JP2001247879A - Process for producing hydrogen and carbon monoxide from combustible waste - Google Patents
Process for producing hydrogen and carbon monoxide from combustible wasteInfo
- Publication number
- JP2001247879A JP2001247879A JP2000063127A JP2000063127A JP2001247879A JP 2001247879 A JP2001247879 A JP 2001247879A JP 2000063127 A JP2000063127 A JP 2000063127A JP 2000063127 A JP2000063127 A JP 2000063127A JP 2001247879 A JP2001247879 A JP 2001247879A
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- JP
- Japan
- Prior art keywords
- thermal decomposition
- oxygen concentration
- carbon monoxide
- ratio
- tar
- 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.)
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Classifications
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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
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
- Y02E50/00—Technologies for the production of fuel of non-fossil origin
- Y02E50/30—Fuel from waste, e.g. synthetic alcohol or diesel
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- Processing Of Solid Wastes (AREA)
- Hydrogen, Water And Hydrids (AREA)
Abstract
Description
【０００１】[0001]
【発明の属する技術分野】本発明は、可燃性廃棄物から
水素と一酸化炭素を製造する方法に関する。水素と一酸
化炭素に富むガスは、燃料電池燃料や、アンモニア、メ
タノール等合成用原料として有効利用することができ
る。[0001] The present invention relates to a method for producing hydrogen and carbon monoxide from combustible waste. The gas rich in hydrogen and carbon monoxide can be effectively used as a fuel for fuel cells, or a raw material for synthesis such as ammonia and methanol.
【０００２】[0002]
【従来の技術】従来、廃棄物をガス化し水素および一酸
化炭素を製造するには、１）特開平１０−１２８２８８
および特開昭５７−３０７９４号公報に示すように、石
炭のガス化などの手法を用いて、廃棄物に酸素、水蒸気
を反応させる方法、２）原料を直接高温下に晒して熱分
解する方法が提案されていた。2. Description of the Related Art Conventionally, it has been required to gasify waste to produce hydrogen and carbon monoxide. 1) JP-A-10-128288
And Japanese Unexamined Patent Publication (Kokai) No. 57-30794, a method of reacting waste with oxygen and water vapor using a technique such as gasification of coal, and 2) a method of directly subjecting raw materials to high temperature and thermally decomposing them. Had been proposed.
【０００３】[0003]
【発明が解決しようとする課題】しかし、前者の方法に
よると、分解反応において酸素、水蒸気を添加する為、
生成ガス中に二酸化炭素が混入したりして、生成ガスの
発熱量を低下させ、生成ガスの低位発熱量は１，５００
ｋｃａｌ／Ｎｍ３ 未満となってしまう。However, according to the former method, since oxygen and steam are added in the decomposition reaction,
For example, carbon dioxide is mixed in the generated gas to lower the calorific value of the generated gas, and the lower calorific value of the generated gas is 1,500.
It becomes kcal / Nm less than 3.
【０００４】また、後者の方法では、熱分解ガス中にタ
ール分が混入してしまい、目的とするガスは回収できな
い。[0004] In the latter method, tar components are mixed in the pyrolysis gas, and the target gas cannot be recovered.
【０００５】本発明の課題は、従来技術の上記問題点を
解消した、可燃性廃棄物からの水素と一酸化炭素の製造
方法を提供することである。An object of the present invention is to provide a method for producing hydrogen and carbon monoxide from combustible waste, which solves the above-mentioned problems of the prior art.
【０００６】[0006]
【課題を解決するための手段】本発明は、（揮発分）／
（固定炭素）比１以上の可燃性廃棄物を酸素濃度３ｖｏ
ｌ％以下の低酸素濃度雰囲気下で温度４００〜１，００
０℃で１次熱分解した後、酸素濃度３ｖｏｌ％以下の低
酸素濃度雰囲気下で温度１，０００〜１，５００℃で２
次熱分解することを特徴とする、可燃性廃棄物からの水
素と一酸化炭素の製造方法を提供するものである。According to the present invention, there is provided a method for producing (volatile) /
(Fixed carbon) Combustible waste with a ratio of 1 or more with an oxygen concentration of 3 vo
temperature of 400 to 1,000 in a low oxygen concentration atmosphere of 1% or less.
After primary pyrolysis at 0 ° C., the mixture is heated at 1,000 to 1,500 ° C. under a low oxygen concentration atmosphere having an oxygen concentration of 3 vol% or less.
It is intended to provide a method for producing hydrogen and carbon monoxide from combustible waste, which is characterized by secondary pyrolysis.
