JP7575052B2 - Carbon dioxide absorbent and method for recovering carbon dioxide from flue gas using the same. - Google Patents
Carbon dioxide absorbent and method for recovering carbon dioxide from flue gas using the same. Download PDFInfo
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- JP7575052B2 JP7575052B2 JP2020198341A JP2020198341A JP7575052B2 JP 7575052 B2 JP7575052 B2 JP 7575052B2 JP 2020198341 A JP2020198341 A JP 2020198341A JP 2020198341 A JP2020198341 A JP 2020198341A JP 7575052 B2 JP7575052 B2 JP 7575052B2
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Description
本発明は、石炭火力発電所において発生する大量の石炭灰を使用した二酸化炭素吸収材、及びそれを使用した排煙中の二酸化炭素の回収方法に関するものである。 The present invention relates to a carbon dioxide absorbent that uses the large amounts of coal ash generated at coal-fired power plants, and a method for recovering carbon dioxide from flue gas using the same.
現在、我が国においては、原子力発電所の再稼働が進まない中で、発電コストが低く安定供給が可能な石炭を燃料とする火力発電が主力電源となっており、最近では我が国の電力構成の３０％強に上っている。 Currently, in Japan, with no progress being made in restarting nuclear power plants, coal-fired thermal power generation, which has low generation costs and allows for a stable supply, has become the main source of electricity, and has recently accounted for just over 30% of the country's electricity mix.
一方、石炭火力は、石炭の燃焼に伴って、大量の石炭灰が生じ大量の二酸化炭素が排出されることから、環境重視、温暖化ガスの削減の意識が高まる中、風当たりが強い電源でもある。当面は石炭火力を活用せざるを得ない状況の中で、これらの二つの問題を解決することは重要な課題といえる。 However, coal-fired power generation is facing strong opposition amid growing concern for the environment and the need to reduce greenhouse gas emissions, as coal combustion produces large amounts of coal ash and emits large amounts of carbon dioxide. As we are faced with a situation in which we have no choice but to continue using coal-fired power generation for the time being, resolving these two issues is an important task.
かかる問題の解決方法として、石炭の燃焼設備から排出される石炭灰をスラリー化し、燃焼排ガスと気液接触させて燃焼廃ガス中の二酸化炭素を吸収させる方法（特許文献１）や、回収した石炭灰をゼオライト製造装置に導いてゼオライトを製造し、このゼオライトを使用して前記燃焼廃ガスから二酸化炭素を回収する方法(特許文献２)などが提案されている。 Methods proposed to solve this problem include a method in which coal ash discharged from coal combustion equipment is made into a slurry and then brought into gas-liquid contact with the combustion exhaust gas to absorb the carbon dioxide in the combustion exhaust gas (Patent Document 1), and a method in which recovered coal ash is led to a zeolite production device to produce zeolite, and this zeolite is used to recover carbon dioxide from the combustion exhaust gas (Patent Document 2).
しかし、前者の方法では二酸化炭素の回収率は１０％程度にとどまり、後者の方法では回収率は向上するものの、新たにゼオライト製造装置が必要となり、さらに石炭灰には、有害金属であるカドミウムや六価クロムなどの重金属が含まれていることから、いずれの方法も使用済み石炭灰の処理が必要であった。 However, the former method only captures about 10% of carbon dioxide, while the latter method improves the capture rate, but requires new zeolite production equipment. Furthermore, coal ash contains heavy metals such as cadmium and hexavalent chromium, which are harmful, so both methods require the disposal of used coal ash.
石炭灰中の重金属に対する既存の対処法としては、セメント材に配合して重金属を不溶化する方法（特許文献３，４）が主流であるが、石炭火力発電所の稼働が増加している状況では、処理能力が限界に近付いている。 The main existing method for dealing with heavy metals in coal ash is to insolubilize them by adding them to cement materials (Patent Documents 3 and 4), but with the increase in the operation of coal-fired power plants, the processing capacity is approaching its limit.
