JPH0338219A - Removing and recovering method for carbon dioxide gas out of exhaust gas - Google Patents
Removing and recovering method for carbon dioxide gas out of exhaust gasInfo
- Publication number
- JPH0338219A JPH0338219A JP1169960A JP16996089A JPH0338219A JP H0338219 A JPH0338219 A JP H0338219A JP 1169960 A JP1169960 A JP 1169960A JP 16996089 A JP16996089 A JP 16996089A JP H0338219 A JPH0338219 A JP H0338219A
- Authority
- JP
- Japan
- Prior art keywords
- carbon dioxide
- gas
- absorption
- dioxide gas
- absorbing solution
- Prior art date
- Legal status (The legal status 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 status listed.)
- Granted
Links
- CURLTUGMZLYLDI-UHFFFAOYSA-N Carbon dioxide Chemical compound O=C=O CURLTUGMZLYLDI-UHFFFAOYSA-N 0.000 title claims abstract description 98
- 238000000034 method Methods 0.000 title claims abstract description 52
- 229910002092 carbon dioxide Inorganic materials 0.000 title claims abstract description 50
- 239000001569 carbon dioxide Substances 0.000 title claims abstract description 37
- 238000010521 absorption reaction Methods 0.000 claims abstract description 90
- 239000007789 gas Substances 0.000 claims abstract description 80
- RAHZWNYVWXNFOC-UHFFFAOYSA-N Sulphur dioxide Chemical compound O=S=O RAHZWNYVWXNFOC-UHFFFAOYSA-N 0.000 claims abstract description 28
- UIIMBOGNXHQVGW-UHFFFAOYSA-M Sodium bicarbonate Chemical compound [Na+].OC([O-])=O UIIMBOGNXHQVGW-UHFFFAOYSA-M 0.000 claims abstract description 22
- CDBYLPFSWZWCQE-UHFFFAOYSA-L Sodium Carbonate Chemical compound [Na+].[Na+].[O-]C([O-])=O CDBYLPFSWZWCQE-UHFFFAOYSA-L 0.000 claims abstract description 17
- 230000008929 regeneration Effects 0.000 claims abstract description 15
- 238000011069 regeneration method Methods 0.000 claims abstract description 15
- 229910000030 sodium bicarbonate Inorganic materials 0.000 claims abstract description 11
- 235000017557 sodium bicarbonate Nutrition 0.000 claims abstract description 11
- 238000010438 heat treatment Methods 0.000 claims abstract description 9
- 229910000029 sodium carbonate Inorganic materials 0.000 claims abstract description 8
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 claims abstract description 5
- 230000001590 oxidative effect Effects 0.000 claims abstract description 5
- 229910052760 oxygen Inorganic materials 0.000 claims abstract description 5
- 239000001301 oxygen Substances 0.000 claims abstract description 5
- QAOWNCQODCNURD-UHFFFAOYSA-L Sulfate Chemical compound [O-]S([O-])(=O)=O QAOWNCQODCNURD-UHFFFAOYSA-L 0.000 claims abstract description 3
- 238000001816 cooling Methods 0.000 claims abstract description 3
- 230000001172 regenerating effect Effects 0.000 claims abstract description 3
- 239000007788 liquid Substances 0.000 claims description 59
- 239000007864 aqueous solution Substances 0.000 claims description 4
- 239000002002 slurry Substances 0.000 abstract description 20
- 235000017550 sodium carbonate Nutrition 0.000 abstract description 7
- 238000011282 treatment Methods 0.000 abstract description 3
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 abstract description 3
- 239000000654 additive Substances 0.000 abstract description 2
- GWBWGPRZOYDADH-UHFFFAOYSA-N [C].[Na] Chemical compound [C].[Na] GWBWGPRZOYDADH-UHFFFAOYSA-N 0.000 abstract 1
- 230000000996 additive effect Effects 0.000 abstract 1
- 239000000463 material Substances 0.000 abstract 1
- 238000010517 secondary reaction Methods 0.000 abstract 1
- 230000002745 absorbent Effects 0.000 description 14
- 239000002250 absorbent Substances 0.000 description 14
- 239000007787 solid Substances 0.000 description 8
- 235000019645 odor Nutrition 0.000 description 5
- 238000000926 separation method Methods 0.000 description 5
- 238000006243 chemical reaction Methods 0.000 description 4
- 230000007423 decrease Effects 0.000 description 4
- BWHMMNNQKKPAPP-UHFFFAOYSA-L potassium carbonate Chemical compound [K+].[K+].[O-]C([O-])=O BWHMMNNQKKPAPP-UHFFFAOYSA-L 0.000 description 4
- HEMHJVSKTPXQMS-UHFFFAOYSA-M Sodium hydroxide Chemical compound [OH-].[Na+] HEMHJVSKTPXQMS-UHFFFAOYSA-M 0.000 description 3
- 239000002253 acid Substances 0.000 description 3
- 239000006227 byproduct Substances 0.000 description 3
- 238000010276 construction Methods 0.000 description 3
- 239000000428 dust Substances 0.000 description 3
- 230000000694 effects Effects 0.000 description 3
- 239000011734 sodium Substances 0.000 description 3
- 238000004065 wastewater treatment Methods 0.000 description 3
- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 description 2
- UGFAIRIUMAVXCW-UHFFFAOYSA-N Carbon monoxide Chemical compound [O+]#[C-] UGFAIRIUMAVXCW-UHFFFAOYSA-N 0.000 description 2
- MYMOFIZGZYHOMD-UHFFFAOYSA-N Dioxygen Chemical compound O=O MYMOFIZGZYHOMD-UHFFFAOYSA-N 0.000 description 2
- 230000005587 bubbling Effects 0.000 description 2
- 238000007796 conventional method Methods 0.000 description 2
- 238000000354 decomposition reaction Methods 0.000 description 2
- 238000006477 desulfuration reaction Methods 0.000 description 2