【０００７】本発明方法を適用できる可燃性廃棄物は、
（揮発分）／（固定炭素）比が１以上のものである。ま
た、本発明方法を適用できる可燃性廃棄物は、低酸素濃
度雰囲気での熱分解により、好ましくは（水）／（ター
ル分）比＝０．５〜１．５の割合で水とタール分を生成
するものである。低酸素濃度雰囲気は酸素濃度０〜３ｖ
ｏｌ％の雰囲気である。１次熱分解温度は４００〜１，
０００℃、好ましくは５００〜８００℃で、２次熱分解
温度は１，０００〜１，５００℃、好ましくは１，１０
０〜１，３００℃である。The flammable waste to which the method of the present invention can be applied includes:
(Volatile) / (fixed carbon) ratio is 1 or more. In addition, the combustible waste to which the method of the present invention can be applied is preferably composed of water and tar components at a ratio of (water) / (tar component) = 0.5 to 1.5 by thermal decomposition in a low oxygen concentration atmosphere. Is generated. Low oxygen concentration atmosphere is oxygen concentration 0-3v
ol% atmosphere. Primary pyrolysis temperature is 400 ~ 1,
2,000 ° C., preferably 500 to 800 ° C., and a secondary pyrolysis temperature of 1,000 to 1,500 ° C., preferably 1,10 ° C.
0 to 1,300 ° C.
【０００８】本発明において、タール分とは、熱分解に
より生成するガス中に含まれる炭素数３以上の炭化水素
を言い、揮発分、固定炭素とは、ＪＩＳＭ８８１２の方
法で測定される揮発分および固定炭素の値を言う。In the present invention, the term “tar” refers to a hydrocarbon having 3 or more carbon atoms contained in a gas generated by thermal decomposition, and the terms “volatile” and “fixed carbon” refer to volatile and fixed carbon measured by the method of JIS M8812. It refers to the value of fixed carbon.
【０００９】[0009]
【発明の実施の形態】本発明を図面に示す実施例に基づ
いて具体的に説明する。DESCRIPTION OF THE PREFERRED EMBODIMENTS The present invention will be specifically described based on embodiments shown in the drawings.
【００１０】まず、実験装置の概要を説明する。First, the outline of the experimental apparatus will be described.
【００１１】廃棄物は、表１に示す性状のごみ再生固形
燃料（ＲＤＦ）である。The waste is refuse-recycled solid fuel (RDF) having the properties shown in Table 1.
【００１２】このＲＤＦは（揮発分）／（固定炭素）比
＞１のものである。５００〜１２００℃の温度範囲で、
酸素濃度＝０［ｖｏｌ％］雰囲気下での、ＲＤＦの熱分
解生成物割合は表２および図１に示す通りである。これ
らより、このＲＤＦは、５００〜１２００℃の温度範囲
で、（水）／（タール分）＝０．５〜１．５［ｋｇ／ｋ
ｇ］のものであることが判る。The RDF has a ratio of (volatile matter) / (fixed carbon)> 1. In the temperature range of 500-1200 ° C,
The ratio of the pyrolysis products of RDF under the atmosphere of oxygen concentration = 0 [vol%] is as shown in Table 2 and FIG. From these, this RDF is (water) / (tar content) = 0.5 to 1.5 [kg / k] in the temperature range of 500 to 1200 ° C.
g].
【００１３】図４において、第１段熱分解炉(1) および
第２段熱分解炉(2) を酸素濃度３ｖｏｌ％以下の低酸素
濃度雰囲気で所定温度に過熱しておいて、上記ＲＤＦを
供給量１０［ｋｇ／ｈ］で第１段熱分解炉(1) に投入
し、第１段熱分解炉(1) および第２段熱分解炉(2) にて
熱分解する。第２段熱分解炉(2) 出口の水素、一酸化炭
素、メタン等のガス組成を経時的にガスクロマトグラフ
（ＴＣＤ）で測定し、平衡状態となったところでデータ
を取る。図４中、(3) (4) (5) は温度制御ヒータ、(6)
はガスクロマトグラフ分析計、(7) は真空ポンプ、(8)
はＲＤＦ投入フィーダー、(9) は撹拌モータ、(10)はイ
ンバータ、(11)はジャケットである。In FIG. 4, the first stage pyrolysis furnace (1) and the second stage pyrolysis furnace (2) are superheated to a predetermined temperature in a low oxygen concentration atmosphere having an oxygen concentration of 3 vol% or less, and the RDF is removed. At a supply rate of 10 [kg / h], it is charged into the first-stage pyrolysis furnace (1) and pyrolyzed in the first-stage pyrolysis furnace (1) and the second-stage pyrolysis furnace (2). The gas composition of hydrogen, carbon monoxide, methane, etc. at the outlet of the second-stage pyrolysis furnace (2) is measured over time with a gas chromatograph (TCD), and data is taken when the equilibrium state is reached. In FIG. 4, (3), (4) and (5) are temperature control heaters, and (6)
Is a gas chromatograph analyzer, (7) is a vacuum pump, (8)
Is an RDF feeding feeder, (9) is a stirring motor, (10) is an inverter, and (11) is a jacket.