本発明者は、重量比が１：５～５：１の軽焼マグネサイトと軽焼ドロマイトを含む石炭灰の固化・不溶化剤に係る特許（特許文献５）を取得しているが、石炭灰には重金属だけでなくＡｓ、Ｆなどの陰イオン成分やＢのような非イオン成分などの有害物質も含まれており、係る固化・不溶化剤では、石炭灰中のすべての有害物質を不溶化することはできなかった。 The inventor has obtained a patent (Patent Document 5) for a coal ash solidification/insolubilization agent that contains lightly burned magnesite and lightly burned dolomite in a weight ratio of 1:5 to 5:1. However, coal ash contains not only heavy metals but also harmful substances such as anionic components such as As and F, and non-ionic components such as B, and this solidification/insolubilization agent was unable to insolubilize all of the harmful substances in the coal ash.
本発明は、石炭灰により空気あるいは排ガス中の二酸化炭素を回収するとともに石炭灰中に含まれる重金属や有害物質を不溶化する方法を提供することを目的とする。 The present invention aims to provide a method for recovering carbon dioxide from air or exhaust gas using coal ash and for insolubilizing heavy metals and harmful substances contained in the coal ash.
上記のような状況に鑑み、本発明者は、石炭灰により二酸化炭素の回収をするとともに石炭灰中に含まれる重金属を不溶化する方法について、鋭意検討した結果、従来の固化・不溶化剤（特許第3706618号）を改良発展させ、焼成温度及び焼成時間を調整することにより、その活性度（Mg含有量）を少なくとも５０％、好ましくは５５～６０％程度に高めた酸化マグネシウム、石膏、ドロマイト、硫酸第一鉄、熔成リン肥、及びカンラン石（Mg2SiO4、Fe2SiO4）を主成分とし、酸化マグネシウムとドロマイトの重量比が１：５～５：１である固化・不溶化剤を、石炭灰に添加混合した状態で、燃焼廃ガスのような二酸化炭素含有ガスと接触させて炭酸化すれば、石炭灰中の重金属だけでなくＡｓ，Ｆ，Ｂなどの有害成分も、石炭灰と強固に結合し、長期間にわたって溶出しないことを突き止め、本発明に至ったものである。
In view of the above circumstances, the present inventors have conducted extensive research into a method for recovering carbon dioxide from coal ash and insolubilizing heavy metals contained in the coal ash. As a result, the inventors have found that by improving and developing a conventional solidification/insolubilizing agent (Patent No. 3706618) and adjusting the firing temperature and firing time to increase the activity (Mg content) to at least 50%, preferably about 55 to 60%, a solidification/insolubilizing agent containing magnesium oxide, gypsum, dolomite, ferrous sulfate, molten phosphate fertilizer, and olivine (Mg 2 SiO 4 , Fe 2 SiO 4 ) as main components, with a weight ratio of magnesium oxide to dolomite of 1:5 to 5:1, and adding the resulting solidification/insolubilizing agent to coal ash and contacting it with a carbon dioxide-containing gas such as combustion exhaust gas to cause carbonation, not only the heavy metals in the coal ash but also harmful components such as As, F and B will bind firmly to the coal ash and will not dissolve for a long period of time, which has led to the present invention.
本発明の酸化マグネシウム、石膏、ドロマイト、硫酸第一鉄、熔成リン肥、及びカンラン石の混合物が、石炭灰中に含まれるカドミウムなどの重金属を不溶出化するメカニズムを図４で説明すると、大気中から大量の二酸化炭素を吸収すると、酸化マグネシウムが炭酸マグネシウムに炭化しながらその針状結晶を成長させる。一方、カドミウムも酸化されるが前記炭酸マグネシウムの針状結晶の成長中にその結晶内に取り込まれるため、長期間、重金属が溶出することがないと考えられる。 The mechanism by which the mixture of magnesium oxide, gypsum, dolomite, ferrous sulfate, molten phosphate, and olivine of the present invention prevents the dissolution of heavy metals such as cadmium contained in coal ash is explained using Figure 4. When a large amount of carbon dioxide is absorbed from the atmosphere, magnesium oxide carbonizes to magnesium carbonate and grows its needle-like crystals. On the other hand, cadmium is also oxidized, but is incorporated into the magnesium carbonate needle-like crystals as they grow, so it is believed that heavy metals will not dissolve for a long period of time.