- 230000023556 desulfurization Effects 0.000 description 2
- 229910001873 dinitrogen Inorganic materials 0.000 description 2
- 229910001882 dioxygen Inorganic materials 0.000 description 2
- 238000002474 experimental method Methods 0.000 description 2
- 230000002349 favourable effect Effects 0.000 description 2
- 239000003546 flue gas Substances 0.000 description 2
- 238000004519 manufacturing process Methods 0.000 description 2
- 230000003647 oxidation Effects 0.000 description 2
- 238000007254 oxidation reaction Methods 0.000 description 2
- 229910000027 potassium carbonate Inorganic materials 0.000 description 2
- 235000011181 potassium carbonates Nutrition 0.000 description 2
- 229920006395 saturated elastomer Polymers 0.000 description 2
- 238000007086 side reaction Methods 0.000 description 2
- 239000000243 solution Substances 0.000 description 2
- 239000000126 substance Substances 0.000 description 2
- LSNNMFCWUKXFEE-UHFFFAOYSA-L sulfite Chemical compound [O-]S([O-])=O LSNNMFCWUKXFEE-UHFFFAOYSA-L 0.000 description 2
- 229910052815 sulfur oxide Inorganic materials 0.000 description 2
- HZAXFHJVJLSVMW-UHFFFAOYSA-N 2-Aminoethan-1-ol Chemical compound NCCO HZAXFHJVJLSVMW-UHFFFAOYSA-N 0.000 description 1
- BVKZGUZCCUSVTD-UHFFFAOYSA-M Bicarbonate Chemical compound OC([O-])=O BVKZGUZCCUSVTD-UHFFFAOYSA-M 0.000 description 1
- LSNNMFCWUKXFEE-UHFFFAOYSA-N Sulfurous acid Chemical compound OS(O)=O LSNNMFCWUKXFEE-UHFFFAOYSA-N 0.000 description 1
- 230000002378 acidificating effect Effects 0.000 description 1
- 150000001412 amines Chemical class 0.000 description 1
- 230000003139 buffering effect Effects 0.000 description 1
- 239000003245 coal Substances 0.000 description 1
- 150000001875 compounds Chemical class 0.000 description 1
- 238000005260 corrosion Methods 0.000 description 1
- 230000007797 corrosion Effects 0.000 description 1
- 238000002425 crystallisation Methods 0.000 description 1
- 230000008025 crystallization Effects 0.000 description 1
- 230000003247 decreasing effect Effects 0.000 description 1
- 238000007599 discharging Methods 0.000 description 1
- 231100000676 disease causative agent Toxicity 0.000 description 1
- 238000005868 electrolysis reaction Methods 0.000 description 1
- 230000007613 environmental effect Effects 0.000 description 1
- 239000012535 impurity Substances 0.000 description 1
- 238000002347 injection Methods 0.000 description 1
- 239000007924 injection Substances 0.000 description 1
- 239000012528 membrane Substances 0.000 description 1
- 231100000614 poison Toxicity 0.000 description 1
- 230000007096 poisonous effect Effects 0.000 description 1
- 239000011736 potassium bicarbonate Substances 0.000 description 1
- 235000015497 potassium bicarbonate Nutrition 0.000 description 1
- 229910000028 potassium bicarbonate Inorganic materials 0.000 description 1
- TYJJADVDDVDEDZ-UHFFFAOYSA-M potassium hydrogencarbonate Chemical compound [K+].OC([O-])=O TYJJADVDDVDEDZ-UHFFFAOYSA-M 0.000 description 1
- 239000002244 precipitate Substances 0.000 description 1
- 239000002994 raw material Substances 0.000 description 1
- 238000004064 recycling Methods 0.000 description 1
- 230000001568 sexual effect Effects 0.000 description 1
- 239000011343 solid material Substances 0.000 description 1
- 238000001179 sorption measurement Methods 0.000 description 1
- 239000002562 thickening agent Substances 0.000 description 1
- WUUHFRRPHJEEKV-UHFFFAOYSA-N tripotassium borate Chemical compound [K+].[K+].[K+].[O-]B([O-])[O-] WUUHFRRPHJEEKV-UHFFFAOYSA-N 0.000 description 1
- 239000002023 wood Substances 0.000 description 1
Classifications
-
- 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
- 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
Landscapes
- Treating Waste Gases (AREA)
- Carbon And Carbon Compounds (AREA)
Abstract
Description
【発明の詳細な説明】
（産業上の利用分野）
本発明は排ガス中から酸性ガス、特に炭酸ガス（ＣＯｔ
） 、亜硫酸ガス（ＳＯ，） 、を吸収除去し、純度の
高い炭酸ガスとして回収する方法に関する。DETAILED DESCRIPTION OF THE INVENTION (Industrial Application Field) The present invention aims to remove acid gas from exhaust gas, particularly carbon dioxide (COt).
), sulfur dioxide gas (SO, ), and a method of absorbing and removing it and recovering it as highly pure carbon dioxide gas.
（従来の技術及び
発明が解決しようとする課題〕
炭酸ガスは、トライアイスの原料等種々な用途を有する
有用な物質であるか、一方においては、近年、地球環境
に！！！要なＪｖｌｌをおよぼす原因物質として大気中
へのその多量な放出か問題とされている。このような状
況下１種々な排ガスに含まれる炭酸ガスを直接大気中に
放出することなしに除去１回収することは環境上及び経
済上、より重要な課題となってきている。(Problems to be solved by conventional techniques and inventions) Carbon dioxide gas is a useful substance that has various uses such as the raw material for Tri-ice, and on the other hand, in recent years, it has become important to The issue is whether large amounts of carbon dioxide gas are released into the atmosphere as a causative agent.Under these circumstances, it is important to remove and recover carbon dioxide contained in various exhaust gases without directly releasing them into the atmosphere. This is becoming a more important issue from a global and economic perspective.
