JP5415045B2 - Carbon dioxide immobilization method - Google Patents
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- JP5415045B2 JP5415045B2 JP2008236451A JP2008236451A JP5415045B2 JP 5415045 B2 JP5415045 B2 JP 5415045B2 JP 2008236451 A JP2008236451 A JP 2008236451A JP 2008236451 A JP2008236451 A JP 2008236451A JP 5415045 B2 JP5415045 B2 JP 5415045B2
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- 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
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Description
本発明は、二酸化炭素固定化方法に関し、特に、固体に二酸化炭素を化学的に吸収させて固定化する方法に関する。 The present invention relates to a carbon dioxide immobilization method, and more particularly to a method for chemically immobilizing carbon dioxide in a solid and immobilizing it.
二酸化炭素（ＣＯ2）は、地球温暖化の原因となる温室効果ガスの一つであり、大気中の二酸化炭素濃度を下げるため種々の方法が提案されている。例えば、気体として大気中に放出されたＣＯ2、又は放出される直前のＣＯ2を地中や水中等に封じ込める二酸化炭素の貯留もその一つに挙げられる。 Carbon dioxide (CO 2 ) is one of the greenhouse gases that cause global warming, and various methods have been proposed to reduce the concentration of carbon dioxide in the atmosphere. For example, CO 2 released into the atmosphere as a gas, or storage of carbon dioxide that confines CO 2 immediately before being released into the ground or in water is one example.
また、鉄鋼製造プロセスで発生するスラグに含まれる未炭酸化Ｃａを利用してＣＯ2含有ガス中のＣＯ2濃度を低減する方法（特許文献１、２参照）、石綿又は石綿含有蛇紋岩を焼成して二酸化炭素固定化材を得る方法（特許文献３）、未焼成カンラン岩を主成分とする汚染物質処理剤により空気中のＣＯ2を吸収する方法（特許文献４）等の化学的吸収法も提案されている。 Further, (see Patent Documents 1 and 2) a method of reducing the CO 2 concentration in the CO 2 containing gas by using a non-carbonated Ca contained in the slag generated in the steel manufacturing process, sintering the asbestos or asbestos containing serpentinite Chemical absorption methods such as a method for obtaining a carbon dioxide-fixing material (Patent Document 3), a method for absorbing CO 2 in the air with a pollutant treating agent mainly composed of uncalcined peridotite (Patent Document 4), etc. Has also been proposed.
しかし、二酸化炭素の貯留については、技術的、コスト的な問題に加え、地殻変動等によって貯留層からＣＯ2が漏洩する虞や、海洋環境等へ悪影響を与える虞があるという問題があった。 However, the storage of carbon dioxide has a problem that, in addition to technical and cost problems, there is a possibility that CO 2 may leak from the reservoir due to crustal deformation or the like, and that the marine environment may be adversely affected.
また、鉄鋼製造プロセスで発生するスラグに含まれる未炭酸化Ｃａを利用する方法については、ＣＯ2の低減量は、鉄鋼製造プロセスでのスラグの発生量に依存し、蛇紋岩やカンラン岩等を利用する方法についても、これらの岩石の採掘や、ボーリングコストの費用が掛かるなどの問題があった。 As for the method of using uncarbonated Ca contained in the slag generated in the steel manufacturing process, the amount of CO 2 reduction depends on the amount of slag generated in the steel manufacturing process, such as serpentine and olivine. There were also problems such as the mining of these rocks and the cost of boring.
そこで、本発明は、上記従来の技術における問題点に鑑みてなされたものであって、ＣＯ2の漏洩や、環境への影響に関する問題がなく、低コストで二酸化炭素を固定化する新たな方法を提供することを目的とする。 Therefore, the present invention has been made in view of the above-mentioned problems in the prior art, and is a new method for immobilizing carbon dioxide at a low cost without problems related to CO 2 leakage and environmental impact. The purpose is to provide.
上記目的を達成するため、本発明者らは、鋭意研究を重ねた結果、従来の微粉炭燃焼による火力発電より発電効率が高く、ＣＯ2排出量が少ないため、今後微粉炭燃焼からの転換が予定されている石炭ガス化複合発電等に用いられる石炭ガス化技術に着目し、石炭ガス化炉へのフラックスの添加により生成したスラグに二酸化炭素を固定することができることを見出し、本発明をなすに至った。 In order to achieve the above object, the present inventors have conducted extensive research, and as a result, the power generation efficiency is higher than that of conventional thermal power generation by pulverized coal combustion and the amount of CO 2 emission is small. Focusing on the coal gasification technology used for coal gasification combined power generation, etc., it is found that carbon dioxide can be fixed to slag generated by adding flux to the coal gasification furnace, and the present invention is made. It came to.