本発明は、かかる知見に基づきなされたもので、次の通りのものである。
（１）酸化マグネシウム、石膏、ドロマイト、硫酸第一鉄、熔成リン肥、及びカンラン石（Mg2SiO4、Fe2SiO4）を含む、石炭の燃焼装置の燃焼残滓及び排ガスから回収される石炭灰用固化・不溶化剤。
（２）石炭の燃焼装置の燃焼残滓及び排ガスから回収される石炭灰に、酸化マグネシウム、石膏、ドロマイト、硫酸第一鉄、熔成リン肥、及びカンラン石（Mg2SiO4、Fe2SiO4）を添加混合してなる、二酸化炭素吸収材。
（３）石炭の燃焼装置の燃焼残滓及び排ガスから回収される石炭灰に、酸化マグネシウム、石膏、ドロマイト、硫酸第一鉄、熔成リン肥、及びカンラン石（Mg2SiO4、Fe2SiO4）を添加混合し、二酸化炭素含有ガスと気液接触させて炭酸化することを特徴とする石炭灰中の重金属不溶化方法。
（４）石炭の燃焼装置の燃焼残滓及び排ガスから回収される石炭灰に、酸化マグネシウム、石膏、ドロマイト、硫酸第一鉄、熔成リン、及びカンラン石（Mg2SiO4、Fe2SiO4）を添加混合し、石炭燃焼廃ガスと気液接触させて炭酸化することを特徴とする石炭燃焼廃ガス中の二酸化炭素回収方法。
The present invention has been made based on such findings and is as follows.
(1) A solidification and insolubilization agent for coal ash recovered from the combustion residue and exhaust gas of coal combustion equipment, which contains magnesium oxide, gypsum, dolomite, ferrous sulfate, molten phosphate fertilizer, and olivine (Mg 2 SiO 4 , Fe 2 SiO 4 ).
(2) A carbon dioxide absorbent comprising coal ash recovered from the combustion residue and exhaust gas of a coal combustion device, and magnesium oxide, gypsum, dolomite, ferrous sulfate, molten phosphate fertilizer, and olivine (Mg 2 SiO 4 , Fe 2 SiO 4 ).
( 3 ) A method for insolubilizing heavy metals in coal ash, comprising adding and mixing magnesium oxide, gypsum, dolomite, ferrous sulfate, molten phosphate fertilizer, and olivine ( Mg2SiO4 , Fe2SiO4 ) to coal ash recovered from the combustion residue and exhaust gas of a coal combustion device, and bringing the mixture into gas-liquid contact with a carbon dioxide-containing gas to carbonate it.
( 4 ) A method for recovering carbon dioxide from coal combustion waste gas, comprising adding and mixing magnesium oxide, gypsum, dolomite, ferrous sulfate, fused phosphorus, and olivine ( Mg2SiO4 , Fe2SiO4 ) to coal ash recovered from the combustion residue and exhaust gas of a coal combustion device, and bringing the mixture into gas-liquid contact with the coal combustion waste gas to carbonate it.
本発明の二酸化炭素吸収材を使用すれば、空気中や燃焼廃ガス中の二酸化炭素が高い効率で回収・除去することができ、二酸化炭素を十分吸収し、炭酸化された廃吸収材からは重金属が浸出することがないので、種々の用途に再利用が可能であり、投棄しても安全である。 By using the carbon dioxide absorbent of the present invention, carbon dioxide in the air or combustion waste gas can be recovered and removed with high efficiency, and since the waste absorbent absorbs carbon dioxide sufficiently and is carbonated, heavy metals do not leach out, so it can be reused for various purposes and is safe to discard.
以下、本発明の実施例に基づき具体的に説明する。但し、本発明は以下の実施例に限定されるものではない。 The present invention will be specifically explained below based on examples. However, the present invention is not limited to the following examples.
