JP3566884B2 - Calcium-containing porous carbon material - Google Patents
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Description
【０００１】
【発明の属する技術分野】
本発明は、例えば排ガス中の塩素系ガスの除去などに用いて好適なカルシウム含有の多孔質炭素材料に関する。
【０００２】
【従来の技術】
例えば、多孔質炭素材料の代表である活性炭は、空気浄化、用材回収、上下水道処理、排水処理などに広く応用され、また木炭も、調湿材や河川浄化、土壌改良材として広く普及しており、例えば排ガス中の塩素系ガスや硫黄酸化物などの除去にも利用されているが、これらは多孔質炭素材料の内部の微細な細孔による吸着特性だけを利用しているに過ぎないのであった。
【０００３】
或いは、これらの活性炭を単独で利用するだけでなく、触媒活性を発現させるように、細孔表面に金属や塩化物を担持させた触媒担持の活性炭も、各種の反応に利用されており、この他に、活性炭の炭化前後に有機物と金属元とを混合させて、金属成分を微細に高分散させ、新たな触媒作用を発現させることも試みられているが、この技術では、炭素元に高価な樹脂を用い、金属元としてＣｏ, Ｎｉ，Ｃｕ，Ｐｔ，Ｍｏ，Ｆｅ等の触媒作用の知られているものを用いており、何れも機能的には、担持した金属の触媒作用を狙いにしたもので高価であった。
【０００４】
【発明が解決しようとする課題】
これらに代わる安価な塩素系ガスの除去技術として、活性炭と消石灰の粉末とを混合したものを、例えば焼却炉の煙道中に吹き込んで、焼却炉から排出される排ガス中の塩素系ガスを除去する技術が知られており、これは、消石灰と塩化水素ガスとの反応性と、活性炭のダイオキシン類などの他の塩素系物質の吸着性を利用したものであるが、消石灰の反応は粒子表面のみで起こるため反応性が低く、また、活性炭の吸着も十分、効率的に行われていないのが現状である。
【０００５】
本発明は、かゝる実情に鑑みて成されたものであって、例えば塩素系ガスや硫黄酸化物等との反応性を極めて高くしたカルシウム含有の多孔質炭素材料を提供することを目的としている。
【０００６】
【課題を解決するための手段】
上記の目的を達成するために、本発明によるカルシウム含有の多孔質炭素材料は、炭化させる前の植物性多孔質材料を水酸化カルシウムの溶液または懸濁液に浸漬させてその植物組織内にカルシウム系化合物を取り込んだ後に炭化させて、植物性多孔質材料中の炭化組織内に、ＣａＣＯ 3 が主体であるカルシウム系化合物を微細に高分散させた点に特徴がある。
【０００７】
即ち、植物性多孔質材料、例えば導管や仮導管を有する一般の木材や、ヤシ繊維やジュート、麻、ビンロウジュ等の連続気孔を有する植物繊維、その他、藁や籾殻、竹などは、これらを炭化させると、例えば木材では導管を作っている組織の微細な孔が多孔質化し、ヤシ繊維などの植物繊維では連続気孔を形成している組織が多孔質化し、更に、藁や籾殻、竹などについても繊維組織が多孔質化して、膨大な表面積を有する多孔質の炭素材料と化す。
【０００８】
一方、これらの植物性多孔質材料を炭化させる前に、これを水酸化カルシウムの溶液または懸濁液に浸漬させると、具体的には、ヤシ繊維やジュート、麻、ビンロウジュ等の連続気孔を有する植物繊維や藁、籾殻などの植物性多孔質材料については、これをそのまま用いて、水酸化カルシウムの溶液または懸濁液に浸漬させると、その植物組織内にカルシウム系化合物を取り込むことができる。
【０００９】
また、木材についても、これをチップ化したり木毛に加工したりして、或いは、おが屑を利用したりして、これを水酸化カルシウムの溶液または懸濁液に浸漬させると、導管や仮導管を作っている組織内の微細な孔にカルシウム系化合物を取り込むことができるのであり、また、竹についても同様であって、これらカルシウム系化合物を取り込んだ植物性多孔質材料を炭化させることで、植物性多孔質材料中の炭化組織内に、ＣａＣＯ 3 が主体であるカルシウム系化合物を微細に高分散させることができるのである。
【００１０】
