CN102899679A - Method for coproducing sulfuric acid by utilizing gypsum mineralized CO2 - Google Patents
Method for coproducing sulfuric acid by utilizing gypsum mineralized CO2 Download PDFInfo
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- CN102899679A CN102899679A CN201210410498XA CN201210410498A CN102899679A CN 102899679 A CN102899679 A CN 102899679A CN 201210410498X A CN201210410498X A CN 201210410498XA CN 201210410498 A CN201210410498 A CN 201210410498A CN 102899679 A CN102899679 A CN 102899679A
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- gypsum
- sulfuric acid
- mineralising
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Abstract
The invention discloses a method for coproducing sulfuric acid by utilizing gypsum mineralized CO2, which comprises the following steps: placing an anion-exchange membrane into an electrolytic cell; dividing the electrolytic cell into an anode area and a cathode area; adding a sodium sulfate solution as a cathode electrolyte into the cathode area; adding a sulfuric acid solution as an anode electrolyte into the anode area; adding the crushed gypsum into the cathode electrolyte of the electrolytic cell while introducing into the carbon dioxide gas; applying a direct current power supply between an anode electrode and a cathode electrode; reducing the hydrogen ion in the cathode electrolyte into hydrogen by the cathode electrode; converting the carbon dioxide in the solution into carbonate; performing replacement reaction on the carbonate and the gypsum, converting the gypsum into calcium carbonate while replacing freely flowing sulfate radical; and causing the sulfate radical to pass through the anion-exchange membrane under the action of current and to combine with the hydrogen ion generated by the anode electrode, thereby generating the sulfuric acid. The method has the advantages of high product extra value, simple technical process, mild reaction condition, and the like.
Description
Technical field
The present invention relates to a kind of CO
2Mineralising discharge-reducing method, particularly a kind of gypsum mineralising CO that utilizes
2Generate the CO of sulfuric acid
2Discharge-reducing method.
Background technology
Climate warming has been the mathematical fact, and the possibility more than 90% is that mankind's activity causes.CO in the global atmosphere
2Mass concentration is by 280 * 10 before the industrial age
-6Increase to 2005 379 * 10
-6Because the greenhouse gas emission that mankind's activity produces increases gradually, expects 2100, the CO in the atmosphere
2Mass concentration will reach 570 * 10
-6, cause Global Temperature to raise 1.9 ℃ sea-level rise 38 cm.Annual necessary 6,000,000,000 tons of CO that reduce in the global range
2Discharging could really prevent global warming.Atmosphere " Greenhouse effect " and global warming will be the living environment problems of maximum of 21 century facing mankind.The human directly a large amount of CO of discharging that in energy resource system, produces also
2It is the major cause that causes this phenomenon to produce.No matter consider from environment protection or from the angle of resource recycling, the CO to discharging in worldwide
2Catch the very urgent task that utilization (CCU) is facing mankind.
At present, traditional CO
2Utilizing method is with CO
2Be converted into the Chemicals such as urea and methyl alcohol, but with CO
2Be converted into the CO of Chemicals
2Consumption is very limited, and a large amount of carbonic acid gas still directly discharges atmosphere, in order to reduce CO
2Be discharged into the amount of atmosphere, in recent years, developed CO
2Be converted into the novel method of organism or polymkeric substance.But these methods are owing to reducing discharging CO
2Amount less, energy consumption is high thereby extensively do not promoted.Therefore, people need to develop new reduction of discharging CO
2Method.
Utilize mineral mineralising CO
2, the Chemicals of obtaining simultaneously high added value are a kind of CO
2Utilize novel method (CMU).The contriver is at CO
2The mineralising field has compared deep research, and " the CO of the rich potassium solution of coproduction has been finished in successively exploitation
2The mineralising method ", " CO of the rich potassium solution of pyroprocess coproduction
2The mineralising method " and " CO of the rich potassium solution of catalysis method coproduction
2The mineralising method ", at CO
2The rich potassium solution of coproduction is CO in the mineralisation process
2Mineralising has reduced discharging the production of potash fertilizer and has made contribution.These methods have been applied for Chinese invention patent.But these completed CO
2The not enough place of mineralising method is, technical process is longer, and energy consumption is higher.