＜本発明の二酸化炭素吸収材を用いた二酸化炭素吸収実験＞
酸化マグネシウム、石膏、ドロマイト、硫酸第一鉄、１７％熔成リン肥、及びカンラン石（Mg2SiO4、Fe2SiO4）から成る薬剤として、アムスエンジニアリング社製固化剤（商品名、「エコハーモニィ EH2008T62」）を利用した。
（１）本発明の二酸化炭素吸収材の調製
・容器に、石炭灰と、酸化マグネシウム、石膏、ドロマイト、硫酸第一鉄、１７％熔成リン肥、及びカンラン石（Mg2SiO4、Fe2SiO4）から成る薬剤を５：１で配合した混合物を131ｇ加え、この混合物に純水51.8ｇ加えて、均一となるよう攪拌した。
・加水した混合物37.21gを46.5mmφ×15mm のガラス製シャーレに加え、これを90mmφ×20mmのプラスチックシャーレに移して直径50mmの円形に形を整え、蓋をした。
（２）二酸化炭素ガスの調製
・30Lガス分析用サンプリングバッグ（商品名「テドラーバッグ」）に既知濃度の二酸化炭素標準ガス（窒素ベース２種標準16.11％）1Lを加え、次いでゼロガス（窒素ガス）16.9Lを加えて、二酸化炭素濃度8000ppmの実験用ガスとした。
（３）試験条件の設定
・20Lガス分析用サンプリングバッグ（商品名「テドラーバッグ」）に切り込みを入れ、上記混合物を入れたシャーレを蓋つきのまま前記切込み部分から入れる。
・切込み部をシーラーで密封し、ポンプでガス分析用サンプリングバッグ内の空気を抜く。
・注射筒を用いて、二酸化炭素濃度8000ppmの実験用ガスを5L注入した。
・実験は、ガス分析用サンプリングバッグ内のプラスチックシャーレの蓋をバッグの外から手で開けることによって開始する。
・所定時間におけるガス分析用サンプリングバッグ内の二酸化炭素濃度を、検知管により採取したガスで計測した。その結果を表１及び図１に示す。
本発明の二酸化炭素吸収材によれば、8,000ppmの二酸化炭素を48時間で二酸化炭素濃度は不検出（100ppm未満）にすることができた。
<Carbon dioxide absorption experiment using the carbon dioxide absorbent of the present invention>
A solidifying agent manufactured by Ams Engineering (trade name: "Eco Harmony EH2008T62") was used as the agent consisting of magnesium oxide, gypsum, dolomite, ferrous sulfate, 17% molten phosphate fertilizer, and olivine (Mg 2 SiO 4 , Fe 2 SiO 4 ).
( 1 ) Preparation of the carbon dioxide absorbent of the present invention: 131 g of a mixture of coal ash and chemicals consisting of magnesium oxide, gypsum, dolomite, ferrous sulfate, 17% molten phosphate fertilizer, and olivine ( Mg2SiO4 , Fe2SiO4 ) in a 5:1 ratio was added to a container, and 51.8 g of pure water was added to this mixture and stirred to make it uniform.
- 37.21 g of the hydrated mixture was added to a 46.5 mm φ x 15 mm glass petri dish, this was then transferred to a 90 mm φ x 20 mm plastic petri dish, shaped into a circle with a diameter of 50 mm, and covered.
(2) Preparation of carbon dioxide gas: 1 L of carbon dioxide standard gas of known concentration (nitrogen-based type 2 standard 16.11%) was added to a 30 L gas analysis sampling bag (product name "Tedlar Bag"), and then 16.9 L of zero gas (nitrogen gas) was added to prepare experimental gas with a carbon dioxide concentration of 8,000 ppm.
(3) Setting of test conditions: Make an incision in a 20 L gas analysis sampling bag (product name "Tedlar Bag"), and insert the petri dish containing the above mixture with the lid still attached through the incision.
- Seal the cut with a sealer and use a pump to remove the air from inside the sampling bag for gas analysis.
- Using a syringe, 5L of experimental gas with a carbon dioxide concentration of 8000ppm was injected.
- The experiment begins by manually opening the lid of a plastic petri dish inside the gas analysis sampling bag from outside the bag.
The carbon dioxide concentration in the sampling bag for gas analysis was measured at a specified time using the gas sampled by a detector tube. The results are shown in Table 1 and Figure 1.
According to the carbon dioxide absorbent of the present invention, it was possible to reduce the carbon dioxide concentration from 8,000 ppm to undetectable levels (less than 100 ppm) within 48 hours.
・累計吸収量（mg）＝吸収量（mg）＋ 前回までの累計吸収量（mg）
・1m2あたりの累計吸収量（g）＝ 累計吸収量（mg）× 10-3 ÷ 混合品表面積（cm2）× 10-4
・Cumulative absorption amount (mg) = Absorption amount (mg) + Cumulative absorption amount up to the previous time (mg)
・Cumulative absorption amount per 1m2 (g) = Cumulative absorption amount (mg) x 10-3 ÷ Mixed product surface area ( cm2 ) x 10-4
本実験で使用した混合物の表面積35.34cm2（概ね50mmφ×10mm）及び重量変化から、本発明の混合物の1ｍ２当たりの累積二酸化炭素吸収量の経時変化は図２のようになった。 From the surface area of the mixture used in this experiment, 35.34 cm 2 (approximately 50 mmφ×10 mm), and the weight change, the change over time in the cumulative carbon dioxide absorption amount per m 2 of the mixture of the present invention is shown in FIG.