従って、本発明によるカルシウム含有の多孔質炭素材料を、例えば排ガス中の塩素系ガスの除去に用いると、多孔質炭素材料のガス吸着特性と微細なカルシウム化合物の高い反応性とによって、塩素系ガスを高効率で除去できるのであり、これに加えて、植物性多孔質材料の炭化組織における細孔径を計測したところ、この孔径が１〜２ｎｍ付近に分布していることと、代表的なダイオキシンの厚みが約０．３ｎｍであって、ダイオキシン類の吸着は、１〜２ｎｍの細孔を有する活性炭が有効であるとされていることから、本発明のカルシウム含有の多孔質炭素材料によれば、ダイオキシン類の吸着も高効率で達成されるのである。
【００１１】
また、本発明によるカルシウム含有の多孔質炭素材料を燃焼時に使用すれば、ガス吸着特性と高い反応性とによって、排ガス中の硫黄酸化物を硫酸カルシウムとして高効率で除去できるのであり、このように除去率が高いことは即ち、従来の活性炭と消石灰の粉末との混合物の使用量に比較して、本発明による多孔質炭素材料の使用量を大幅に削減できるのであって、その分、使用済の炭素材料の例えば埋め立て処理等が軽減されることになる。
【００１２】
更に、カルシウム含有の多孔質炭素材料を水質浄化のプロセスに用いると、カルシウムを含有することで、トリハロメタン等の有機塩素系化合物の反応吸着性が高まり、高効率での水質浄化も達成されるのであって、植物性多孔質材料として、ヤシ繊維やジュート、麻などをコスト的に安価に入手できる上に、処理に苦慮している間伐材や倒木材料、籾殻なども利用できることから、本発明によるカルシウム含有の多孔質炭素材料によれば、ガス浄化や水質浄化にとって好適な材料がコスト的に安価に提供されるのである。
【００１３】
【発明の実施の形態】
以下、本発明の実施の形態を図面に基づいて説明する。図１は例えば焼却炉１の煙道に接続された排ガス処理設備の一部を示し、後述するカルシウム含有の多孔質炭素材料２の投入手段３と、この多孔質炭素材料２を捕捉するためのバグフィルター４とを備えている。
【００１４】
カルシウム含有の多孔質炭素材料２は、セルロースを主成分とする植物性多孔質材料を水酸化カルシウムの溶液または懸濁液に浸漬させてその植物組織内にカルシウム系化合物 を取り込んだ後に炭化させたものであって、この炭化によって、植物性多孔質材料中の炭化組織内に、ＣａＣＯ 3 が主体であるカルシウム系化合物が微細に高分散されることになる。
【００１５】
詳しくは、植物性多孔質材料として、例えばヤシ繊維やジュート、麻、ビンロウジュ、更には、竹や木材（間伐材、伐採木、廃木材など）、中でも好ましくは吸水性の高い針葉樹を、チップ化したものや木毛に加工したもの、更には、おが屑、藁、籾殻などを選択して、これを石灰水（水酸化カルシウムの溶液）または浸漬後表面に石灰が付着しない程度の薄い石灰乳（水酸化カルシウムの懸濁液）に３時間以上浸し、これを取り出して後に乾燥し、一般的な炭化炉を用いて炭化させるのであり、この際、石灰が表面に付着しない程度に植物性多孔質材料を石灰乳に浸すのは、石灰が大きな粒子になって、反応性が低下することが判明しているからである。
【００１６】
炭化の温度範囲は、４００〜１３００℃とし、好ましくは、６００〜１０００℃とするが、これは、４００℃付近の温度以下では、Ｃａ（ＯＨ）2 が分解せずに、冷却後そのままＣａ（ＯＨ）2 が残ってしまったり、炭化が十分に進まなかったりするからである。
【００１７】
また、１３００℃付近の温度以上で炭化させてもよいのであるが、これでは耐火物やエネルギーコストが極めて高くなることから、１３００℃以下としているのであり、実験結果では、６００〜１０００℃の温度範囲で、Ｃａ（ＯＨ）2 の分解が確実に起こり、かつ、炭素材料の表面積も確実に大きくなることが判明していることから、好適には、６００〜１０００℃の温度範囲で炭化させるものとしているのであって、この温度範囲で炭化させた炭素材料中のカルシウム化合物は、主にＣａＣＯ3 が主体となっており、反応性を高める上で、Ｃａとして１％以上を含ませることが必要であると考える。
【００１８】