【００１４】（比較例１）第１段熱分解炉(1) の熱分解
温度を５００、８００、１２００℃とし、第２段熱分解
炉(2) での処理は行わず、第１段熱分解炉(1) 出口での
ガスとタールの生成割合を測定した。この結果を表３お
よび図２に示す。これらから、熱分解温度が高くなる
と、ガスの生成割合が増加し、８００℃以上の熱分解温
度では、約４５〜５０［ｗｔ％］のガスが生成した。ま
た、タール分は温度上昇とともに減少するものの、１２
００℃であっても２０［ｗｔ％］生成した。(Comparative Example 1) The first-stage pyrolysis furnace (1) was set at a pyrolysis temperature of 500, 800, or 1200 ° C., and was not treated in the second-stage pyrolysis furnace (2). The rate of gas and tar production at the outlet of the cracking furnace (1) was measured. The results are shown in Table 3 and FIG. From these, when the thermal decomposition temperature was increased, the gas generation ratio was increased, and at a thermal decomposition temperature of 800 ° C. or higher, about 45 to 50 wt% of gas was generated. Although the tar content decreases with increasing temperature,
Even at 00 ° C., 20 wt% was formed.
【００１５】水素と一酸化炭素の生成量を図３に示す。
水素と一酸化炭素の生成量は、温度上昇とともに増加
し、１２００℃ではそれぞれ２９０［Ｎｍ３ ／ｋｇ
（ＲＤＦ）］と１６７［Ｎｍ３ ／ｋｇ］であった。ま
た、メタンも１００［Ｎｍ３ ／ｋｇ］生成した。FIG. 3 shows the amounts of hydrogen and carbon monoxide generated.
The production amounts of hydrogen and carbon monoxide increase with increasing temperature, and at 1200 ° C., 290 [Nm 3 / kg
(RDF)] and 167 [Nm 3 / kg]. In addition, methane was also produced at 100 [Nm 3 / kg].
【００１６】（実施例１）第１段熱分解炉(1) の熱分解
温度を５００℃とし、第２段熱分解炉(2) の熱分解温度
１２００℃とし、酸素濃度３ｖｏｌ％以下の低酸素濃度
雰囲気で上記ＲＤＦを供給量１０［ｋｇ／ｈ］で第１段
熱分解炉(1) に投入し、第１段熱分解炉(1) および第２
段熱分解炉(2) にて熱分解した。第２段熱分解炉(2) 出
口のガスとタールの生成割合を測定した。この結果を表
３および図２に示す。これらからタール分が完全に分解
したことが判る。ガス生成割合も向上し、４０［ｗｔ
％］の成分がガスとなった。(Example 1) The first stage pyrolysis furnace (1) had a pyrolysis temperature of 500 ° C., the second stage pyrolysis furnace (2) had a pyrolysis temperature of 1200 ° C., and had a low oxygen concentration of 3 vol% or less. The above RDF is supplied to the first-stage pyrolysis furnace (1) at a supply rate of 10 kg / h in an oxygen concentration atmosphere, and the first-stage pyrolysis furnace (1) and the second
It was pyrolyzed in a two-stage pyrolysis furnace (2). The rate of gas and tar formation at the outlet of the second-stage pyrolysis furnace (2) was measured. The results are shown in Table 3 and FIG. From these, it can be seen that the tar component was completely decomposed. Gas generation ratio also improved, 40 [wt]
%] Became gas.
【００１７】水素と一酸化炭素の生成量を図３に示す。
水素と一酸化炭素の生成量が上昇し、それぞれ４５０
［Ｎｍ３ ／ｋｇ］と２６１［Ｎｍ３ ／ｋｇ］であっ
た。また、メタンはほとんど生成せず、その生成量はわ
ずか７．２［Ｎｍ３ ／ｋｇ］であった。FIG. 3 shows the amounts of hydrogen and carbon monoxide generated.
Hydrogen and carbon monoxide production increased to 450
[Nm 3 / kg] and 261 [Nm 3 / kg]. Further, almost no methane was produced, and the produced amount was only 7.2 [Nm 3 / kg].
【００１８】（実施例２）第１段熱分解炉(1) の熱分解
温度を８００℃とし、第２段熱分解炉(2) の熱分解温度
を１２００℃とし以外、実施例１と同様にして、ガスと
タールの生成割合を測定した。この結果を表３および図
２に示す。これらから、タール分が完全に分解したこと
が判る。ガス生成割合も向上し、５０［ｗｔ％］の成分
がガスとなった。Example 2 Same as Example 1 except that the first stage pyrolysis furnace (1) had a pyrolysis temperature of 800 ° C. and the second stage pyrolysis furnace (2) had a pyrolysis temperature of 1200 ° C. Then, the generation ratio of gas and tar was measured. The results are shown in Table 3 and FIG. From these, it can be seen that the tar component was completely decomposed. The gas generation ratio also improved, and 50 [wt%] of the components became gas.