炭酸ガスの除去法としては従来、吸着法、アルカノール
アミン法、熱炭酸カリ法、深冷分離法、膜分離法等が提
案され実施されている。しかしながらこれらの方法は、
建設費、運転費か高くなることに加え、液の分解による
臭気の発生、排水処理設備の必要性、装置の腐蝕、Ｍの
耐久性、副反応による性能の低下等の多くの問題点かあ
る。As methods for removing carbon dioxide gas, adsorption methods, alkanolamine methods, hot potassium carbonate methods, cryogenic separation methods, membrane separation methods, etc. have been proposed and put into practice. However, these methods
In addition to higher construction and operating costs, there are many problems such as odor generation due to decomposition of the liquid, need for wastewater treatment equipment, corrosion of equipment, durability of M, and reduced performance due to side reactions. .
また、炭酸ガスの吸収、除去に炭酸ナトリウム（Ｎａ２
ＣＯ３）の水溶液を用いる方法も知られている。しかし
なかこの方法は単に吸収液のアルカリ性を利用して酸性
ガスである炭酸ガスを吸収する方法にすぎない、また吸
収の効率も、ＮａＨＣＯ，の溶解度かＫＨＣＯ３よりも
劣るため、炭酸カリ法よりも劣るとされている。さらに
、この方法においては吸収液の再生効率か低いため建設
費、運転費か細注に比較して高くなる欠点があると言わ
れている。In addition, sodium carbonate (Na2) is used to absorb and remove carbon dioxide gas.
A method using an aqueous solution of CO3) is also known. However, this method is simply a method of absorbing carbon dioxide, which is an acidic gas, by using the alkalinity of the absorption liquid, and the absorption efficiency is also inferior to the solubility of NaHCO or KHCO3, so it is better than the potassium carbonate method. It is considered inferior. Furthermore, this method is said to have the disadvantage that the regeneration efficiency of the absorption liquid is low, resulting in higher construction and operating costs compared to fine injection.
排ガス、特にボイラー排ガスやキルン排ガス中にはダス
ト、水分が多く含まれ、Ｊｘｍガス濃度か５〜２０％で
ありかつ処理量か多いため建設費、運転費か高く、また
、悪臭等の二次公害の問題もあり、上記従来法の適用は
困難である。Exhaust gas, especially boiler exhaust gas and kiln exhaust gas, contains a lot of dust and moisture, and the Jxm gas concentration is 5 to 20%, and the amount of treatment is large, resulting in high construction and operating costs, and secondary problems such as bad odors. Due to the problem of pollution, it is difficult to apply the above conventional method.
従って１本発明の目的は、上記従来技術の欠点を有さな
い排ガス、特にボイラー排ガス中のｌＪｉ’酸ガスを除
去、回収する方法を提供することである。SUMMARY OF THE INVENTION It is therefore an object of the present invention to provide a method for removing and recovering lJi' acid gases in exhaust gases, in particular boiler exhaust gases, which does not have the disadvantages of the prior art described above.
さらに１本発明の目的は、排ガス中の有害ガス、特に亜
硫酸ガスを除去し、排ガス中から高効率で高純度の炭酸
ガスを除去、回収する方法を提供することである。A further object of the present invention is to provide a method for removing harmful gases, particularly sulfur dioxide gas, from exhaust gas, and removing and recovering highly purified carbon dioxide gas from exhaust gas with high efficiency.
〔課題を解決するための手段）
前記目的を遠戚するための本発明は、排ガスから炭酸ガ
スを除去、回収する方法において、水性吸収液による炭
酸ガスの吸収工程、炭酸ガスを吸収した水性吸収液の少
なくとも一部分を抜き出して加熱し、炭酸ガスを放出さ
せる水性吸収液の再生工程、及び再生された水性吸収液
を冷却し、前記吸収工程に戻す工程を含み、前記水性吸
収液か主として炭酸ナトリウム及び炭酸水素ナトリウム
からなるスラリーを含むことを特徴とする方法、である
。[Means for Solving the Problems] The present invention, which is distantly related to the above object, provides a method for removing and recovering carbon dioxide from exhaust gas, which includes a step of absorbing carbon dioxide with an aqueous absorption liquid, and an aqueous absorption process that absorbs carbon dioxide. a regeneration step of the aqueous absorption liquid in which at least a portion of the liquid is extracted and heated to release carbon dioxide gas, and a step of cooling the regenerated aqueous absorption liquid and returning it to the absorption step, wherein the aqueous absorption liquid is mainly made of sodium carbonate. and a slurry consisting of sodium bicarbonate.
本発明においては、炭酸ガスの吸収液として炭酸ナトリ
ウム及び炭酸水素ナトリウムから主としてなるスラリー
を含む水性吸収液を用いる。吸収工程ては、炭酸ガスは
、溶解した及び固体の炭酸ナトリウムと反応して炭酸水
素ナトリウムを生成するか、本発明の吸収液においては
、炭酸水素ナトリウムは飽和状態にあるため、炭酸ガス
の反応吸収によって生成した炭酸水素ナトリウムはその
まま固体として析出する。In the present invention, an aqueous absorption liquid containing a slurry mainly composed of sodium carbonate and sodium hydrogen carbonate is used as the carbon dioxide absorption liquid. In the absorption process, carbon dioxide gas reacts with dissolved and solid sodium carbonate to produce sodium hydrogen carbonate, or in the absorption liquid of the present invention, since sodium hydrogen carbonate is in a saturated state, the reaction of carbon dioxide gas occurs. Sodium hydrogen carbonate produced by absorption precipitates as a solid.
