CN109516912B - Method for sealing carbon dioxide - Google Patents
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- CN109516912B CN109516912B CN201811363621.0A CN201811363621A CN109516912B CN 109516912 B CN109516912 B CN 109516912B CN 201811363621 A CN201811363621 A CN 201811363621A CN 109516912 B CN109516912 B CN 109516912B
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- C—CHEMISTRY; METALLURGY
- C07—ORGANIC CHEMISTRY
- C07C—ACYCLIC OR CARBOCYCLIC COMPOUNDS
- C07C51/00—Preparation of carboxylic acids or their salts, halides or anhydrides
- C07C51/41—Preparation of salts of carboxylic acids
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- C01—INORGANIC CHEMISTRY
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- C01D7/00—Carbonates of sodium, potassium or alkali metals in general
- C01D7/18—Preparation by the ammonia-soda process
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- C11—ANIMAL OR VEGETABLE OILS, FATS, FATTY SUBSTANCES OR WAXES; FATTY ACIDS THEREFROM; DETERGENTS; CANDLES
- C11D—DETERGENT COMPOSITIONS; USE OF SINGLE SUBSTANCES AS DETERGENTS; SOAP OR SOAP-MAKING; RESIN SOAPS; RECOVERY OF GLYCEROL
- C11D1/00—Detergent compositions based essentially on surface-active compounds; Use of these compounds as a detergent
- C11D1/66—Non-ionic compounds
- C11D1/83—Mixtures of non-ionic with anionic compounds
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- C—CHEMISTRY; METALLURGY
- C11—ANIMAL OR VEGETABLE OILS, FATS, FATTY SUBSTANCES OR WAXES; FATTY ACIDS THEREFROM; DETERGENTS; CANDLES
- C11D—DETERGENT COMPOSITIONS; USE OF SINGLE SUBSTANCES AS DETERGENTS; SOAP OR SOAP-MAKING; RESIN SOAPS; RECOVERY OF GLYCEROL
- C11D17/00—Detergent materials or soaps characterised by their shape or physical properties
- C11D17/06—Powder; Flakes; Free-flowing mixtures; Sheets
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- C—CHEMISTRY; METALLURGY
- C11—ANIMAL OR VEGETABLE OILS, FATS, FATTY SUBSTANCES OR WAXES; FATTY ACIDS THEREFROM; DETERGENTS; CANDLES
- C11D—DETERGENT COMPOSITIONS; USE OF SINGLE SUBSTANCES AS DETERGENTS; SOAP OR SOAP-MAKING; RESIN SOAPS; RECOVERY OF GLYCEROL
- C11D3/00—Other compounding ingredients of detergent compositions covered in group C11D1/00
- C11D3/02—Inorganic compounds ; Elemental compounds
- C11D3/04—Water-soluble compounds
- C11D3/046—Salts
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- C—CHEMISTRY; METALLURGY
- C11—ANIMAL OR VEGETABLE OILS, FATS, FATTY SUBSTANCES OR WAXES; FATTY ACIDS THEREFROM; DETERGENTS; CANDLES
- C11D—DETERGENT COMPOSITIONS; USE OF SINGLE SUBSTANCES AS DETERGENTS; SOAP OR SOAP-MAKING; RESIN SOAPS; RECOVERY OF GLYCEROL
- C11D3/00—Other compounding ingredients of detergent compositions covered in group C11D1/00
- C11D3/02—Inorganic compounds ; Elemental compounds
- C11D3/04—Water-soluble compounds
- C11D3/08—Silicates
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- C—CHEMISTRY; METALLURGY
- C11—ANIMAL OR VEGETABLE OILS, FATS, FATTY SUBSTANCES OR WAXES; FATTY ACIDS THEREFROM; DETERGENTS; CANDLES
- C11D—DETERGENT COMPOSITIONS; USE OF SINGLE SUBSTANCES AS DETERGENTS; SOAP OR SOAP-MAKING; RESIN SOAPS; RECOVERY OF GLYCEROL
- C11D3/00—Other compounding ingredients of detergent compositions covered in group C11D1/00
- C11D3/02—Inorganic compounds ; Elemental compounds
- C11D3/04—Water-soluble compounds
- C11D3/10—Carbonates ; Bicarbonates
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- C—CHEMISTRY; METALLURGY
- C11—ANIMAL OR VEGETABLE OILS, FATS, FATTY SUBSTANCES OR WAXES; FATTY ACIDS THEREFROM; DETERGENTS; CANDLES
- C11D—DETERGENT COMPOSITIONS; USE OF SINGLE SUBSTANCES AS DETERGENTS; SOAP OR SOAP-MAKING; RESIN SOAPS; RECOVERY OF GLYCEROL
- C11D3/00—Other compounding ingredients of detergent compositions covered in group C11D1/00
- C11D3/16—Organic compounds