［比較例１］
＜石炭灰に代えて砂を用いた試験＞
実施例１で石炭灰に代えて山砂（A）、及び再生砂（B）を使用し、薬剤と精製水を下記表に示される様に加えて実施例１と同様に固化してペレット状とし、二酸化炭素濃度が5400ppmの空気を、実施例１と同様な容器中にそれぞれ入れて密封し、容器中の気体の二酸化炭素濃度の経時的変化を計測した。その結果を表２に示す。
[Comparative Example 1]
<Test using sand instead of coal ash>
Instead of coal ash in Example 1, mountain sand (A) and reclaimed sand (B) were used, and chemicals and purified water were added as shown in the table below, and solidified into pellets in the same manner as in Example 1. Air with a carbon dioxide concentration of 5400 ppm was placed in a container similar to that in Example 1 and sealed, and the change over time in the carbon dioxide concentration of the gas in the container was measured. The results are shown in Table 2.
表２から明らかなように、薬剤の添加量を増やすと吸収速度は増加するが、これらの二酸化炭素吸収材では、４８時間を過ぎても二酸化炭素を完全に吸収することができなかった。 As is clear from Table 2, the absorption rate increases with an increase in the amount of the agent added, but these carbon dioxide absorbents were unable to completely absorb carbon dioxide even after 48 hours.
＜本発明の薬剤による焼却灰中の有害物質の溶出試験＞
中部電力の発電施設から排出されたフライアッシュを用い、本発明の薬剤による有害物質の不溶化実験を行った。
使用したフライアッシュの物性は以下の表３に示す通りで、Ｃｄ，ＣＮ，Ｐｂ，Ｃｒ＋6，Ａｓ，Ｈｇ，Ｓｅ，Ｆ，及びＢの含有量は環境基準をクリアーしているが、Ｃｒ＋6，Ａｓ，Ｓｅ，Ｆ，及びＢの溶出量は環境基準値をオバーしていた。
<Elution test of harmful substances in incineration ash using the agent of the present invention>
Using fly ash discharged from a power generation facility of Chubu Electric Power, an experiment was carried out on the insolubilization of harmful substances using the agent of the present invention.
The physical properties of the fly ash used are shown in Table 3 below. The contents of Cd, CN, Pb, Cr +6 , As, Hg, Se, F, and B met environmental standards, but the leaching amounts of Cr +6 , As, Se, F, and B exceeded the environmental standards.
上記フライアッシュ300gに、酸化マグネシウム、石膏、ドロマイト、硫酸第一鉄、１７％熔成リン肥、及びカンラン石（Mg2SiO4、Fe2SiO4）から成る薬剤（アムスエンジニアリング社製固化剤、商品名、「エコハーモニィ EH2008TX-27」）11ｇ及び高炉Ｂ型セメント45.0ｇを添加混合して、固化した４日間養生した試料片により、原灰で環境基準値をオバーしていたＣｒ＋6，Ａｓ，Ｓｅ，Ｆ，及びＢについて溶出試験を行った。溶出量の測定は、環境省告示第18号に基づき、成分ごとにＪＩＳ規格に定められた方法により行った。
結果は表４に示す通りで、いずれも環境基準値をクリアーしていた。
11g of a chemical consisting of magnesium oxide, gypsum, dolomite, ferrous sulfate, 17 % molten phosphate fertilizer, and olivine ( Mg2SiO4 , Fe2SiO4 ) (solidifying agent manufactured by AMS Engineering, product name "Eco Harmony EH2008TX-27") and 45.0g of blast furnace type B cement were added to 300g of the above fly ash, mixed, and cured for 4 days to perform elution tests on Cr +6 , As, Se, F, and B, which exceeded the environmental standard values in the raw ash. The elution amount was measured according to the method specified in the JIS standard for each component, based on Notification No. 18 of the Ministry of the Environment.