Ｎａ２ＣＯ３＋ＣＯ２＋）１２０−＋２ＮａｆｌＣＯ３
ＮａＨＣＯ＝ （液） −＋ＮａＨＣ（Ｊｒ （固）↓
したかって、本吸収液には強力なｐＨ緩衝作用かあり、
さらに再生吸収液スラリーが循環により投入されること
から炭酸ガスの反応吸収によるｐＨの低下かほとんど生
しることなく、炭酸ガスの吸収に適した高いｐＨか常に
雑持されることになる（第１図参ｆ！り。Na2CO3+CO2+)120-+2NaflCO3
NaHCO= (liquid) -+NaHC(Jr (solid)↓
Therefore, this absorption liquid has a strong pH buffering effect,
Furthermore, since the regenerated absorption liquid slurry is fed in through circulation, there is almost no pH drop due to reaction and absorption of carbon dioxide gas, and a high pH suitable for carbon dioxide absorption is always present. See Figure 1 f!
本発明の吸収工程の際及び／又は吸収工程の後において
、酸素を含む酸化性ガスを吸収液スラリーに導入するこ
とによって排ガス中に含まれる亜硫酸ガス（ＳＯ２）を
硫酸塩（ＳＯ４”−）として吸収液スラリー中に固定す
ることができる。During and/or after the absorption process of the present invention, sulfur dioxide gas (SO2) contained in the exhaust gas is converted into sulfate (SO4''-) by introducing an oxidizing gas containing oxygen into the absorption liquid slurry. It can be immobilized in an absorbent slurry.
従来技術においては、排ガス中のＣ０２と８０２の除去
は別々に行なわれることが好ましいと考えられる。すな
わち１例えば、ＳＯ３をＣａ系の吸収剤で除去し、Ｃ０
２をアミン系の吸収剤で除去する方法である。このとき
、ＳＯ２除去後のガスにその吸収剤か随伴し、Ｃ０２の
吸収剤中に混入することによる吸収効率の低下等の問題
の発生、あるいはシステムか極めて複雑になるという問
題等が考えられる。In the prior art, it is considered preferable that the removal of C02 and 802 in the exhaust gas be performed separately. That is, 1. For example, by removing SO3 with a Ca-based absorbent, CO
2 is removed using an amine-based absorbent. At this time, the absorbent accompanies the gas after SO2 removal and mixes into the CO2 absorbent, which may cause problems such as a decrease in absorption efficiency, or the system becomes extremely complicated.
しかし、本発明の方法によれば異質の吸収剤からなる系
を使用する必要かなく、上記問題点を全く生しることな
しに、一連の工程において効率よ〈Ｓ０２及びＣＯ３を
除去することができる、かつ、吸収液に酸素を含む酸化
性ガスを導入することにより再生工程て５２０３２−な
どの副生物の生成を無くすことかできるので、副生物の
特別な系外排出工程か不要になる。However, according to the method of the present invention, it is not necessary to use a system consisting of a different type of absorbent, and it is possible to efficiently remove S02 and CO3 in a series of steps without causing any of the above problems. By introducing an oxidizing gas containing oxygen into the absorption liquid, it is possible to eliminate the production of by-products such as 52032- during the regeneration process, thereby eliminating the need for a special process for discharging by-products from the system.
さらに、本発明によるＳＯ□の固定化はＳＯ１除表な目
的とする場合たけてなく ＳＯｘを排煙脱硫装置で除去
し、その後、ＣＯ３の除去を行う場合にも有効である。Furthermore, the immobilization of SO□ according to the present invention is not only effective when the purpose is to remove SO1, but also when SOx is removed by a flue gas desulfurization device and then CO3 is removed.
排煙脱硫装置で脱硫されたガス中にも少量のＳＯ□は残
存しているので、これにより得られるＣＯ□カスの純度
の低下や副生物の生成等の問題か発生するので本発明の
酸化性ガスの導入は。Since a small amount of SO□ remains in the gas desulfurized by the flue gas desulfurization equipment, this may cause problems such as a decrease in the purity of the CO□ residue obtained and the generation of by-products. The introduction of sexual gases.
これらに対して効果を発揮することかできる。It can be effective against these.
また、本発明の方法において、ＳＯ２の除去をＣＯ２の
吸収工程の前の工程において別途行なうこともできる。Furthermore, in the method of the present invention, SO2 removal can be performed separately in a step before the CO2 absorption step.
このＳ０２の除去工程における吸収液としては上記炭酸
ナトリウム及び炭酸水素ナトリウムのスラリーを含む吸
収液を循環使用することもできるか、この吸収液の固−
液分離後のＰ液を用いることか好ましい、ＳＯ□の吸収
工程において、Ｃ０２の吸収が起こらない条件にするた
めには、吸収液のｐＨはガス中ＣＯ□の平衡分圧の関係
から７．０以下か好ましく、ＳＯ□吸収能力の面から３
以上であることか好ましい。As the absorption liquid in this S02 removal step, it is possible to use the above-mentioned absorption liquid containing a slurry of sodium carbonate and sodium bicarbonate in a circulating manner, or to remove the solids of this absorption liquid.
It is preferable to use the P liquid after liquid separation. In order to create conditions in which CO2 absorption does not occur in the SO□ absorption process, the pH of the absorption liquid should be set to 7.0 from the equilibrium partial pressure of CO□ in the gas. 0 or less, preferably 3 from the standpoint of SO□ absorption capacity
It is preferable that it is above.