- C11D3/20—Organic compounds containing oxygen
- C11D3/2075—Carboxylic acids-salts thereof
- C11D3/2082—Polycarboxylic acids-salts thereof
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- C—CHEMISTRY; METALLURGY
- C11—ANIMAL OR VEGETABLE OILS, FATS, FATTY SUBSTANCES OR WAXES; FATTY ACIDS THEREFROM; DETERGENTS; CANDLES
- C11D—DETERGENT COMPOSITIONS; USE OF SINGLE SUBSTANCES AS DETERGENTS; SOAP OR SOAP-MAKING; RESIN SOAPS; RECOVERY OF GLYCEROL
- C11D3/00—Other compounding ingredients of detergent compositions covered in group C11D1/00
- C11D3/16—Organic compounds
- C11D3/20—Organic compounds containing oxygen
- C11D3/22—Carbohydrates or derivatives thereof
- C11D3/222—Natural or synthetic polysaccharides, e.g. cellulose, starch, gum, alginic acid or cyclodextrin
- C11D3/225—Natural or synthetic polysaccharides, e.g. cellulose, starch, gum, alginic acid or cyclodextrin etherified, e.g. CMC
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- C—CHEMISTRY; METALLURGY
- C11—ANIMAL OR VEGETABLE OILS, FATS, FATTY SUBSTANCES OR WAXES; FATTY ACIDS THEREFROM; DETERGENTS; CANDLES
- C11D—DETERGENT COMPOSITIONS; USE OF SINGLE SUBSTANCES AS DETERGENTS; SOAP OR SOAP-MAKING; RESIN SOAPS; RECOVERY OF GLYCEROL
- C11D1/00—Detergent compositions based essentially on surface-active compounds; Use of these compounds as a detergent
- C11D1/02—Anionic compounds
- C11D1/12—Sulfonic acids or sulfuric acid esters; Salts thereof
- C11D1/14—Sulfonic acids or sulfuric acid esters; Salts thereof derived from aliphatic hydrocarbons or mono-alcohols
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- C—CHEMISTRY; METALLURGY
- C11—ANIMAL OR VEGETABLE OILS, FATS, FATTY SUBSTANCES OR WAXES; FATTY ACIDS THEREFROM; DETERGENTS; CANDLES
- C11D—DETERGENT COMPOSITIONS; USE OF SINGLE SUBSTANCES AS DETERGENTS; SOAP OR SOAP-MAKING; RESIN SOAPS; RECOVERY OF GLYCEROL
- C11D1/00—Detergent compositions based essentially on surface-active compounds; Use of these compounds as a detergent
- C11D1/02—Anionic compounds
- C11D1/12—Sulfonic acids or sulfuric acid esters; Salts thereof
- C11D1/22—Sulfonic acids or sulfuric acid esters; Salts thereof derived from aromatic compounds
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- C—CHEMISTRY; METALLURGY
- C11—ANIMAL OR VEGETABLE OILS, FATS, FATTY SUBSTANCES OR WAXES; FATTY ACIDS THEREFROM; DETERGENTS; CANDLES
- C11D—DETERGENT COMPOSITIONS; USE OF SINGLE SUBSTANCES AS DETERGENTS; SOAP OR SOAP-MAKING; RESIN SOAPS; RECOVERY OF GLYCEROL
- C11D1/00—Detergent compositions based essentially on surface-active compounds; Use of these compounds as a detergent
- C11D1/66—Non-ionic compounds
- C11D1/72—Ethers of polyoxyalkylene glycols
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Abstract
The invention discloses a method for sealing and storing carbon dioxide, which is directly applied to the production of oxalate after capturing and absorbing the carbon dioxide by using inorganic alkali, wherein the oxalate is used as a detergent auxiliary agent and is used in a clothes detergent, and calcium oxalate crystals are formed by the oxalate and calcium ions in water in the clothes washing process, so that the utilization and the mineralization sealing and storage of the carbon dioxide are realized. According to the invention, carbon dioxide is absorbed by carbonate and directly used for producing oxalate, so that a large amount of energy loss in the regeneration process of the adsorbent is avoided, and zero emission can be realized in the whole process; oxalate prepared by carbon dioxide is used as a detergent auxiliary agent, and the carbon dioxide is mineralized and sealed finally by a mode of forming calcium oxalate precipitate by combining oxalate and calcium ions in the clothes washing process, so that the greenhouse effect is relieved.