The results are shown in Table 4, and all of the results met the environmental standards.
本実験では、石炭灰に積極的に二酸化炭素を吸収していないが、養生中に空気中の微量な二酸化炭素が吸収された可能性があり、図４の理論に従えば、燃焼廃ガスとの接触により積極的に二酸化炭素を吸収させれば、石炭灰中の重金属や有害物質の溶出量をさらに減少させることが期待できる。 In this experiment, the coal ash did not actively absorb carbon dioxide, but it is possible that trace amounts of carbon dioxide from the air were absorbed during curing. According to the theory in Figure 4, if carbon dioxide is actively absorbed by contact with combustion exhaust gas, it is expected that the amount of heavy metals and harmful substances leaching out of the coal ash can be further reduced.
上記実施例１によれば、本発明の固化、不溶化剤を20重量％添加混合し固化した石炭灰は、１m2当たり最大で二酸化炭素を16.51ｇ吸収できることが分かった。
本発明の固化、不溶化剤を20重量％添加混合し固化した石炭灰１m3から１cm角の立方体の小片を106個作った場合、その表面積は6×106cm2＝600m2となる。
上記固化物の比重は約0.7なので、固化物１t当たりの二酸化炭素吸収量は、
600m2×16.51g/m2÷0.7＝14150g＝14.15kg
となる。
According to the above Example 1, it was found that coal ash solidified by adding and mixing 20% by weight of the solidification and insolubilization agent of the present invention can absorb a maximum of 16.51 g of carbon dioxide per 1 m2 .
When 10 6 small cubes with a size of 1 cm on a side are made from 1 m 3 of coal ash that has been solidified by adding and mixing 20% by weight of the solidifying and insolubilizing agent of the present invention, the surface area of each cube is 6 x 10 6 cm 2 = 600 m 2 .
The specific gravity of the solidified material is about 0.7, so the amount of carbon dioxide absorbed per ton of solidified material is:
600m 2 ×16.51g/m 2 ÷0.7=14150g=14.15kg
It becomes.
１cm角の小片とした上記固化物を、燃焼排ガスなどと接触させれば、固化物１t当たり最大で二酸化炭素14.15kgを吸収させることが可能であり、吸収後の固化物からは、石炭灰中の有害物質の溶出がないので、各種構造物の骨材、舗装道路の路盤材、埋め立て工事における地盤強化材として安全に利用できる。 When the above solidified material, cut into small pieces measuring 1 cm square, is brought into contact with combustion exhaust gas, it is possible to absorb up to 14.15 kg of carbon dioxide per ton of solidified material. Since the solidified material does not leach harmful substances from the coal ash after absorption, it can be safely used as aggregate for various structures, roadbed material for paved roads, and as a ground reinforcement material in landfill work.
また、実施例２によれば、本発明の固化・不溶化剤とセメントなどの固化剤を添加混合し固化した石炭灰は、大気中で十分養生させることにより、石炭灰中の有害物質の溶出が環境基準を満たす数値まで減少させることができるので、そのまま各種建造物や建築物の外壁や通水性を有する舗装道路の路盤材として利用すれば、建築物、構造物、あるいは道路自体に二酸化炭素吸収機能を持たせることができる。 In addition, according to Example 2, coal ash solidified by adding and mixing the solidification/insolubilization agent of the present invention with a solidification agent such as cement can be sufficiently cured in the atmosphere to reduce the leaching of harmful substances in the coal ash to a value that satisfies environmental standards. Therefore, if the coal ash is used as it is for the exterior walls of various buildings and structures, or as a roadbed material for paved roads that have water permeability, the building, structure, or road itself can have a carbon dioxide absorption function.
Claims (4)
A method for recovering carbon dioxide from coal combustion waste gas, comprising the steps of: adding magnesium oxide, in which the activity of magnesium has been increased to 50% to 60%, to coal ash recovered from the combustion residue and exhaust gas of a coal combustion device; adding gypsum, dolomite, ferrous sulfate, molten phosphate fertilizer, and olivine ( Mg2SiO4 , Fe2SiO4 ) so that the weight ratio of magnesium oxide to dolomite is 1:5 to 5:1; mixing and hydrating the mixture; and bringing the mixture into gas-liquid contact with the coal combustion waste gas to carbonate it.
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