具体的に、赤松のチップ（厚さ１ｍｍで５ｍｍ角）１００ｇを１０リットルの石灰水に３時間浸漬させ、１１０℃で半日乾燥させた後、９００℃で炭化させたところ、原料中のＣａ（ＯＨ）2 は主としてＣａＣＯ3 が主体となっており、炭素材料中にはＣａとして約６％を含有していた。
【００１９】
更に、ヤシ繊維についても、同様にして石灰水に浸漬後、炭化させたところ、Ｃａとして約７％を含有する炭素材料を得たのであり、このＣａの含有量が多い理由は、ヤシ繊維は吸水性が高いことに加えて、顕微鏡写真を図面化した図２に照らして明らかなように、ヤシ繊維ａは、その表面に、歪で複雑な形状の筋状の凹溝ｂを多数有する上に、複雑な形状の大小様々な窪みｃを有し、更に、図示はしないが、大小様々な連続細孔を中空状に有して、炭化組織全体の表面積が膨大であることから、その炭化組織内にＣａＣＯ3 （カルシウム系化合物）ｄが微細に高分散されることとなり、これによって、赤松のチップに比べてＣａの含有量が多なっているのである。
【００２０】
これらの炭化物０．５ｇを石英ガラス管中に置き、ＨＣｌ６００ｐｐｍのガスを２００℃で１時間通過させた時のＨＣｌ吸収量を測定した。比較として焼却炉用の活性炭３０％入り消石灰においても同様な試験を行った。
【００２１】
その結果、ＨＣｌ吸収量は、本発明品であるカルシウム含有の多孔質炭素材料２は、赤松のチップで５４％、ヤシ繊維で８３％を吸収したのに対して、活性炭入り消石灰では５２％であった。
【００２２】
この実験結果から明らかなように、ヤシ繊維ａによるカルシウム含有の多孔質炭素材料２を、例えば排ガス中の塩素系ガスの除去に用いると、多孔質炭素材料２のガス吸着特性と微細なカルシウム化合物の高い反応性とによって、排ガス中の塩素系ガスを高効率で除去することができる。
【００２３】
或いは、ヤシ繊維ａによるカルシウム含有の多孔質炭素材料２を例えば焼却炉に投入して、燃焼時に使用すれば、ガス吸着特性と高い反応性とによって、排ガス中の硫黄酸化物を硫酸カルシウムとして高効率で除去できるのであり、更に、水質浄化のプロセスに用いると、多孔質炭素材料２がカルシウムを含有することで、トリハロメタン等の有機塩素系化合物の反応吸着性が高まり、高効率での水質浄化も達成されるのである。
【００２４】
一方、赤松のチップによるカルシウム含有の多孔質炭素材料２については、活性炭入り消石灰と同じ程度のＨＣｌを吸収することから、この赤松のチップによるカルシウム含有の多孔質炭素材料２は、活性炭入り消石灰の代替え品として好適に用いることができるのであり、勿論、この多孔質炭素材料２は、排ガス中の脱硫や水質浄化にも大きな効果をもたらすことに変わりはない。
【００２５】
加えて、従来の活性炭入り消石灰では、バグフィルター４への付着が多くて集塵能力が低下し易いのに比較して、本発明によるカルシウム含有の多孔質炭素材料２は、バグフィルター４への付着が大幅に低減されるのであって、集塵能力の低下が抑止される上に、多孔質炭素材料２の回収が容易である点でも機能的に優れる。
【００２６】
【発明の効果】
以上説明したように本発明によれば、炭化させる前の植物性多孔質材料を水酸化カルシウムの溶液または懸濁液に浸漬させてその植物組織内にカルシウム系化合物を取り込んだ後に炭化させ、得られる多孔質の炭素材料中にＣａＣＯ 3 が主体であるカルシウム系化合物を微細に高分散させた反応性の高い材料、即ち、例えば排ガス中の塩素系ガスや硫黄酸化物等を高効率で除去できる上に、水質浄化も高効率で達成される好適な材料が、コスト的に安価に提供される。
【図面の簡単な説明】
【図１】排ガス処理設備の一部の構成図である。
【図２】顕微鏡写真を図面化し、かつ、その一部を取り出して拡大図示したヤシ繊維表面の模式図である。
【符号の説明】
ａ…植物性多孔質材料、ｄ…カルシウム系化合物。[0001]
TECHNICAL FIELD OF THE INVENTION
The present invention relates to a calcium-containing porous carbon material suitable for use, for example, for removing chlorine-based gas in exhaust gas.