すなわち、本発明は、二酸化炭素固定化方法であって、石炭をガス化する石炭ガス化炉にフラックスを添加し、該フラックスの添加により生成したスラグに、二酸化炭素を固定する二酸化炭素固定化方法であって、前記スラグは、ＣａＯを１０質量％以上６５質量％以下、ＭｇＯを１．０質量％以上３０質量％以下、Ｆｅ2Ｏ3を２．０質量％以上２５質量％以下含有するもののうち、前記二酸化炭素を５質量％以上３０質量％以下固定するものであることを特徴とする。 That is, the present invention is a carbon dioxide fixing method, wherein a flux is added to a coal gasification furnace for gasifying coal , and carbon dioxide is fixed to slag generated by the addition of the flux. a is, the slag, CaO 65 wt% to 10 wt%, 30 wt% to 1.0 wt% of MgO less, although containing Fe 2 O 3 2.0 wt% to 25 wt% or less of, characterized in that the carbon dioxide is intended for fixing 5% by weight to 30% by weight or less.
このフラックスとして、ＣａＯを５質量％以上５０質量％以下、ＭｇＯを０．５質量％以上２０質量％以下、Ｆｅ2Ｏ3を１．０質量％以上１５質量％以下含有するものを用いることで、生成したスラグに二酸化炭素をより多く固定することができる。 By using a flux containing 5% to 50% by weight of CaO, 0.5% to 20% by weight of MgO, and 1.0% to 15% by weight of Fe 2 O 3 as this flux. More carbon dioxide can be fixed to the generated slag.
また、上述のようにして生成されたスラグをコンクリート用骨材、地下空洞の充填材、裏込材又は埋め戻し材として利用することができる。但し、スラグをコンクリート用骨材として利用する場合には、コンクリートの中性化を防止するため、コンクリート中の遊離石灰の量を５質量％以下になるように調整する。 Moreover, the slag produced | generated as mentioned above can be utilized as an aggregate for concrete, a filler of an underground cavity, a backing material, or a backfilling material. However, when slag is used as an aggregate for concrete, the amount of free lime in the concrete is adjusted to 5% by mass or less in order to prevent the neutralization of the concrete.
さらに、前記スラグを骨材としてコンクリートを製造し、該コンクリートを藻礁、魚礁、海底山脈又は消波ブロックとして利用することができる。特に、上記コンクリートを藻礁として使用することで、藻礁に成長した海藻によって二酸化炭素を吸収し、さらに二酸化炭素吸収量を増加させることができる。 Furthermore, concrete can be produced using the slag as an aggregate, and the concrete can be used as algae reefs, fish reefs, submarine mountains or wave-dissipating blocks. In particular, by using the above concrete as an algae reef, carbon dioxide can be absorbed by seaweed grown on the algae reef, and the amount of carbon dioxide absorbed can be further increased.
以上のように、本発明によれば、ＣＯ2の漏洩や、環境への影響に関する問題がなく、低コストで二酸化炭素を固定化する新たな方法を提供することができる。 As described above, according to the present invention, it is possible to provide a new method for fixing carbon dioxide at a low cost without problems related to CO 2 leakage and environmental impact.
上述のように、本発明は、二酸化炭素固定化方法であって、石炭をガス化する石炭ガス化炉にフラックスを添加し、該フラックスの添加により生成したスラグに二酸化炭素を固定することを特徴とする。 As described above, the present invention is a carbon dioxide fixing method, wherein a flux is added to a coal gasification furnace that gasifies coal, and carbon dioxide is fixed to slag generated by the addition of the flux. And
上記石炭ガス化炉は、石炭ガス化複合発電設備等に用いられるものであって、図１に示すように、石炭ガス化炉に、石炭と、ガス化剤と、フラックスを供給し、高圧下で燃焼させ、生成ガスと蒸気を得るものであって、その際に溶融スラグが排出される。石炭ガス化複合発電設備では、前記生成ガスでガスタービンを回転させて発電するとともに、蒸気で蒸気タービンを回転させて発電を行う。ここで、ガス化剤に酸素を用いるのが酸素吹きガス化発電であり、ガス化剤に空気を用いるのが空気吹きガス化発電である。 The coal gasification furnace is used in a coal gasification combined power generation facility or the like, and as shown in FIG. 1, the coal gasification furnace is supplied with coal, a gasifying agent, and a flux under high pressure. In order to obtain product gas and steam, the molten slag is discharged. In the coal gasification combined cycle power generation facility, power is generated by rotating a gas turbine with the generated gas and rotating a steam turbine with steam. Here, oxygen-blown gasification power generation uses oxygen as the gasifying agent, and air-blown gasification power generation uses air as the gasifying agent.
