10—Supported membranes; Membrane supports
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
    • C01B32/00—Carbon; Compounds thereof
    • C01B32/50—Carbon dioxide
    • C01B32/55—Solidifying
    • C—CHEMISTRY; METALLURGY
    • C04—CEMENTS; CONCRETE; ARTIFICIAL STONE; CERAMICS; REFRACTORIES
    • C04B—LIME, MAGNESIA; SLAG; CEMENTS; COMPOSITIONS THEREOF, e.g. MORTARS, CONCRETE OR LIKE BUILDING MATERIALS; ARTIFICIAL STONE; CERAMICS; REFRACTORIES; TREATMENT OF NATURAL STONE
    • C04B41/00—After-treatment of mortars, concrete, artificial stone or ceramics; Treatment of natural stone
    • C04B41/009—After-treatment of mortars, concrete, artificial stone or ceramics; Treatment of natural stone characterised by the material treated
    • C—CHEMISTRY; METALLURGY
    • C04—CEMENTS; CONCRETE; ARTIFICIAL STONE; CERAMICS; REFRACTORIES
    • C04B—LIME, MAGNESIA; SLAG; CEMENTS; COMPOSITIONS THEREOF, e.g. MORTARS, CONCRETE OR LIKE BUILDING MATERIALS; ARTIFICIAL STONE; CERAMICS; REFRACTORIES; TREATMENT OF NATURAL STONE
    • C04B41/00—After-treatment of mortars, concrete, artificial stone or ceramics; Treatment of natural stone
    • C04B41/45—Coating or impregnating, e.g. injection in masonry, partial coating of green or fired ceramics, organic coating compositions for adhering together two concrete elements
    • C04B41/50—Coating or impregnating, e.g. injection in masonry, partial coating of green or fired ceramics, organic coating compositions for adhering together two concrete elements with inorganic materials
    • C04B41/5007—Coating or impregnating, e.g. injection in masonry, partial coating of green or fired ceramics, organic coating compositions for adhering together two concrete elements with inorganic materials with salts or salty compositions, e.g. for salt glazing
    • C04B41/501—Coating or impregnating, e.g. injection in masonry, partial coating of green or fired ceramics, organic coating compositions for adhering together two concrete elements with inorganic materials with salts or salty compositions, e.g. for salt glazing containing carbon in the anion, e.g. carbonates
    • C—CHEMISTRY; METALLURGY
    • C04—CEMENTS; CONCRETE; ARTIFICIAL STONE; CERAMICS; REFRACTORIES
    • C04B—LIME, MAGNESIA; SLAG; CEMENTS; COMPOSITIONS THEREOF, e.g. MORTARS, CONCRETE OR LIKE BUILDING MATERIALS; ARTIFICIAL STONE; CERAMICS; REFRACTORIES; TREATMENT OF NATURAL STONE
    • C04B41/00—After-treatment of mortars, concrete, artificial stone or ceramics; Treatment of natural stone
    • C04B41/80—After-treatment of mortars, concrete, artificial stone or ceramics; Treatment of natural stone of only ceramics
    • C04B41/81—Coating or impregnation
    • C04B41/85—Coating or impregnation with inorganic materials
    • 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
    • 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)
  • Chemical Kinetics & Catalysis (AREA)
  • Engineering & Computer Science (AREA)
  • Ceramic Engineering (AREA)
  • Inorganic Chemistry (AREA)
  • Organic Chemistry (AREA)
  • Materials Engineering (AREA)
  • Structural Engineering (AREA)
  • Oil, Petroleum & Natural Gas (AREA)
  • General Chemical & Material Sciences (AREA)
  • Analytical Chemistry (AREA)
  • Manufacturing & Machinery (AREA)
  • Separation Using Semi-Permeable Membranes (AREA)

Abstract

The invention relates to the field of inorganic membrane preparation, in particular to a ceramic-carbonate compact taking a ceramic material as a support bodyA two-phase inorganic membrane comprising two phases, one being a ceramic phase as a support and the other being a carbonate phase; the ceramic phase is made of samarium oxide doped cerium oxide, and the carbonate phase is mixed carbonate. The carbonate phase is mixed carbonate consisting of lithium carbonate and sodium carbonate, and the mixing ratio of the lithium carbonate to the sodium carbonate is 52:48 mol%. The compact inorganic membrane can directly separate CO at high temperature2The cooling process of mixed exhaust gas is omitted, load energy is saved, and production economic benefits are improved in a direction-changing mode.