[0002]
[Prior art]
For example, activated carbon, a representative of porous carbon materials, is widely applied to air purification, material recovery, water and sewage treatment, wastewater treatment, etc.Charcoal is also widely used as a moisture conditioner, river purification and soil improvement material. For example, they are also used to remove chlorine-based gas and sulfur oxides in exhaust gas.However, these use only the adsorption characteristics of fine pores inside the porous carbon material. there were.
[0003]
Alternatively, not only these activated carbons are used alone, but also a catalyst-supported activated carbon in which a metal or chloride is supported on the pore surface so as to exhibit catalytic activity, is also used for various reactions. Other attempts have been made to mix the organic matter with the metal source before and after the carbonization of the activated carbon to finely and highly disperse the metal component and to develop a new catalytic action. A resin with a known catalytic action, such as Co, Ni, Cu, Pt, Mo, Fe, etc., is used as a metal source. It was expensive.
[0004]
[Problems to be solved by the invention]
As an inexpensive technology for removing chlorine-based gas instead of these, a mixture of activated carbon and slaked lime powder is blown into, for example, the flue of an incinerator to remove chlorine-based gas in exhaust gas discharged from the incinerator. Technology is known, which utilizes the reactivity of slaked lime with hydrogen chloride gas and the adsorption of other chlorine-based substances such as dioxins in activated carbon, but the reaction of slaked lime is limited to the particle surface. As a result, the reactivity is low, and the adsorption of activated carbon is not sufficient and efficient at present.
[0005]
The present invention has been made in view of such circumstances, and has an object to provide a calcium-containing porous carbon material having extremely high reactivity with, for example, a chlorine-based gas or a sulfur oxide. I have.
[0006]
[Means for Solving the Problems]
In order to achieve the above-mentioned object, the calcium-containing porous carbon material according to the present invention is provided by immersing a plant porous material before carbonization in a solution or suspension of calcium hydroxide so that calcium is contained in the plant tissue. It is characterized in that a calcium-based compound mainly composed of CaCO 3 is finely and highly dispersed in a carbonized tissue of a plant porous material by carbonizing after taking in a system-based compound.
[0007]
That is, plant porous materials, for example, general wood having conduits and temporary conduits, plant fibers having continuous pores such as coconut fiber, jute, hemp, areca, etc., straw, chaff, bamboo, etc. For example, in wood, the fine pores of the tissue forming the conduit become porous, and in the plant fiber such as palm fiber, the tissue forming continuous pores becomes porous, and furthermore, straw, chaff, bamboo, etc. Also, the fibrous structure becomes porous, and becomes a porous carbon material having an enormous surface area.
[0008]
On the other hand, before carbonizing these vegetable porous materials, when they are immersed in a solution or suspension of calcium hydroxide, specifically, they have continuous pores such as coconut fiber, jute, hemp, areca, etc. For a plant porous material such as plant fiber, straw, and rice hull, if this is used as it is and immersed in a solution or suspension of calcium hydroxide, the calcium compound can be taken into the plant tissue.
[0009]
Also, when wood is turned into chips or processed into wool, or sawdust is used, and immersed in a calcium hydroxide solution or suspension, the pipe or temporary pipe is used. The calcium-based compound can be taken into the fine pores in the tissue that is making the same, and the same is true for bamboo, by carbonizing the plant-based porous material incorporating these calcium-based compounds, The calcium-based compound mainly composed of CaCO 3 can be finely and highly dispersed in the carbonized tissue in the vegetable porous material.