上記石炭ガス化炉では、炉内に投入するガス化剤空気の量を少なくし、空気比を下げた運転を行うことにより生成ガス発熱量が高くなるなどガス化性能が高くなる。しかし、噴流床方式石炭ガス化炉では、石炭中の灰分を溶融スラグとして排出させるため、炉内の温度を灰の融点以上になるように運転し、灰融点の高い石炭（高灰融点炭）をガス化する場合には、炉内温度を高温に保つためにガス化剤空気の投入量を増加させて高空気比で運転する。その結果、高灰融点炭では、ガス化性能が低下する。 In the above coal gasification furnace, gasification performance is improved by reducing the amount of gasifying air introduced into the furnace and reducing the air ratio to increase the generated gas heat generation amount. However, in the spouted bed type coal gasifier, the ash content in the coal is discharged as molten slag, so the temperature in the furnace is operated to be higher than the melting point of ash, and coal with a high ash melting point (high ash melting point coal) Is gasified, the operation is performed at a high air ratio by increasing the input amount of gasifying agent air in order to keep the furnace temperature at a high temperature. As a result, with high ash melting point coal, gasification performance decreases.
そこで、高灰融点炭の灰融点を降下させ、低空気比運転を可能としてガス化性能を高く維持するため、フラックスを炉内に添加する。すなわち、フラックスは、高灰融点炭の灰融点を下げるために添加されるものであって、ＣａＯ、ＭｇＯ、Ｆｅ2Ｏ3、Ｎａ2Ｏ、Ｋ2Ｏ等の塩基性成分を多く含有する。 Therefore, flux is added to the furnace in order to lower the ash melting point of the high ash melting point coal, to enable operation at a low air ratio and to maintain high gasification performance. That is, the flux is added to lower the ash melting point of the high ash melting point coal, and contains a lot of basic components such as CaO, MgO, Fe 2 O 3 , Na 2 O, K 2 O and the like.
上述のように石炭ガス化炉で生成したスラグは、石炭ガス化炉内で１２００℃程度となっているが、その後冷却されて８００℃程度となり、石炭ガス化炉から排出されて水冷されてガラス状となる。このスラグの性状は、使用する石炭、添加されるフラックスにより異なり、種々の化学組成、結晶状態を呈する。 As described above, the slag generated in the coal gasification furnace is about 1200 ° C. in the coal gasification furnace, but is then cooled to about 800 ° C., discharged from the coal gasification furnace, and water-cooled to glass. It becomes a shape. The properties of this slag vary depending on the coal used and the added flux, and exhibit various chemical compositions and crystal states.
本発明者らは、このようにして生成されたスラグの化学組成、結晶状態より、該スラグにＣＯ2を固定することができる可能性があるものと考え、種々試験を行ったところ、該スラグにＣＯ2を固定することができることを確認した。 The present inventors considered that there was a possibility that CO 2 could be fixed to the slag from the chemical composition and crystal state of the slag thus produced, and various tests were conducted. It was confirmed that CO 2 can be fixed on the surface.
表１に示すように、３種類のガス化スラグと、鉄鋼スラグと、台湾蛇紋岩と、アリゾナカンラン岩を用意し、各々を７５μｍに粉砕し、φ１５ｍｍの型に入れて２０ｋｇ／ｍ3で成型したものをコンクリートの中性化促進試験装置を用い、２８日経過後にＣＯ2の増加率を測定したところ、表１に示すような結果となった。尚、ＣＯ2増加率は、試験前後のサンプルの重量の差を試験前のサンプルの重量で除して算出した。 As shown in Table 1, three types of gasification slag, steel slag, Taiwan serpentine, and Arizona peridotite are prepared, each pulverized to 75 μm, put into a 15 mm mold and molded at 20 kg / m 3 . When the increase rate of CO 2 was measured after elapse of 28 days using a concrete neutralization promotion test apparatus, the results shown in Table 1 were obtained. The CO 2 increase rate was calculated by dividing the difference in the weight of the sample before and after the test by the weight of the sample before the test.