Description

Ceramic-carbonate compact two-phase inorganic membrane with ceramic material as support
Technical Field
The invention relates to the field of inorganic membrane preparation, in particular to a ceramic-carbonate compact two-phase inorganic membrane taking a ceramic material as a support body.
Background
Currently, the main sources of carbon emissions are thermal power plants and chemical plants. CO22The capture technology can effectively control carbon emission. CO22Is the first step of the capture technique and is also the most important step. Chemical absorption is a mature industrial separation of CO2But this technique also has significant drawbacks. In the whole absorption process, the absorption efficiency of the absorbent is low, the absorption capacity is small, and the temperature of the high-temperature gas needs to be reduced to a lower temperature (generally, the temperature needs to be reduced) in the operation process<150 c) which all result in a large amount of additional energy consumption and loss and thus increase the separation cost.
Compared with the conventional CO2The separation method, the membrane separation method has the characteristics of simple equipment, small floor area, low energy consumption, simple operation and the like, develops rapidly in recent years and is considered to have great potential to develop into CO2The technology of industrial separation. Organic polymer membranes and some inorganic membranes (e.g., microporous inorganic membranes) although having some CO2Separation efficiency, but these membranes still cannot be operated at high temperatures: (>Separation of CO at 600 ℃ C2And high temperature rich in CO2The temperature of the mixed gas (such as flue gas and reformed synthesis gas) is generally 500-1000 ℃, so that the temperature of the mixed gas needs to be reduced to below 150 ℃ by separating CO2 in the high-temperature gas by adopting the traditional method, a large amount of load energy is consumed in the temperature reduction process, and the production and emission reduction cost is increased.
Disclosure of Invention
In order to solve the problems, the invention provides a ceramic-carbonate compact two-phase inorganic membrane taking a ceramic material as a support, which can separate CO in a temperature range of 500-1000 DEG C2。
In order to achieve the purpose, the invention adopts the technical scheme that:
a ceramic-carbonate compact two-phase inorganic membrane taking a ceramic material as a support is characterized in that: the inorganic membrane comprises two phases, one being a ceramic phase as a support and the other being a carbonate phase; the ceramic phase is made of samarium oxide doped cerium oxide (Sm)2O3 doped-CeO2SDC), the carbonate phase is mixed carbonate.
Preferably, the carbonate phase is a mixed carbonate composed of lithium carbonate and sodium carbonate, and the mixing ratio of the lithium carbonate and the sodium carbonate is 52:48 mol%.
Preferably, the carbonate phase is a mixed carbonate composed of lithium carbonate, sodium carbonate and potassium carbonate, and the mixing ratio of lithium carbonate, sodium carbonate and potassium carbonate is 42.5/32.5/25 mol%.
Further, during preparation, a hollow fiber tubular, sheet or thick tubular ceramic support body is prepared by a phase transition spinning method, the support body is of a porous structure, and the average pore diameter is 1-2 microns; then, the mixed carbonate is burnt to a molten state, the molten carbonate is impregnated into the pore channels of the ceramic support body by a direct infiltration method, and the pores of the support body are filled to form the compact ceramic-carbonate two-phase hollow fiber inorganic membrane.
The invention has the following beneficial effects:
1) the compact inorganic membrane can directly separate CO at high temperature2The cooling process of the mixed exhaust gas is omitted, the load energy is saved, and the production economic benefit is improved due to the diversion;
2) due to a special high temperature separation mechanism, the ceramic membrane is used for CO2The selectivity of (A) can reach infinity theoretically, to CO2Has single selectivity, thereby expanding the application environment and the field of the invention.
Drawings
Fig. 1 is a schematic structural diagram of a ceramic-carbonate dense dual-phase inorganic membrane using a ceramic material as a support according to an embodiment of the present invention.
Fig. 2 is a working principle diagram of a ceramic-carbonate dense dual-phase inorganic membrane using a ceramic material as a support according to an embodiment of the present invention.
Detailed Description
The present invention will be described in detail with reference to specific examples. The following examples will assist those skilled in the art in further understanding the invention, but are not intended to limit the invention in any way. It should be noted that variations and modifications can be made by persons skilled in the art without departing from the spirit of the invention. All falling within the scope of the present invention.
Example 1
As shown in fig. 1, a ceramic-carbonate dense two-phase inorganic membrane using a ceramic material as a support comprises two phases, one of which is a ceramic phase as a support and the other of which is a carbonate phase; the ceramic phase is made of samarium oxide doped cerium oxide (Sm)2O3 doped-CeO2SDC), the carbonate phase is mixed carbonate; the carbonate phase is mixed carbonate consisting of lithium carbonate and sodium carbonate, and the mixing ratio of the lithium carbonate to the sodium carbonate is 52:48 mol%.