Gypsum (CaSO
42H
2O) be topmost vitriol on the earth, the plaster of paris extensively is present in the sedimentogeneous rock, and reserves are abundant.In addition, the waste gypsum main component is calcium sulfate, and in the production process of the industries such as phosphoric acid, annual have a large amount of gypsum as industrial waste to produce, and only China just has 5,000 ten thousand tons of dischargings is just arranged about every year, and the phosphogypsum total amount of piling up at present is above 500,000,000 tons.The accumulation of a large amount of waste gypsums has not only taken tract, and can polluted-water and soil.Because effectively do not utilize the method for calcium sulfate in the waste gypsum at present, the waste gypsum of bulk deposition has endangered agriculture production, livestock growth and breeding and HUMAN HEALTH, becomes the environmental problem that needs to be resolved hurrily.But containing 18.6% element sulphur in the gypsum, and China's sulphur resource is very deficient.Gypsum is discharged as solid waste, not only cause environmental pollution, and wasted valuable sulphur resource.Therefore, more efficientlyly both can eliminate CO in the urgent need to developing
2And waste gypsum, but the novel method of valuable sulphur resource in the efficient recovery waste gypsum again.
Summary of the invention:
For the deficiency that prior art exists, purpose of the present invention aims to provide a kind of new CO
2Utilize method---utilize gypsum mineralising CO
2Co-producing sulfuric acid is to solve prior art CO
2The problems such as the technical process that the mineralising method exists is long, and energy consumption is higher, thus the pollution of CO2 and waste gypsum is eliminated in realization, reclaims valuable sulphur resource.
Basic ideas of the present invention are by with CO
2Mineralising is combined with the method for film electrolysis, realizes CO
2With the mineralising of gypsum, produce and separate sulfuric acid, thereby break thermodynamic(al)equilibrium, in low voltage, realize utilizing weakly acidic CO under the normal temperature and pressure
2Produce the chemical process of highly acid sulfuric acid.
The present invention proposes utilizes gypsum mineralising CO
2The method of co-producing sulfuric acid, its main contents are: anion-exchange membrane is placed electrolyzer, make electrolyzer be divided into two parts in positive polar region and negative pole district, add the metabisulfite solution as negative pole electrolytic solution in the negative pole district, the anodal sulphuric acid soln that adds as anode electrolyte, the powder gypsum is joined in the negative pole electrolytic solution of electrolyzer, be filled with simultaneously carbon dioxide, between anode electrode and negative electrode, apply direct supply, negative electrode is reduced to hydrogen with the hydrogen ion in the negative electrode liquid, so that the carbon dioxide conversion in the solution is carbonate, carbonate and gypsum generation replacement(metathesis)reaction are converted into calcium carbonate with gypsum, displace simultaneously free-pouring sulfate radical, sulfate radical sees through anion-exchange membrane under galvanic action, be combined with the hydrogen ion that anode electrode produces and generate sulfuric acid.
In the technique scheme, the hydrogen ion that described anode electrode produces can be produced by the gas diffusion electrode oxidizes hydrogen gas, also can be produced by the hydroxide radical in the metal platinum anodizing anode electrode liquid.The hydrogen of gas diffusion electrode oxidation preferably comes from the hydrogen that negative electrode produces, and certainly, also can come from other place.
In the technique scheme, described gypsum can be the plaster of paris ore of occurring in nature, and the main component that also can be the Industrial processes generation is the industrial product of gypsum, such as the waste gypsum that produces in the production process of phosphoric acid.
In the technique scheme, the gypsum that adds in the negative pole electrolytic solution is generally the powder gypsum, and its particle size is at least less than 10 purpose gypsum powders.