また、 ＳＯ，の吸収方法は、亜硫酸のｐＨ１衝作用を
利用する方法や吸収同時酸化方式（空気の導入）等にて
行うことかてきる。In addition, SO can be absorbed by a method that utilizes the pH 1 oxidation effect of sulfite, or by an absorption and simultaneous oxidation method (introduction of air).
このように前段においてＳ０２の吸収を行なう場合、Ｓ
Ｏ□の吸収工程においては、Ｓｏまたけでなく、ＩＩＦ
、 １１α等の有害ガス、ダスト等も除去できるので、
後段のＣＯ□吸収工程に与える悪影響を小さくし、ＣＯ
ｔの吸収効率を高めることができる。従って、この方法
は、多くの夾雑物を含む排ガス、例えば石油１石炭燃焼
ボイラーの排ガス用に適している。In this way, when absorbing S02 in the previous stage, S
In the absorption process of O□, not only So but also IIF
It can also remove harmful gases such as , 11α, dust, etc.
Reduces the negative impact on the subsequent CO□ absorption process and reduces CO□
The absorption efficiency of t can be increased. This method is therefore suitable for exhaust gases containing many impurities, for example the exhaust gases of oil-coal fired boilers.
この場合においても吸収液中に酸素を含む酸化性ガスを
導入すれば、ＳＯ８をＳＯ１′−として吸収液中に固定
できる。吸収液中に生成された５０４２−は所望により
環境問題を全く生しることなしに、放流、晶析あるいは
隔膜重席分離等により糸外へ排出することかできる。Even in this case, if an oxidizing gas containing oxygen is introduced into the absorption liquid, SO8 can be fixed in the absorption liquid as SO1'-. If desired, the 5042- produced in the absorbing liquid can be discharged out of the yarn by discharge, crystallization, diaphragm separation, etc. without causing any environmental problems.
炭酸ガスのＮａ、ＧＯ，による反応吸収工程は、Ｎａ、
Ｃ０３＋ＣＯｔ＋Ｈ，０： Ｎａ１ｌＣ０３の平衡の面
からは低温であることか望ましいが、反応速度及び熱収
支による運転費用の経済性を併せて考慮したとき４０〜
６０℃で行なうことが好ましい。The reaction absorption process of carbon dioxide gas with Na, GO,
C03+COt+H,0: From the viewpoint of equilibrium of Na1lC03, it is desirable that the temperature is low, but when considering the economy of operating costs due to reaction rate and heat balance, 40~
Preferably, the temperature is 60°C.
上記吸収工程において炭酸ガスを吸収した吸収液スラリ
ーの全部又は一部分か吸収液スラリーの炭酸ガス放出の
ため再生工程に移送される。再生工程へ移送される吸収
液スラリーの炭酸水素ナトリウムを含む固形分濃度を加
熱再生を行なう前に適当な装置１例えばサイクロン、シ
ックナー、遠心分離機等を用いて上げておくことか１吸
収液単位量当りのＣＯ３含有酸を上げることになり、従
って加熱再生に必要な熱量を低減することとなるので好
ましい。All or a portion of the absorbent slurry that has absorbed carbon dioxide gas in the absorption step is transferred to a regeneration step in order to release carbon dioxide gas from the absorbent slurry. Before heating and regenerating the absorbent slurry to be transferred to the regeneration process, it is necessary to increase the concentration of solids containing sodium bicarbonate using an appropriate device such as a cyclone, thickener, centrifuge, etc. This is preferable because it increases the amount of CO3-containing acid per unit amount and therefore reduces the amount of heat required for thermal regeneration.
本発明において炭酸ガス吸収に用いられる装置は特に制
限的ではなく１通常ガス吸収に用いられる装置を使用す
ることかできるか、スラリー生成を伴うことから、対ス
ラリー性を有する装置１例えば特公昭５５−３７２９５
に開示されているガスバブリング方式を採用するものか
奸ましい。In the present invention, the device used for absorbing carbon dioxide gas is not particularly limited; 1. Devices normally used for gas absorption may be used; or, since slurry generation is involved, a device having slurry resistance 1, for example, Japanese Patent Publication No. 55 -37295
It seems suspicious that it uses the gas bubbling method disclosed in .
炭酸ガスを吸収した吸収液スラリーを約１１０〜１３０
°Ｃに加熱することによって加熱再生を行なう、この加
熱再生は再生に通常使用される棚段塔、充項塔等を使用
して行なうことかできるが、スラリーに対応か容易な蒸
発缶を使用することが好ましい。また適宜フラッシュタ
ンクの併用も可能である。About 110 to 130% of the absorbent slurry that has absorbed carbon dioxide gas
Thermal regeneration is performed by heating to °C. This heating regeneration can be performed using plate columns, packed columns, etc. that are normally used for regeneration, but an evaporator can be used because it is easy to handle slurry. It is preferable to do so. It is also possible to use a flash tank as appropriate.
この加熱による温度上昇に伴いＮａＨＣ（１＋の溶解度
か−Ｅ昇し溶液中のＮａ＊ＣＯ，／ Ｎａ１ｌＣＯ，比
か小さくなる。このために、ｐＨは自動的に低下し、Ｃ
０２の放出（吸収液スラリーの再生）に有利な条件か生
じるが１通常、ＣＯ□の放出か進行するとｐＨか次第に
上昇し、徐々にＣＯ３の放出に不利な条件となる。As the temperature rises due to this heating, the solubility of NaHC (1+ -E increases and the ratio of Na*CO,/Na1lCO, in the solution decreases. Therefore, the pH automatically decreases and the
Conditions are favorable for the release of CO2 (regeneration of the absorbent slurry), but as the release of CO□ progresses, the pH gradually increases, and conditions gradually become unfavorable for the release of CO3.