During preparation, a hollow fiber tubular, sheet or thick tubular ceramic support body is prepared by a phase transition spinning method, the support body is of a porous structure, and the average pore diameter is 1-2 microns; then, the mixed carbonate is burnt to a molten state, the molten carbonate is impregnated into the pore channels of the ceramic support body by a direct infiltration method, and the pores of the support body are filled to form the compact ceramic-carbonate two-phase hollow fiber inorganic membrane.
Example 2
A ceramic-carbonate dense two-phase inorganic membrane using a ceramic material as a support comprises two phases, one phase is a ceramic phase as the support, and the other phase is a carbonate phase; the ceramic phase is made of samarium oxide doped cerium oxide (Sm)2O3doped-CeO2SDC), the carbonate phase is mixed carbonate; the carbonate phase is mixed carbonate consisting of lithium carbonate and sodium carbonate, and the mixing ratio of the lithium carbonate to the sodium carbonate is 52:48 mol%.
During preparation, a hollow fiber tubular and flaky ceramic support body is prepared by a phase transition spinning method, the support body is of a porous structure, and the average pore diameter is 1-2 microns; then, the mixed carbonate is burnt to a molten state, the molten carbonate is impregnated into the pore channels of the ceramic support body by a direct infiltration method, and the pores of the support body are filled to form the compact ceramic-carbonate two-phase hollow fiber inorganic membrane.
Example 3
A ceramic-carbonate dense two-phase inorganic membrane using a ceramic material as a support comprises two phases, one phase is a ceramic phase as the support, and the other phase is a carbonate phase; the ceramic phase is made of samarium oxide doped cerium oxide (Sm)2O3doped-CeO2SDC), the carbonate phase is mixed carbonate; the carbonate phase is mixed carbonate consisting of lithium carbonate and sodium carbonate, and the mixing ratio of the lithium carbonate to the sodium carbonate is 52:48 mol%.
During preparation, a thick tubular ceramic support body is prepared by a phase transition spinning method, the support body is of a porous structure, and the average pore diameter is 1-2 microns; then, the mixed carbonate is burnt to a molten state, the molten carbonate is impregnated into the pore channels of the ceramic support body by a direct infiltration method, and the pores of the support body are filled to form the compact ceramic-carbonate two-phase hollow fiber inorganic membrane.
Example 4
As shown in fig. 1, a ceramic-carbonate dense two-phase inorganic membrane using a ceramic material as a support comprises two phases, one of which is a ceramic phase as a support and the other of which is a carbonate phase; the ceramic phase is made of samarium oxide doped cerium oxide (Sm)2O3 doped-CeO2SDC), the carbonate phase is mixed carbonate; the carbonate phase is a mixed carbonate composed of lithium carbonate, sodium carbonate and potassium carbonate, and the mixing ratio of the lithium carbonate, the sodium carbonate and the potassium carbonate is 42.5/32.5/25 mol%.
During preparation, a hollow fiber tubular ceramic support body is prepared by a phase transition spinning method, the support body is of a porous structure, and the average pore diameter is 1-2 microns; then, the mixed carbonate is burnt to a molten state, the molten carbonate is impregnated into the pore channels of the ceramic support body by a direct infiltration method, and the pores of the support body are filled to form the compact ceramic-carbonate two-phase hollow fiber inorganic membrane.
It is noted that the support material of the ceramic membrane may be replaced by some material having a high oxygen ion conductivity, such as certain perovskite materials.
The specific separation principle of the ceramic-carbonate two-phase inorganic membrane of the present invention is shown in fig. 2: when the mixed gas is in contact with the membrane, CO2Will react with oxygen ions (O) in the ceramic phase2-) Combined to form carbonate ion (CO)3 2-) CO formed3 2-Will conduct in the carbonate phase in the film layer. CO on gas supply side of inorganic membrane2Is much higher than the other side, so the chemical gradient difference causes the carbonate to be conducted toward the side of lower concentration at all times. When CO is present3 2-A decomposition reaction occurs when the gas is conducted to the other surface of the inorganic membrane, i.e., from CO3 2-Decomposition to CO2And O2-. To maintain internal electrical balance, O2-Direction of conduction and CO3 2-Are in opposite directions, so that CO3 2-Decomposed O2-Will conduct to the gas supply side to continue to combine with CO2Thereby achieving the continuous CO separation2The purpose of (1). It can be seen from the mechanism that since the ceramic-carbonate inorganic membrane is a dense membrane, and the separation process is ion selective conduction. Therefore, the membrane separates CO2Is usually provided with a pair of CO2And the operating temperature range of the membrane is 500-1000 ℃, so that the membrane can be applied to high-temperature CO in an oxidizing environment2Separation (e.g. flue gas), and can also be used for CO in high temperature reducing atmosphere2Separation, such as H in a hydrogen production process (e.g., IGCC system)2And CO2The mixed gas is separated.
The foregoing description of specific embodiments of the present invention has been presented. It is to be understood that the present invention is not limited to the specific embodiments described above, and that various changes or modifications may be made by one skilled in the art within the scope of the appended claims without departing from the spirit of the invention. The embodiments and features of the embodiments of the present application may be combined with each other arbitrarily without conflict.