In the technique scheme, the concentration of anode electrolyte sulfuric acid is controlled to be 0.01 mol/L to 5 mol/L usually, and the concentration of negative pole electrolysis molten sulfur acid sodium solution is 0.1 mol/L to 5 mol/L.
In the technique scheme, negative electrode material can be metal platinum, palladium metal or metallic nickel.
In the technique scheme, when the hydrogen that utilizes negative pole to produce is originated as the hydrogen of positive gas diffusion electrode, gypsum and CO
2It is as follows that the mineralising reaction occurs:
CaSO
4·2H
2O + CO
2 → CaCO
3 + H
2SO
4 + H
2O (1)
In essence, this is that one " weak acid carbonic acid " produces the replacement(metathesis)reaction of " strong acid sulfuric acid ", and the chemical reaction rule of " strong acid weak acid processed " that this and people know is contrary.Calculation of thermodynamics also shows, this reaction is at standard state (25 ℃, the Gibbs free energy (G) under 1atm) is 85.12 kJ/mol(〉 50 kJ/mol).This means, the chemical process of this " weak acid strong acid processed " can not spontaneously be carried out.
The gypsum mineralising CO that the present invention proposes
2The novel method of co-producing sulfuric acid has solved gypsum mineralising CO
2In the process, the science difficult problem that " weak acid strong acid processed " can not spontaneously carry out has realized utilizing weakly acidic CO
2Produce highly acid sulfuric acid, broken the conventional thought of " strong acid weak acid processed ".Under certain conditions, this process only needs the voltage of 0.8V just can carry out, the realization of this process, so that less energy-consumption, low cost is efficiently utilized CO
2Become possibility, for solving global CO
2The reduction of discharging problem provides a kind of important method.
The gypsum mineralising CO that the present invention proposes
2The novel method of co-producing sulfuric acid, raw material sources are abundant, and added value of product is high.The waste gypsum of plaster of paris ore or industrial output, the method mineralising CO that all can adopt the present invention to propose
2Product sulfuric acid is not only the raw material of numerous Chemicals, but also is widely used in other sector of the national economy, and calcium carbonate is widely used in coating, cement and foodstuff additive; And breakthrough processing perplex for a long time the processing problem of people's waste gypsum, when effectively utilizing waste resource, solved an environmental pollution difficult problem, make the numerous industries that produce waste gypsum move towards the road that develops in a healthy way.
Description of drawings
When Fig. 1 is anode electrode employing gas diffusion electrode, gypsum mineralising CO
2The co-producing sulfuric acid schematic diagram
When Fig. 2 is anode electrode employing metal electrode, gypsum mineralising CO
2The co-producing sulfuric acid schematic diagram
1---gas diffusion electrode (positive pole), 2---anion-exchange membrane, 3---the negative pole metal electrode, 4---hydrogen gas buffer, 5---metal platinum electrode (positive pole)
Embodiment
Below in conjunction with accompanying drawing, the present invention is described in further detail by embodiment.It is important to point out; following examples are only for the present invention is described further; can not be interpreted as limiting the scope of the invention; affiliated art skilled staff is according to the foregoing invention content; the present invention is made some nonessential improvement and implementation is carried out in adjustment; very easily accomplish, therefore, such improvement should still belong to protection scope of the present invention with adjustment.
The mineralisation process of the present embodiment as shown in Figure 1.Electrolyzer is by only allowing negatively charged ion to see through, and the anion-exchange membrane 2 that can stop positively charged ion to see through is divided into positive and negative two zones.The H that adds 0.2mol/L
2SO
4Solution as anode electrolyte, adds the Na of 1.2mol/L to the anodal electrolyzer
2SO
4Solution to the negative pole electrolyzer as negative pole electrolytic solution.Anode electrode adopts gas diffusion electrode 1, and negative electrode adopts platinum electrode 3.Weighing 3g dried gypsum adds in the negative pole electrolytic solution, the CO that passes at negative pole bottom of electrolytic tank bubbling
2Flow is 20 ml/min, and the hydrogen that negative electrode is produced is collected and entered surge tank 4, passes into gas diffusion electrode from the hydrogen in the surge tank, under the voltage of 1.5V, carries out electrolytic reaction 1 h.With the oven dry of negative pole electrolyzer solid electrolytic product, obtain containing CO
2The solid of mineralization product calcium carbonate.Sulfuric acid concentration in the anode electrode liquid is increased to 0.7 mol/L.The current efficiency of producing calcium carbonate is 94.1%, and the current efficiency of producing sulfuric acid is 95.1%.