[0010]
Therefore, when the calcium-containing porous carbon material according to the present invention is used, for example, for the removal of chlorine-based gas in exhaust gas, the chlorine-based gas is removed due to the gas adsorption characteristics of the porous carbon material and the high reactivity of fine calcium compounds. Can be removed with high efficiency. In addition, when the pore size in the carbonized tissue of the plant porous material was measured, this pore size was distributed in the vicinity of 1 to 2 nm, and the typical dioxin According to the calcium-containing porous carbon material of the present invention, since the activated carbon having a pore of 1 to 2 nm is effective for adsorbing dioxins and having a thickness of about 0.3 nm, Dioxin adsorption is also achieved with high efficiency.
[0011]
Further, if the calcium-containing porous carbon material according to the present invention is used at the time of combustion, the sulfur oxides in the exhaust gas can be removed as calcium sulfate with high efficiency due to the gas adsorption characteristics and high reactivity. The high removal rate means that the use amount of the porous carbon material according to the present invention can be greatly reduced as compared with the use amount of a conventional mixture of activated carbon and slaked lime powder. For example, the landfill treatment of the carbon material is reduced.
[0012]
Furthermore, when a calcium-containing porous carbon material is used in the water purification process, the inclusion of calcium enhances the reactive adsorption of organic chlorinated compounds such as trihalomethane and achieves highly efficient water purification. Therefore, as a vegetable porous material, palm fiber, jute, hemp, etc. can be obtained at a low cost, and in addition, thinning materials, fallen tree materials, rice husks, etc., which are difficult to treat, can be used. According to the porous carbon material containing calcium, a material suitable for gas purification and water purification can be provided at a low cost.
[0013]
BEST MODE FOR CARRYING OUT THE INVENTION
Hereinafter, embodiments of the present invention will be described with reference to the drawings. FIG. 1 shows, for example, a part of an exhaust gas treatment facility connected to a flue of an incinerator 1, a charging means 3 for a calcium-containing
[0014]
The calcium-containing
[0015]
More specifically, as a porous vegetable material, for example, coconut fiber, jute, hemp, areca, bamboo and wood (thinned wood, cut wood, waste wood, etc.), and among them, preferably, conifers having high water absorption are formed into chips. And whisks, and also sawdust, straw, rice hulls, etc., which are then selected from lime water (a solution of calcium hydroxide) or thin lime milk (so that lime does not adhere to the surface after immersion) (Suspension of calcium hydroxide) for 3 hours or more, take out, dry, and carbonize using a general carbonization furnace. The material is immersed in milk of lime because it has been found that the lime becomes large particles and the reactivity is reduced.
[0016]
The temperature range of the carbonization is 400 to 1300 ° C., preferably 600 to 1000 ° C. At a temperature of around 400 ° C. or lower, Ca (OH) 2 does not decompose, This is because OH) 2 remains or carbonization does not proceed sufficiently.
[0017]
Further, carbonization may be performed at a temperature of about 1300 ° C. or higher. However, since refractory and energy costs are extremely high, the temperature is set to 1300 ° C. or lower. It has been found that the decomposition of Ca (OH) 2 surely occurs and the surface area of the carbon material surely increases within the range, so that carbonization is preferably performed in a temperature range of 600 to 1000C. The calcium compound in the carbon material carbonized in this temperature range is mainly composed of CaCO 3 , and it is necessary to contain 1% or more as Ca in order to enhance the reactivity. I believe that.
[0018]
Specifically, 100 g of Akamatsu chips (1 mm thick and 5 mm square) were immersed in 10 liters of lime water for 3 hours, dried at 110 ° C for half a day, and then carbonized at 900 ° C. OH) 2 was mainly composed of CaCO 3 , and contained about 6% as Ca in the carbon material.