しかしながら、本方法では、吸収液中にはＣ０２放出に
ともないＮａｔＣＯｔ濃度は飽和状態となり加熱再生に
よって生成した％ａ、ＣＯ，はそのまま固体として析出
する。また、Ｃ０２の放出により減少した溶液中のＮａ
ＨＣＯ３は固体のＮａＨＣＯｓの溶解により補充される
ために、はぼ飽和状態で一定に保持される。このために
、木刀法においては、ＣＯ□の放出によるｐｉの上昇か
ほとんど生しることなく、ＣＯｔの放出に有利な条件が
維持される（第１図参照）。However, in this method, the concentration of NatCOt in the absorption liquid reaches a saturated state as CO2 is released, and the %a, CO, produced by heating regeneration is deposited as a solid. In addition, Na in the solution decreased due to the release of CO2.
The HCO3 is kept constant near saturation because it is replenished by dissolving solid NaHCOs. For this reason, in the Bokuto method, there is almost no increase in pi due to the release of CO□, and conditions favorable to the release of COt are maintained (see Figure 1).
上記再生工程で再生された吸収液スラリー（主としてＮ
ａ２ＧＯ＋を含む固形物からなる）は冷却されて、吸収
工程へ移送され、循環使用に供される。このとき再生工
程へ移送される低温の吸収液スラリーと吸収工程へ移送
される高温の吸収液スラリーとの間で相互に熱交換を行
なうことか運転費の経済上有利である。The absorbent slurry regenerated in the above regeneration process (mainly N
The solid material containing a2GO+) is cooled and transferred to the absorption process for recycling. At this time, it is advantageous in terms of operating costs to mutually exchange heat between the low-temperature absorbent slurry transferred to the regeneration process and the high-temperature absorbent slurry transferred to the absorption process.
本発明の循環使用される水性吸収液にアルカノールアミ
ン及び／又はその化合物（例えばアルカノールアミンホ
ウ酸カリ）を水性吸収液の前記重量に対して５重量％以
下の量で添加することによりＣＯｌの吸収効率を上げる
ことができる。５重量％より多く添加すると、アルカノ
ールアミンの分解による悪臭の発生や運転費か高くなる
等の問題か生し易くなるので好ましくない。Absorption of COl by adding an alkanolamine and/or its compound (for example, alkanolamine potassium borate) to the aqueous absorption liquid used for circulation in the present invention in an amount of 5% by weight or less based on the weight of the aqueous absorption liquid. It can increase efficiency. Addition of more than 5% by weight is not preferable because problems such as generation of bad odor due to decomposition of the alkanolamine and increase in operating costs are likely to occur.
以下、実施例により本発明をより異体的に説明する。Hereinafter, the present invention will be explained in more detail with reference to Examples.
（実施例１）
木１１にＮａ２ＣＯｚ １８０ ｇとＮａＨＣＯ３３８
０ｇを加えて、主としてＮａＨＣＯ３からなる固形物を
含む吸収液を調整した。この吸収液にＣＯ，１２％を含
有するｇ素ガスを４００旧／時間のｆＩｉ、量で導入し
、バブリング方式の気液接触を行なわせた。(Example 1) 180 g of Na2COz and 338 NaHCO on wood 11
0 g was added to prepare an absorption liquid containing solids mainly consisting of NaHCO3. A gram gas containing 12% CO was introduced into this absorption liquid at an amount of 400 fIi/hour to effect gas-liquid contact by bubbling.
この炭酸ガスを吸収した吸収液の一部分を加熱槽に送り
、１１５〜１３５℃で加熱してＣＯｔを放出させた。放
出したＣ０２ガスは多量の水蒸気を含むため冷却して水
を分離した。A portion of the absorption liquid that absorbed carbon dioxide gas was sent to a heating tank and heated at 115 to 135°C to release COt. Since the released CO2 gas contained a large amount of water vapor, it was cooled to separate water.
ＣＯｔ放出後の再生スラリー液は冷却後、吸収液に混合
した。After COt release, the regenerated slurry liquid was cooled and mixed with the absorption liquid.
以上の結果、安定した７０％以上のＣＯ□吸収率及び９
５％以上の純度を有するＣＯ２ガスが得られた。また吸
収液のＣＯＤ値は０であった。As a result of the above, a stable CO□ absorption rate of 70% or more and a
CO2 gas with a purity of more than 5% was obtained. Moreover, the COD value of the absorption liquid was 0.
従って、特別な排水処理設備は不要であることか確認さ
れた。Therefore, it was confirmed that special wastewater treatment equipment is not required.
また、同一装置において吸収液としてモノエタノールア
ミンの２５％水溶液を用いた場合の約６０％の熱量で吸
収液を再生することができた。Furthermore, in the same apparatus, the absorption liquid could be regenerated with approximately 60% of the amount of heat required when a 25% aqueous solution of monoethanolamine was used as the absorption liquid.
（実施例２）
吸収液として、実施例１で用いた吸収液に３＠量％のジ
ェタノールアミンを添加した吸収液を使用した以外は実
施例１と同様にして実験を行なった。(Example 2) An experiment was conducted in the same manner as in Example 1, except that an absorption liquid obtained by adding 3% by weight of jetanolamine to the absorption liquid used in Example 1 was used as the absorption liquid.
その結果、ＣＯ□の吸収率は約１５％上昇し、８５％か
得られた。また、吸収液の再生に要した熱量は実施例１
の場合とほぼ同等であった。As a result, the absorption rate of CO□ increased by about 15%, reaching 85%. In addition, the amount of heat required to regenerate the absorption liquid is as shown in Example 1.