Claims (4)

1. A ceramic-carbonate compact two-phase inorganic membrane taking a ceramic material as a support is characterized in that: the inorganic membrane comprises two phases, one being a ceramic phase as a support and the other being a carbonate phase; the ceramic phase is made of samarium oxide doped cerium oxide, and the carbonate phase is mixed carbonate.
2. The ceramic-carbonate dense two-phase inorganic membrane supported on a ceramic material according to claim 1, wherein: the carbonate phase is mixed carbonate consisting of lithium carbonate and sodium carbonate, and the mixing ratio of the lithium carbonate to the sodium carbonate is 52:48 mol%.
3. The ceramic-carbonate dense two-phase inorganic membrane supported on a ceramic material according to claim 1, wherein: the carbonate phase is a mixed carbonate composed of lithium carbonate, sodium carbonate and potassium carbonate, and the mixing ratio of the lithium carbonate, the sodium carbonate and the potassium carbonate is 42.5/32.5/25 mol%.
4. The ceramic-carbonate dense two-phase inorganic membrane supported on a ceramic material according to claim 1, wherein: during preparation, a hollow fiber tubular, sheet or thick tubular ceramic support body is prepared by a phase transition spinning method, the support body is of a porous structure, and the average pore diameter is 1-2 microns; then, the mixed carbonate is burnt to a molten state, the molten carbonate is impregnated into the pore channels of the ceramic support body by a direct infiltration method, and the pores of the support body are filled to form the compact ceramic-carbonate two-phase hollow fiber inorganic membrane.
CN202110082114.5A 2021-01-21 2021-01-21 Ceramic-carbonate compact two-phase inorganic membrane with ceramic material as support Pending CN112546878A (en)

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Citations (4)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN102489175A (en) * 2011-12-20 2012-06-13 天津工业大学 Preparation method of ceramic/molten salt double-phase composite gas separating film
CN103071397A (en) * 2013-01-17 2013-05-01 南京工业大学 Method for preparing high temperature CO2 separation membrane
US20150090125A1 (en) * 2013-09-05 2015-04-02 The Arizona Board Of Regents For And On Behalf Of Arizona State University Tubular ceramic-carbonate dual-phase membranes and methods of manufacture thereof
CN106669437A (en) * 2017-01-16 2017-05-17 中国矿业大学(北京) Preparation method of novel high-efficiency biphase CO2 electrochemical separation membrane

Patent Citations (4)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN102489175A (en) * 2011-12-20 2012-06-13 天津工业大学 Preparation method of ceramic/molten salt double-phase composite gas separating film
CN103071397A (en) * 2013-01-17 2013-05-01 南京工业大学 Method for preparing high temperature CO2 separation membrane
US20150090125A1 (en) * 2013-09-05 2015-04-02 The Arizona Board Of Regents For And On Behalf Of Arizona State University Tubular ceramic-carbonate dual-phase membranes and methods of manufacture thereof
CN106669437A (en) * 2017-01-16 2017-05-17 中国矿业大学(北京) Preparation method of novel high-efficiency biphase CO2 electrochemical separation membrane

Non-Patent Citations (4)

* Cited by examiner, † Cited by third party
Title
CHEN，TJ: "High CO2 permeability of ceramic-carbonate dual-phase hollow fiber membrane at medium-high temperature", 《JOURNAL OF MEMBRANE SCIENCE》 *
LU, B: "Asymmetric Thin Samarium Doped Cerium Oxide-Carbonate Dual-Phase Membrane for Carbon Dioxide Separation", 《INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH》 *
NORTON, TT: "Carbon dioxide permeation properties and stability of samarium-doped-ceria carbonate dual-phase membranes", 《JOURNAL OF MEMBRANE SCIENCE》 *
区英鸿: "《塑料手册》", 28 February 1991, 兵器工业出版社 *

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Application publication date: 20210326