Ｎｏ１〜３の３種類のガス化スラグについては、Ｎｏ１のガス化スラグＡのみが高いＣＯ2増加率を示すが、Ｎｏ２、Ｎｏ３のガス化スラグについては、ほとんどＣＯ2が増加することはなかった。この点より、ＣａＯ含有率がＣＯ2増加率に大きく影響しているものと推測できる。また、Ｎｏ３の鉄鋼スラグは、ＣＯ2増加率が１０％と高いが、これは、鉄鋼スラグのＣａＯ含有率が４２．９質量％と高く、さらにその略々半分が遊離石灰であることが理由であると推測される。さらに、Ｎｏ４、Ｎｏ５の台湾蛇紋岩、アリゾナカンラン岩について見ると、アリゾナカンラン岩が高いＣＯ2増加率を示している。アリゾナカンラン岩は、ＭｇＯ及びＦｅ2Ｏ3含有率が高いことから、これらがＣＯ2増加率の上昇に寄与しているものと推測される。 For the three types of gasification slags No. 1 to 3, only No. 1 gasification slag A shows a high CO 2 increase rate, but for No. 2 and No. 3 gasification slags, CO 2 hardly increased. . From this point, it can be estimated that the CaO content greatly affects the CO 2 increase rate. In addition, the No. 3 steel slag has a high CO 2 increase rate of 10%. This is because the CaO content of the steel slag is as high as 42.9% by mass, and almost half of it is free lime. It is estimated that. Furthermore, when looking at No4 and No5 Taiwan serpentine and Arizona peridotite, Arizona peridotite shows a high CO 2 increase rate. Arizona peridotite has a high content of MgO and Fe 2 O 3 , so it is presumed that these contribute to an increase in the CO 2 increase rate.
以上のように、ガス化スラグについて、その化学組成等を適切なものとすることにより、ＣＯ2の固定化が可能となるものと推測されるが、特に、ガス化スラグに含まれるＣａＯ、 ＭｇＯ及びＦｅ2Ｏ3含有率を調整することで、ＣＯ2の固定化可能量を上昇させることができる。ガス化スラグのこれらの化学組成は、ガス化の対象となる石炭の種類、添加するフラックスの種類等によって変化することから、石炭の種類に応じて適切なフラックスを選択する必要がある。 As described above, it is presumed that the gasification slag can be fixed with CO 2 by making the chemical composition and the like appropriate, and in particular, CaO, MgO contained in the gasification slag. By adjusting the Fe 2 O 3 content, the amount of CO 2 that can be immobilized can be increased. Since these chemical compositions of the gasification slag change depending on the type of coal to be gasified, the type of flux to be added, etc., it is necessary to select an appropriate flux according to the type of coal.
従って、ガス化スラグの対象となる石炭の種類にもよるが、石炭ガス化炉に添加するフラックスは、ＣａＯを５質量％以上５０質量％以下、ＭｇＯを０．５質量％以上２０質量％以下、Ｆｅ2Ｏ3を１．０質量％以上１５質量％以下含有するものが好ましい。このようなフラックスを用いることで、石炭ガス化炉に投入される種々の石炭に対応することができ、得られたガス化スラグのＣＯ2の固定化可能量を大きくすることができる。 Therefore, depending on the type of coal that is the target of the gasification slag, the flux added to the coal gasification furnace is CaO 5 mass% to 50 mass%, MgO 0.5 mass% to 20 mass%. , Fe 2 O 3 containing 1.0 mass% or more and 15 mass% or less is preferable. Such fluxes By using, can correspond to various coal is introduced into the coal gasification furnace, as possible out to increase the immobilizable amount of CO 2 resulting gasification slag.