Description
Technical Field
The invention relates to a method for utilizing and sealing carbon dioxide, in particular to a method for utilizing and sealing carbon dioxide, which takes carbon dioxide as a raw material to prepare oxalate, uses the oxalate as a detergent auxiliary agent, and generates calcium oxalate in the using process of a detergent so as to achieve the purpose of utilizing and sealing the carbon dioxide.
Background
The main reason for global warming is the emission of greenhouse gases, and CO in the emitted greenhouse gases2The contribution exceeds 60%. Among them, fossil fuel power generation occupies CO21/4 for discharge. In order to meet the power demand of daily life, the CO discharged by coal-fired power plants2The capture and utilization are an important problem.
CO for coal-fired power plants2Problem, different CO's were proposed2The trapping method comprises physical adsorption, chemical adsorption, membrane separation, biological fixation, low-temperature separation and the like. The membrane separation is difficult to balance the separation amount and the separation purity of the carbon dioxide; the operation energy consumption of low-temperature separation is high, and the method is only suitable for occasions of high-purity carbon dioxide; the scale of physical adsorption treatment is small, the physical adsorption treatment is greatly influenced by temperature and pressure, and good adsorption performance is difficult to achieve particularly when the partial pressure of carbon dioxide is low; immature biological fixing technology and the like. The chemical adsorption method has the advantages of excellent adsorption performance under the condition of low partial pressure of carbon dioxide, easy large-scale operation and capability of being matched with CO in a large-scale power plant2The advantages of matching capture scale are considered to be the most likely method to be applied to industrial scale at present. However, this method has disadvantages that the energy consumption for regenerating the adsorbent is high, the adsorbent is lost during the regeneration process, and the effect of reducing the carbon dioxide emission is not significant in practice.
Disclosure of Invention
The invention aims to provide a whole set of process flow for capturing, utilizing and sealing carbon dioxide. Meanwhile, an inorganic alkali tower is added behind the carbonization tower and is used for absorbing unconverted carbon dioxide, and the obtained carbonate can be recycled, so that zero emission of carbon dioxide in industry is realized.
The invention provides a method for capturing, utilizing and mineralizing carbon dioxide. The adsorbent adsorbing carbon dioxide is directly utilized after capture, thereby avoiding a large amount of energy consumption, realizing 'zero emission' due to a cyclic closed production process. Meanwhile, oxalate is added into washing powder as a detergent auxiliary agent, and can form stable calcium oxalate precipitation with calcium ions in water in the washing process so as to achieve the effect of carbon dioxide sequestration.
The invention provides a method for sealing and storing carbon dioxide, which is directly applied to the production of oxalate after capturing and absorbing the carbon dioxide by using inorganic alkali, wherein the oxalate is used as a detergent auxiliary agent for a clothes detergent, and calcium oxalate crystals are formed by the oxalate and calcium ions in water in the clothes washing process, so that the utilization and the mineralization sealing and storage of the carbon dioxide are realized.