It was almost the same as in the case of .
処理ガス中に臭気は認められなかった。No odor was observed in the treated gas.
（実施例３）
被処理ガスとしてＣＯ□１２％、９０，２００ｐｐｍを
含有する窒素ガスを用い、さらに加熱槽へ送る前にｍＪ
ガスを、２ＯＮＩ／時間のｆＩｉ量て吸収液に導入した
以外は実施例１と同様にして実験を行なった。(Example 3) Nitrogen gas containing 12% CO□ and 90,200 ppm was used as the gas to be treated, and further mJ was used before sending it to the heating tank.
The experiment was carried out in the same manner as in Example 1, except that the gas was introduced into the absorption liquid in an amount fIi of 2 ONI/hour.
その結果、ＣＯ６の吸収率は７０％以上であり、ＳＯ２
の吸収率は９０％以上であった。得られたＣＯ，ガスの
純度は９５％以上であった。As a result, the absorption rate of CO6 was over 70%, and the absorption rate of SO2 was over 70%.
The absorption rate was 90% or more. The purity of the obtained CO gas was 95% or more.
なお、上記の実施例において酸素ガスを導入しなかった
場合、得られたＣＯ，ガス中にはＳ０２ガスか確認され
、また、冷却器（熱交換器〉より排出するトレン中には
Ｓ〇−−が含まれていた。また、吸収液中にはＣＯＤに
寄与するＳ、０３の生成が認められた。In addition, when oxygen gas was not introduced in the above example, S02 gas was confirmed in the CO and gas obtained, and S02 gas was found in the train discharged from the cooler (heat exchanger). In addition, the production of S,03, which contributes to COD, was observed in the absorption liquid.
（実施例４）
ＣＯ□の吸収工程の前の工程において、まずＳＯ２の吸
収を行なった。 ＳＯＲの吸収液としては炭酸ガスの吸
収液の固−液分離後のｒ液を用いｐｕａ、ｓにて吸収を
行った。被処理ガスであるＣ０．１２％、ＳＯｘ ２０
０ ｐｐｍを含む窒素ガスを４００ Ｎ＋／時間の流量
で吸収液に導入し、同時に酸素ガスを２ＯＮ＋／時間の
流量で導入した、そして、吸収液の一部を系外へ抜き出
した。(Example 4) In the step before the CO□ absorption step, SO2 was first absorbed. As the absorption liquid for SOR, the r liquid after solid-liquid separation of the carbon dioxide absorption liquid was used, and absorption was performed in pua and s. Processed gas: C0.12%, SOx 20
Nitrogen gas containing 0 ppm was introduced into the absorption liquid at a flow rate of 400 N+/hour, and at the same time oxygen gas was introduced at a flow rate of 2ON+/hour, and a portion of the absorption liquid was drawn out of the system.
次に、上記工程を通過した被処理ガスを炭酸ガス吸収液
（実施例１と同様に調整した）に導入した。吸収液ｐＨ
は内生された吸収液スラリーと５％ＮａＯＨ水溶液で１
０．５〜１１．０とした。このとき同時にｍ毒ガスを２
ＯＮ＋／時間の流ので導入した。その他の処理は実施例
１と同様な方法で行なった。Next, the gas to be treated that had passed through the above steps was introduced into a carbon dioxide absorption liquid (prepared in the same manner as in Example 1). Absorption liquid pH
is 1 with internalized absorption liquid slurry and 5% NaOH aqueous solution.
It was set to 0.5 to 11.0. At this time, 2 m poisonous gas
It was introduced because of the ON+/time flow. Other treatments were performed in the same manner as in Example 1.
得られた結果は、ＣＯ□の吸収率か７０％以−Ｅであり
、ＳＯ□の吸収率か９７％以上であった。The obtained results were that the absorption rate of CO□ was 70% or more, and the absorption rate of SO□ was 97% or more.
また、得られたＣＯ，ガスの純度は９５％以上であった
。Ｓ０２を吸収し、抜き出した液については、隔膜電解
法によりＮａ０１１か再生されることか確認された。Moreover, the purity of the obtained CO and gas was 95% or more. It was confirmed that Na011 could be regenerated from the liquid extracted after absorbing S02 by diaphragm electrolysis.
（発明の効果）
本発明によれば、特別な添加物を必要とすることなく、
有害な副反応も起こらない、従って、悪臭、有害物の排
出がなく、特別な排水処理も不要である。(Effect of the invention) According to the present invention, without the need for special additives,
No harmful side reactions occur; therefore, there are no foul odors or harmful substances discharged, and no special wastewater treatment is required.
運転コストが安価な、効率の良い炭酸ガスの吸収除去、
回収を行なうことかできる。Efficient absorption and removal of carbon dioxide with low operating costs,
Collection can be carried out.
多量に排出され、ダスト含有量の多い排ガス、特にボイ
ラー排ガス等の場合においても、１５０°Ｃ以下の条件
において効率よく炭酸ガスを除去、回収することかでき
る。Even in the case of exhaust gas that is discharged in large quantities and has a high dust content, especially boiler exhaust gas, carbon dioxide gas can be efficiently removed and recovered under conditions of 150° C. or lower.
また、本発明の方法、特に実施例３及び４の方法によれ
ばＣ０２及びＳＯ３を同一のＮａ系吸収液で処理するこ
とが可能となり、簡単なシステムで効率良く運転するこ
とかできる。Further, according to the method of the present invention, particularly the methods of Examples 3 and 4, it becomes possible to treat CO2 and SO3 with the same Na-based absorption liquid, and the system can be operated efficiently with a simple system.