The mineralisation process of the present embodiment as shown in Figure 1.Electrolyzer is by only allowing negatively charged ion to see through, and the anion-exchange membrane 2 that can stop positively charged ion to see through is divided into positive and negative two zones.The H that adds 0.1mol/L
2SO
4Solution as anode electrolyte, adds the Na of 1.5mol/L to the anodal electrolyzer
2SO
4Solution to the negative pole electrolyzer as negative pole electrolytic solution.Anode electrode adopts gas diffusion electrode 1, and negative electrode adopts platinum electrode 3.The dry phosphogypsum solid waste of weighing 5g adds in the negative pole electrolytic solution, the CO that passes at negative pole bottom of electrolytic tank bubbling
2Flow is 20 ml/min, and the hydrogen that negative electrode is produced is collected and entered surge tank 4, passes into gas diffusion electrode from the hydrogen in the surge tank, under the voltage of 2.6V, carries out electrolytic reaction 1 h. with the oven dry of negative pole electrolyzer solid electrolytic product, obtains containing CO
2The solid of mineralization product calcium carbonate.Sulfuric acid concentration in the anode electrode liquid is increased to 1.5 mol/L.The current efficiency of producing calcium carbonate is 94.5%, and the current efficiency of producing sulfuric acid is 94.7%
The mineralisation process of the present embodiment as shown in Figure 2.Electrolyzer is by only allowing negatively charged ion to see through, and the anion-exchange membrane 2 that can stop positively charged ion to see through is divided into positive and negative two zones.The H that adds 0.1 mol/L
2SO
4Solution as anode electrolyte, adds the Na of 1 mol/L to the anodal electrolyzer
2SO
4Solution to the negative pole electrolyzer as negative pole electrolytic solution.Anode electrode adopts metal platinum electrode 5, and negative electrode adopts metallic nickel electrode 3.Weighing 3g dried gypsum adds in the negative pole electrolytic solution, the CO that passes at negative pole bottom of electrolytic tank bubbling
2Flow is 20 ml/min, under the voltage of 2.6 V, carries out electrolytic reaction 1 h.With the oven dry of negative pole electrolyzer solid electrolytic product, obtain containing CO
2The solid of mineralization product calcium carbonate, the sulfuric acid concentration in the anode electrode liquid is increased to 0.85 mol/L.The current efficiency of producing calcium carbonate is 94.2%, and the reaction efficiency of producing sulfuric acid is 94.5%.
Claims (10)
1. one kind is utilized gypsum mineralising CO
2The method of co-producing sulfuric acid, it is characterized in that: anion-exchange membrane is placed electrolyzer, make electrolyzer be divided into positive polar region and negative pole district, add the metabisulfite solution as negative pole electrolytic solution in the negative pole district, the anodal sulphuric acid soln that adds as anode electrolyte, the gypsum of pulverizing is joined in the negative pole electrolytic solution of electrolyzer, be filled with simultaneously carbon dioxide, between anode electrode and negative electrode, apply direct supply, negative electrode is reduced to hydrogen with the hydrogen ion in the negative pole electrolytic solution, so that the carbon dioxide conversion in the solution is carbonate, carbonate and gypsum generation replacement(metathesis)reaction are converted into calcium carbonate with gypsum, displace simultaneously free-pouring sulfate radical, sulfate radical sees through anion-exchange membrane under galvanic action, be combined with the hydrogen ion that anode electrode produces and generate sulfuric acid.