Further, the method for sequestering carbon dioxide comprises the following steps:
the method comprises the following steps: preparing oxalate by taking carbon dioxide as a raw material:
(1) introducing the purified power plant tail gas into a reaction bed containing wet carbonate, and carrying out the following chemical reactions: x2CO3+CO2+H2O→2XHCO3(ii) a Then, the hydroxide solution is connected to absorb unreacted carbon dioxide, and the following chemical reactions occur: 2XOH + CO2→X2CO3+H2O; wherein X represents potassium or sodium;
(2) adding water into the bicarbonate produced in the step (1) to perform chemical reaction with hydrogen under a noble metal Pd/C catalyst: XHCO3+H2→HCOOX+H2O; in the step, the mass ratio of the bicarbonate to the water is 1-1.3;
(3) evaporating, centrifuging and drying formate, heating the formate to 320-440 ℃ by using an industrially common method for dehydrogenation reaction to obtain oxalate, collecting the removed hydrogen, and returning the hydrogen to the step (2) for recycling;
step two: use of oxalate for detergent builder preparation detergents:
(1) adding deionized water into a batching pot, heating to 50-60 ℃, and starting stirring;
(2) sequentially adding an anionic surfactant, oxalate, sodium carbonate, sodium silicate and anhydrous sodium sulfate into a batching pot;
(3) after the mixture in the batching pot is uniformly stirred, sequentially adding the nonionic surfactant and the anti-redeposition agent;
(4) after stirring uniformly, transferring the slurry into a tray, and drying in an oven at 100 ℃;
(5) drying for 10-14 h, taking out the solid, grinding in a mortar, and sieving with a 100-mesh sieve to obtain a powder detergent;
step three: in the washing process of the detergent, calcium oxalate and calcium ions in water form calcium oxalate crystals with the particle size of 1-5 mu m, so that utilization, mineralization and storage of carbon dioxide are realized.
In the above method, the detergent comprises the following components:
0.1 to 10.0 percent of nonionic surfactant
1.0 to 30.0 percent of anionic surfactant
1.0 to 30.0 percent of oxalate
1.0 to 15.0 percent of silicate
0 to 10.0 percent of sodium carbonate
0.5 to 5.0% of anti-redeposition agent
The balance of sodium sulfate.
Further, the detergent comprises the following components:
2.0 to 8.0 percent of nonionic surfactant
3.0 to 20.0 percent of anionic surfactant
Oxalate 10.0-25.0%
3.0 to 6.0 percent of silicate
3.0 to 10.0 percent of sodium carbonate
1.0-3.0% of anti-redeposition agent
The balance of sodium sulfate.
Further, the nonionic surfactant is selected from: c12~C18Fatty alcohol-polyoxyethylene ether of (C)12~C18Any one of condensates of an alcohol and an ethylene oxide/propylene oxide block copolymer.
Further, the anionic surfactant is selected from: c12~C18Alkyl benzene sulfonate, alpha-alkenyl sodium sulfonate, C12~16Any of secondary alkyl sulfonates.
Further, the oxalate is: sodium oxalate or potassium oxalate.
Further, the silicate is selected from: layered sodium silicate, potassium silicate, sodium metasilicate.
Further, the anti-redeposition agent is selected from the group consisting of: any one of acrylic acid polymer and sodium salt thereof, polyvinylpyrrolidone, sodium carboxymethylcellulose, acrylic acid-maleic anhydride copolymer and sodium salt thereof, polyvinyl alcohol, styrene acrylic acid copolymer.
The invention has the beneficial effects that:
(1) according to the invention, carbon dioxide is absorbed by carbonate and directly used for producing oxalate, so that a large amount of energy loss in the regeneration process of the adsorbent is avoided, and zero emission of carbon dioxide can be realized in the whole process;
(2) oxalate prepared by carbon dioxide is used as a detergent auxiliary agent, and the carbon dioxide is mineralized and sealed in a mode of forming calcium oxalate precipitate by combining oxalate and calcium ions in the clothes washing process, so that the greenhouse effect is relieved;
(3) provides a phosphate-free builder with high cost performance and environmental friendliness.
Drawings
FIG. 1 is an XRD pattern of the collected solid after completion of washing in examples 1 to 6;
FIG. 2 is an SEM photograph of the collected solid after completion of washing in examples 1 to 6.
Detailed Description
Introducing purified power plant tail gas into a reaction bed containing wet sodium carbonate, and reacting at 40 ℃ to generate sodium bicarbonate;
adding water with equal mass into sodium bicarbonate, stirring 5% of Pd/C (the load of Pd on C is 10%), introducing hydrogen, keeping the hydrogen pressure in a reactor at 1 atmospheric pressure, completing the reaction when the pH value of the solution solid disappears and is kept constant, and evaporating, centrifuging and drying the solution to obtain sodium formate solid;
and reacting the obtained sodium formate solid at 350 ℃ for 35min to complete the dehydrogenation of sodium formate to prepare sodium oxalate.