[0019]
Furthermore, the coconut fiber was similarly immersed in lime water and carbonized to obtain a carbon material containing about 7% as Ca. The reason for the high Ca content was that coconut fiber was In addition to the high water absorption, as apparent from FIG. 2 in which the micrograph is drawn, the palm fiber a has a large number of strain-shaped concave grooves b on the surface thereof. In addition, it has variously large and small depressions c of a complicated shape, and further, although not shown, has continuous holes of various sizes large and small, and the surface area of the entire carbonized tissue is enormous. CaCO 3 (calcium-based compound) d is finely and highly dispersed in the tissue, thereby increasing the Ca content as compared with the Akamatsu chips.
[0020]
0.5 g of these carbides was placed in a quartz glass tube, and the amount of HCl absorbed when a gas containing 600 ppm of HCl was passed at 200 ° C. for 1 hour was measured. As a comparison, the same test was performed on slaked lime containing 30% activated carbon for incinerators.
[0021]
As a result, the absorption amount of HCl was 54% for the calcium-containing
[0022]
As is clear from the experimental results, when the
[0023]
Alternatively, if the
[0024]
On the other hand, the calcium-containing
[0025]
In addition, in contrast to the conventional slaked lime containing activated carbon, which adheres to the
[0026]
【The invention's effect】
As described above, according to the present invention, the vegetable porous material before carbonization is immersed in a solution or suspension of calcium hydroxide to incorporate the calcium-based compound into the plant tissue, and thereafter carbonized, Highly reactive material in which a calcium-based compound mainly composed of CaCO 3 is finely and highly dispersed in a porous carbon material to be obtained, that is, for example, a chlorine-based gas or sulfur oxide in an exhaust gas can be removed with high efficiency. In addition, a suitable material that can achieve water purification with high efficiency is provided at a low cost.
[Brief description of the drawings]
FIG. 1 is a configuration diagram of a part of an exhaust gas treatment facility.
FIG. 2 is a schematic view of a palm fiber surface in which a micrograph is drawn and a part thereof is taken out and enlarged.
[Explanation of symbols]
a: vegetable porous material; d: calcium-based compound.
Claims (2)
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| JP12725099A JP3566884B2 (en) | 1999-05-07 | 1999-05-07 | Calcium-containing porous carbon material |
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| JP12725099A JP3566884B2 (en) | 1999-05-07 | 1999-05-07 | Calcium-containing porous carbon material |
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| JP2000319011A JP2000319011A (en) | 2000-11-21 |
| JP3566884B2 true JP3566884B2 (en) | 2004-09-15 |
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| AU2002241523A1 (en) | 2000-11-29 | 2002-06-11 | Research Foundation Of The City University Of New York | Process to prepare adsorbents from organic fertilizer and their applications for removal of acidic gases from wet air streams |
| JP4804659B2 (en) * | 2001-07-11 | 2011-11-02 | 日本植生株式会社 | Method for producing porous carbon material for protein adsorption |
| US6962616B1 (en) | 2003-08-08 | 2005-11-08 | Research Foundation Of The City University Of New York | Preparation of adsorbents from organic fertilizer and mineral oil and their application for removal of acidic gases from sulfur containing wet gas streams |
| KR101393120B1 (en) | 2005-09-08 | 2014-05-08 | 리서치 파운데이션 오브 더 시티 유니버시티 오브 뉴욕 | Catalytic adsorbents obtained from municipal sludges, industrial sludges, compost and tobacco waste and process for their production |
| US20080300131A1 (en) | 2005-09-08 | 2008-12-04 | Research Foundation Of The City University Of New York | Catalytic adsorbents obtained from municipal sludges, industrial sludges, compost and tobacco waste and a rotary drying process for their production |
| JP4840846B2 (en) * | 2005-09-13 | 2011-12-21 | 秋田県 | Phosphorus recovery material, production method thereof, and fertilizer using phosphorus recovery material |
| CN103305950A (en) * | 2012-03-07 | 2013-09-18 | 行地纺织品有限公司 | Production method of betel nut yarn |
| WO2019049611A1 (en) * | 2017-09-08 | 2019-03-14 | 杉山 修 | Production method for hydrogen gas |
| CN114082404A (en) * | 2021-12-02 | 2022-02-25 | 中国热带农业科学院分析测试中心 | Betel nut waste-based biochar material and preparation method and application thereof |
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