また、生成されるガス化スラグについても、ガス化スラグの対象となる石炭の種類、及び添加するフラックスの化学組成等にもよるが、ＣａＯを１０質量％以上６５質量％以下、ＭｇＯを１．０質量％以上３０質量％以下、Ｆｅ2Ｏ3を２．０質量％以上２５質量％以下含有するものが好ましい。このようなガス化スラグであれば、ＣＯ2を５質量％以上３０質量％以下固定することが可能となる。 Further, the generated gasified slag also depends on the type of coal to be gasified slag and the chemical composition of the flux to be added, but CaO is 10 mass% or more and 65 mass% or less, and MgO is 1. Those containing 0% by mass to 30% by mass and Fe 2 O 3 of 2.0% by mass to 25% by mass are preferable. With such gasification slag, CO 2 can be fixed at 5 mass% or more and 30 mass% or less.
次に、上記ガス化スラグの利用方法の一例について説明する。図２に示すように、ガス化スラグを２〜５ｍｍ程度に粉砕し、コンクリート用の骨材を製造し、この骨材を用いてコンクリートを製造する。このコンクリートは、通常のコンクリートと同様の用途に用いることができる。特に、このコンクリートを用いて藻礁を製造し、海中に沈めて海藻を生やすと、海藻によって二酸化炭素を吸収することができ、さらに二酸化炭素吸収量を増加させることができる。 Next, an example of the utilization method of the said gasification slag is demonstrated. As shown in FIG. 2, gasified slag is pulverized to about 2 to 5 mm to produce an aggregate for concrete, and concrete is produced using this aggregate. This concrete can be used for the same use as ordinary concrete. In particular, when this concrete is used to produce algae reefs and sink into the sea to produce seaweeds, carbon dioxide can be absorbed by the seaweeds, and the amount of carbon dioxide absorbed can be increased.
また、前記ガス化スラグを、石炭等を採掘した後の廃坑、採石場跡等の地下空洞に充填材として用いることもできる。これにより、ガス化スラグを二酸化炭素の固定と、充填材としての利用の両方に用いることができる。現在、国家間で廃棄物を移動させることは条約で禁じられているが、上記ガス化スラグであれば、二酸化炭素の固定及び充填材として使用することができるため、国家間での移動も可能となり、石炭ガス化に用いた石炭を提供した国の石炭の廃坑に戻して充填材として用いることも可能となる。 The gasified slag can also be used as a filler in underground cavities such as abandoned mines and quarry ruins after mining coal or the like. Thereby, gasification slag can be used for both fixation of carbon dioxide and utilization as a filler. Currently, it is prohibited by the Convention to move waste between countries, but if it is the above gasification slag, it can be used as carbon dioxide fixation and filler, so it can also be moved between countries. Thus, it is possible to return to the abandoned coal mine in the country that provided the coal used for coal gasification and use it as a filler.
以上のように、本発明では、スラグにＣＯ2を化学的に吸収させて固定化するため、ＣＯ2の漏洩や、環境への影響に関する問題は発生しない。また、本発明では、石炭ガス化炉にフラックスを添加して生成したスラグにＣＯ2を固定するが、このフラックスは、本来高灰融点炭の灰融点を下げるために添加されるものである。従って、生成したスラグのＣＯ2を固定可能量を増加させる目的でフラックスの性状を調整する必要があるものの、ＣＯ2の固定そのものに要するコストは極めて低い。 As described above, in the present invention, since CO 2 is chemically absorbed and fixed in the slag, problems relating to CO 2 leakage and environmental impact do not occur. In the present invention, CO 2 is fixed to slag produced by adding a flux to a coal gasifier, and this flux is originally added to lower the ash melting point of high ash melting point coal. Therefore, although it is necessary to adjust the properties of the flux in order to increase the amount of CO 2 that can be fixed in the generated slag, the cost required for fixing CO 2 itself is extremely low.
Claims (4)
前記スラグは、ＣａＯを１０質量％以上６５質量％以下、ＭｇＯを１．０質量％以上３０質量％以下、Ｆｅ2Ｏ3を２．０質量％以上２５質量％以下含有するもののうち、前記二酸化炭素を５質量％以上３０質量％以下固定するものであることを特徴とする二酸化炭素固定化方法。 A carbon dioxide fixing method of fixing a carbon dioxide to a slag generated by adding a flux to a coal gasification furnace that gasifies coal ,
The slag, CaO 65 wt% to 10 wt%, 30 wt% to 1.0 wt% of MgO less, among those containing Fe 2 O 3 2.0 wt% to 25 wt% or less, the dioxide carbon dioxide immobilization method which characterized in that for fixing to 30 wt% to 5 wt% of carbon.
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