The obtained sodium oxalate is used in different washing powder formulas, and the washing powder preparation process comprises the following steps:
the raw materials are weighed according to the components and contents in the table 1. (1) Adding deionized water into a batching pot, heating to 50-60 ℃, and starting stirring; (2) sequentially adding an anionic surfactant, a builder, sodium carbonate, sodium silicate and anhydrous sodium sulfate into a batching pot; (3) after the mixture in the batching pot is uniformly stirred, sequentially adding the nonionic surfactant and the anti-redeposition agent; (4) after stirring uniformly, transferring the slurry into a tray, and drying in an oven at 100 ℃; (5) and after drying for 10-14 h, taking out the solid, grinding in a mortar, and sieving by a 100-mesh sieve to obtain the powder detergent.
1. Stain removal evaluation test
In order to verify the detergency of the detergent powder composition prepared by using the oxalate as a detergent auxiliary agent, a detergency test is carried out.
The detergency test method refers to GB/T13174-2008 'determination of detergency and circular washing performance of detergent for clothes' standard, and tests are carried out by adopting three types of dirty cloth of national standard carbon black oil stain cloth JB-01, national standard protein stain cloth JB-02 and national standard sebum stain cloth JB-03.
The experimental conditions were: adopting 250ppm hard water, the concentration of the detergent is 2g/L, the washing time is 20min, the temperature is 30 ℃, adopting an RQHL-III type vertical decontamination machine specified by national standard, and the rotating speed is 120 r/min.
2. Demonstration of calcium oxalate formation
To verify that oxalate was indeed precipitated as calcium oxalate during the washing, 300ml of the solution washed in the above example was taken out, centrifuged at 8000 rpm for 10min in a high speed centrifuge, the supernatant liquid was decanted, the solid was collected and dried at 40 ℃ for 24h by vacuum drying. The PXRD scanning range 2 theta is 5-50 degrees, the 4 degrees/min scanning is carried out, and the scanning electron microscope is used for characterization.
As shown in fig. 1, in conjunction with fig. 1Description is carried out: the collected solids were 14.320 ° and 20.073 ° at 2 Thetao、32.231oAnd 32.231 degrees, which are characteristic peaks of calcium oxalate dihydrate, the crystal planes (200), (211), (411) and (213) are respectively inclined, which proves that the calcium oxalate dihydrate exists in the solid. Whereas example 4 had 14.927o, 24.366oAnd 30.105oIs a characteristic peak of calcium oxalate monohydrate, which respectively corresponds to crystal faces(020) and. This demonstrates that the washed solid of example 4 contains a mixture of calcium oxalate monohydrate and calcium oxalate dihydrate, while the other is calcium oxalate dihydrate.
From the electron micrograph of FIG. 2, when the solid is magnified 5000 times, it can be clearly seen that the solid particles are spherical, because the calcium oxalate dihydrate is influenced by the surfactant and the polymer in the forming process, so that the calcium oxalate dihydrate is changed into a sphere from a typical double rectangular pyramid, and the particle size is distributed in the range of 1-5 μm.
From the above evaluations it can be seen that the detergent compositions formulated with oxalate all outperformed the standard detergent except in example 1 and XRD and SEM characterisations show that by washing with oxalate formulated detergent, oxalate can be precipitated as calcium oxalate for the purpose of indirect mineralization of carbon dioxide.