2. the gypsum mineralising CO that utilizes according to claim 1
2The method of co-producing sulfuric acid is characterized in that: the hydrogen ion that described anode electrode produces produced by the anode electrode oxidizes hydrogen gas or anode electrode oxidation anode electrolyte in hydroxide radical produced.
3. the gypsum mineralising CO that utilizes according to claim 2
2The method of co-producing sulfuric acid is characterized in that: the hydrogen of described anode electrode oxidation comes from the hydrogen that negative electrode produces.
4. the gypsum mineralising CO that utilizes according to claim 2
2The method of co-producing sulfuric acid is characterized in that: the anode electrode of described oxidizes hydrogen gas is gas diffusion electrode.
5. the gypsum mineralising CO that utilizes according to claim 2
2The method of co-producing sulfuric acid is characterized in that: the anode electrode hydroxy in the described oxidation anode electrode liquid is the metal platinum electrode.
6. the gypsum mineralising CO that utilizes according to claim 1
2The method of co-producing sulfuric acid is characterized in that: the described mode that is filled with carbon dioxide is that bubbling is filled with.
7. the gypsum mineralising CO that utilizes according to claim 1
2The method of co-producing sulfuric acid is characterized in that: described gypsum can be the plaster of paris ore of occurring in nature, and the main component that also can be the Industrial processes generation is the industrial product of gypsum.
8. the gypsum mineralising CO that utilizes according to claim 1
2The method of co-producing sulfuric acid is characterized in that: the gypsum of described pulverizing is that particle size is at least less than 10 purpose gypsum powders.
9. the gypsum mineralising CO that utilizes according to claim 1
2The method of co-producing sulfuric acid is characterized in that: the concentration of described anode electrolyte sulfuric acid is 0.01 mol/L to 5 mol/L, and the concentration of negative pole electrolysis molten sulfur acid sodium solution is 0.1 mol/L to 5 mol/L.
10. the gypsum mineralising CO that utilizes according to claim 1
2The method of co-producing sulfuric acid is characterized in that: described negative electrode material is metal platinum, palladium metal or metallic nickel.
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|---|---|---|---|
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|---|---|---|---|
| CN201210410498.XA CN102899679B (en) | 2012-10-24 | 2012-10-24 | Utilize gypsum mineralising CO 2the method of co-producing sulfuric acid |
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Cited By (7)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN102978653A (en) * | 2012-11-30 | 2013-03-20 | 四川大学 | Method for membrane electrolysis of mineralized CO2 co-produced strong acid |
| CN103952747A (en) * | 2014-04-15 | 2014-07-30 | 株洲冶炼集团股份有限公司 | Electro-deposition device for composite lead-carbon material |
| CN103966622A (en) * | 2014-04-30 | 2014-08-06 | 四川大学 | Method for realizing separation of potassium-rich solution through hydrochloric acid coproduced by utilizing membrane electrolysis technology to mineralize CO2 |
| CN104591100A (en) * | 2015-01-15 | 2015-05-06 | 贵州大学 | Method for preparing sulphuric acid from ardealite by membrane separation method |
| CN106757119A (en) * | 2016-12-09 | 2017-05-31 | 大连理工大学 | One kind is for realizing CO2The electro-chemical systems that capture is sealed up for safekeeping with mineralising |
| CN113874099A (en) * | 2019-06-14 | 2021-12-31 | 加州大学评议会 | Basic cation enrichment and water electrolysis to provide CO2Mineralization and global scale carbon management |
| WO2024163758A1 (en) * | 2023-02-03 | 2024-08-08 | Travertine Technologies, Inc. | Methods and systems for phosphoric acid and ammonium salt production |
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| Publication number | Priority date | Publication date | Assignee | Title |
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| WO2024163758A1 (en) * | 2023-02-03 | 2024-08-08 | Travertine Technologies, Inc. | Methods and systems for phosphoric acid and ammonium salt production |
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