第１図は、本発明の方法の各工程におけるｐＨの安定性
を概念的に示すグラフである。
ｗ４２図は、本発明の方法の全工程の１！要を示す図で
ある。FIG. 1 is a graph conceptually showing the pH stability in each step of the method of the present invention. Figure w42 shows 1! of all steps of the method of the present invention! FIG.
Claims (1)
、水性吸収液による炭酸ガスの吸収工程、炭酸ガスを吸
収した水性吸収液の少なくとも一部分を抜き出して加熱
し、炭酸ガスを放出させる水性吸収液の再生工程、及び
再生された水性吸収液を冷却し、前記吸収工程に戻す工
程を含み、前記水性吸収液が主として炭酸ナトリウム及
び／又は炭酸水素ナトリウムからなるスラリーを含むこ
とを特徴とする方法。 ２、酸素を含む酸化性ガスを、前記吸収工程において又
は前記吸収工程と再生工程との中間の工程において、前
記水性吸収液に導入することによって排ガス中の亜硫酸
ガスを硫酸塩として固定することを特徴とする請求項１
の方法。 ３、前記吸収工程の前に、炭酸ナトリウム及び炭酸水素
ナトリウムを含む水溶液を用いるＳＯ＿２の吸収工程を
設けることを特徴とする請求項１の方法。[Claims] 1. A method for recovering and removing carbon dioxide gas from exhaust gas, which includes a step of absorbing carbon dioxide gas using an aqueous absorption liquid, and extracting and heating at least a portion of the aqueous absorption liquid that has absorbed carbon dioxide gas to remove carbon dioxide gas. a step of regenerating the aqueous absorption liquid to be released; and a step of cooling the regenerated aqueous absorption liquid and returning it to the absorption step; How to characterize it. 2. Fixing sulfur dioxide gas in exhaust gas as sulfate by introducing an oxidizing gas containing oxygen into the aqueous absorption liquid in the absorption step or in an intermediate step between the absorption step and the regeneration step. Claim 1
the method of. 3. The method according to claim 1, characterized in that, before the absorption step, an SO_2 absorption step using an aqueous solution containing sodium carbonate and sodium bicarbonate is provided.
Priority Applications (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP1169960A JPH0338219A (en) | 1989-07-03 | 1989-07-03 | Removing and recovering method for carbon dioxide gas out of exhaust gas |
Applications Claiming Priority (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP1169960A JPH0338219A (en) | 1989-07-03 | 1989-07-03 | Removing and recovering method for carbon dioxide gas out of exhaust gas |
Publications (2)
| Publication Number | Publication Date |
|---|---|
| JPH0338219A true JPH0338219A (en) | 1991-02-19 |
| JPH0521610B2 JPH0521610B2 (en) | 1993-03-25 |
Family
ID=15896021
Family Applications (1)
| Application Number | Title | Priority Date | Filing Date |
|---|---|---|---|
| JP1169960A Granted JPH0338219A (en) | 1989-07-03 | 1989-07-03 | Removing and recovering method for carbon dioxide gas out of exhaust gas |
Country Status (1)
| Country | Link |
|---|---|
| JP (1) | JPH0338219A (en) |
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| WO2001005489A1 (en) * | 1999-07-19 | 2001-01-25 | Ebara Corporation | Apparatus and method for cleaning acidic gas |
| WO2004113226A1 (en) * | 2003-06-18 | 2004-12-29 | Kabushiki Kaisha Toshiba | System and method for collecting carbon dioxide in exhaust gas |
| WO2006100667A1 (en) * | 2005-03-21 | 2006-09-28 | Cargill, Incorporated A Register Delaware Corporation Of | A method for the enhanced production of algal biomass |
| EP1733782A1 (en) * | 2005-06-15 | 2006-12-20 | Kvaerner Power Oy | A method and an apparatus for removing carbon dioxide from sulphur dioxide containing flue gases |
| JP2013544636A (en) * | 2010-10-18 | 2013-12-19 | 武▲漢凱▼迪▲電▼力股▲分▼有限公司 | Method and apparatus for recovering carbon dioxide in flue gas using activated sodium carbonate |
| WO2015052325A1 (en) * | 2013-10-11 | 2015-04-16 | Nilu - Stiftelsen Norsk Institutt For Luftforskning | Capture of carbon dioxide |
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|---|---|---|---|---|
| WO2001005489A1 (en) * | 1999-07-19 | 2001-01-25 | Ebara Corporation | Apparatus and method for cleaning acidic gas |
| WO2004113226A1 (en) * | 2003-06-18 | 2004-12-29 | Kabushiki Kaisha Toshiba | System and method for collecting carbon dioxide in exhaust gas |
| WO2006100667A1 (en) * | 2005-03-21 | 2006-09-28 | Cargill, Incorporated A Register Delaware Corporation Of | A method for the enhanced production of algal biomass |
| EP1733782A1 (en) * | 2005-06-15 | 2006-12-20 | Kvaerner Power Oy | A method and an apparatus for removing carbon dioxide from sulphur dioxide containing flue gases |
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| US7910079B2 (en) | 2005-06-15 | 2011-03-22 | Metso Power Oy | Method and an apparatus for removing carbon dioxide from sulphur dioxide containing flue gases |
| JP2013544636A (en) * | 2010-10-18 | 2013-12-19 | 武▲漢凱▼迪▲電▼力股▲分▼有限公司 | Method and apparatus for recovering carbon dioxide in flue gas using activated sodium carbonate |
| WO2015052325A1 (en) * | 2013-10-11 | 2015-04-16 | Nilu - Stiftelsen Norsk Institutt For Luftforskning | Capture of carbon dioxide |
Also Published As
| Publication number | Publication date |
|---|---|
| JPH0521610B2 (en) | 1993-03-25 |
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