Claims (4)
1. A method of sequestering carbon dioxide, characterized by: inorganic alkali is used for capturing and absorbing carbon dioxide and then is directly applied to the production of oxalate, the oxalate is used as a detergent auxiliary agent for a clothes detergent, and calcium oxalate crystals are formed by the oxalate and calcium ions in water in the washing process, so that the utilization and mineralization sealing of the carbon dioxide are realized;
the method for sequestering carbon dioxide comprises the following steps:
the method comprises the following steps: preparing oxalate by taking carbon dioxide as a raw material:
(1) introducing the purified power plant tail gas into a reaction bed containing wet carbonate, and carrying out the following chemical reactions: x2CO3+CO2+H2O→2XHCO3(ii) a And (3) carrying out subsequent inorganic base: the hydroxide solution, which absorbs the unreacted carbon dioxide, undergoes the following chemical reaction: 2XOH + CO2→X2CO3+H2O; wherein X represents potassium or sodium;
(2) adding water into the bicarbonate produced in the step (1) to perform chemical reaction with hydrogen under a noble metal Pd/C catalyst: XHCO3+H2→HCOOX+H2O; in the step, the mass ratio of the bicarbonate to the water is 1-1.3;
(3) evaporating, centrifuging and drying formate, heating the formate to 320-440 ℃ by using an industrially common method for dehydrogenation reaction to obtain oxalate, collecting the removed hydrogen, and returning the hydrogen to the step (2) for recycling;
step two: use of oxalate for detergent builder preparation detergents:
(1) adding deionized water into a batching pot, heating to 50-60 ℃, and starting stirring;
(2) sequentially adding an anionic surfactant, oxalate, sodium carbonate, sodium silicate and anhydrous sodium sulfate into a batching pot;
(3) after the mixture in the batching pot is uniformly stirred, sequentially adding the nonionic surfactant and the anti-redeposition agent;
(4) after stirring uniformly, transferring the slurry into a tray, and drying in an oven at 100 ℃;
(5) drying for 10-14 h, taking out the solid, grinding in a mortar, and sieving with a 100-mesh sieve to obtain a powder detergent;
step three: in the washing process of the obtained detergent, oxalate and calcium ions in water form calcium oxalate crystals with the particle size of 1-5 mu m, so that utilization, mineralization and sealing of carbon dioxide are realized;
the detergent comprises the following components:
0.1 to 10.0 percent of nonionic surfactant
1.0 to 30.0 percent of anionic surfactant
1.0 to 30.0 percent of oxalate
1.0 to 15.0 percent of sodium silicate
0 to 10.0 percent of sodium carbonate
0.5 to 5.0% of anti-redeposition agent
The balance of sodium sulfate;
the nonionic surfactant is selected from: c12~C18Fatty alcohol-polyoxyethylene ether of (C)12~C18Any one of condensates of an alcohol and an ethylene oxide/propylene oxide block copolymer;
the anionic surfactant is selected from: c12~C18Alkyl benzene sulfonate, alpha-alkenyl sodium sulfonate, C12~16Any of secondary alkyl sulfonates.
2. The method of sequestering carbon dioxide of claim 1, wherein: the detergent comprises the following components:
2.0 to 8.0 percent of nonionic surfactant
3.0 to 20.0 percent of anionic surfactant
Oxalate 10.0-25.0%
3.0 to 6.0 percent of sodium silicate
3.0 to 10.0 percent of sodium carbonate
1.0-3.0% of anti-redeposition agent
The balance of sodium sulfate.
3. The method of sequestering carbon dioxide of claim 1, wherein: the oxalate is as follows: sodium oxalate or potassium oxalate.
4. The method of sequestering carbon dioxide of claim 1, wherein: the anti-redeposition agent is selected from the group consisting of: any one of acrylic acid polymer and sodium salt thereof, polyvinylpyrrolidone, sodium carboxymethylcellulose, acrylic acid-maleic anhydride copolymer and sodium salt thereof, polyvinyl alcohol, styrene acrylic acid copolymer.
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CN1732252A (en) * | 2002-11-04 | 2006-02-08 | 荷兰联合利华有限公司 | Laundry detergent composition |
CN107207390A (en) * | 2015-02-04 | 2017-09-26 | 国际壳牌研究有限公司 | The method for preparing oxalic acid |
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CN1732252A (en) * | 2002-11-04 | 2006-02-08 | 荷兰联合利华有限公司 | Laundry detergent composition |
CN107207390A (en) * | 2015-02-04 | 2017-09-26 | 国际壳牌研究有限公司 | The method for preparing oxalic acid |
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WO2023052192A1 (en) * | 2021-09-29 | 2023-04-06 | Shell Internationale Research Maatschappij B.V. | Method for generating a hydrogel from a co2 gas stream |
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