【００１９】水素と一酸化炭素生成量を図３に示す。水
素と一酸化炭素の生成量が上昇し、それぞれ６７２［Ｎ
ｍ３ ／ｋｇ］、３３６［Ｎｍ３ ／ｋｇ］生成した。
また、メタンもほとんど生成せず、その生成量はわずか
３８．７［Ｎｍ３ ／ｋｇ］であった。FIG. 3 shows the amounts of hydrogen and carbon monoxide produced. The production amounts of hydrogen and carbon monoxide increase, and 672 [N
m 3 / kg] and 336 [Nm 3 / kg].
Further, almost no methane was produced, and the produced amount was only 38.7 [Nm 3 / kg].
【００２０】（比較例２）原料を、灰分＝７．５、揮発
分＝２０．９、固定炭素＝７０．４（揮発分／固定炭素
＝０．３）の石炭に代え、第１段熱分解炉(1) の熱分解
温度を５００℃とし、第２段熱分解炉(2) の熱分解温度
１２００℃とした以外、実施例１と同様にして、ガスと
タールの生成割合を測定した。この結果、タール分は完
全には分解せず、３［ｗｔ％］残った。また、すすが１
５［ｗｔ％］と大量に生成した。ガス生成割合も２３
［ｗｔ％］と低く、目的とするガス回収ができなかっ
た。(Comparative Example 2) The raw material was replaced with coal having an ash content of 7.5, a volatile content of 20.9, and a fixed carbon of 70.4 (volatile matter / fixed carbon = 0.3), and the first stage heat was used. The gas and tar production ratio was measured in the same manner as in Example 1 except that the pyrolysis temperature of the cracking furnace (1) was set to 500 ° C. and the pyrolysis temperature of the second-stage pyrolysis furnace (2) was set to 1200 ° C. . As a result, the tar content was not completely decomposed, and 3 [wt%] remained. In addition, soot 1
A large amount of 5 [wt%] was produced. Gas generation ratio is also 23
[Wt%], the target gas could not be recovered.
【００２１】以上のように、揮発分率の比較的高い原料
を用い、２段階で熱分解することで、１段目の熱分解で
生成した水とタール分が２段目において下記のように見
掛け上反応し、効率よく水素と一酸化炭素が得られるこ
とが判る。As described above, by using a raw material having a relatively high volatile content and performing pyrolysis in two stages, the water and tar generated in the first stage of pyrolysis can be converted into the following in the second stage: It can be seen that they react apparently and hydrogen and carbon monoxide can be obtained efficiently.
【００２２】 Ｃ１０Ｈ１４ ＋ １０Ｈ２ Ｏ → １０ＣＯ ＋ １７Ｈ２ （１３８） １０（１８） *) （ ）内は分子量。C 10 H 14 + 10H 2 O → 10CO + 17H 2 (138) 10 (18) *) () indicates the molecular weight.
【００２３】[0023]
【００２４】上記式中、Ｃ１０Ｈ１４は、回収したター
ル分をＴＧ−ＧＣ／ＭＳで分析することによって求めた
タール分の平均分子式である。[0024] In the above formula, C 10 H 14 is collected tar is the average molecular formula of tar obtained by analyzing with TG-GC / MS.
【００２５】上記式を見ると、タール分と水は見掛け上
１：１０［ｍｏｌ］で反応し、質量日は１３８：１８０
＝１：１．３となる為、熱分解でタール分と水がほぼ当
量生成する原料からは、酸素と水蒸気を加えることなく
反応が進行し、高効率で水素と一酸化炭素が生成するも
のと思われる。According to the above formula, the tar component and water apparently react at 1:10 [mol], and the mass day is 138: 180.
= 1: 1.3, the reaction proceeds without the addition of oxygen and water vapor from the raw material that produces tar and water in equivalent amounts by thermal decomposition, and hydrogen and carbon monoxide are generated with high efficiency I think that the.
【００２６】[0026]
【表１】 [Table 1]
【００２７】[0027]
【表２】 [Table 2]
【００２８】[0028]
【表３】 [Table 3]
【００２９】[0029]
【００３０】[0030]
【発明の効果】従来技術では、熱分解の際、酸素と水蒸
気を一定割合で投入する必要があり、また、酸素と水蒸
気を投入する為、得られるガス中には二酸化炭素混入な
どの問題もあった。According to the prior art, it is necessary to supply oxygen and water vapor at a constant rate during thermal decomposition, and since oxygen and water vapor are supplied, there is also a problem that carbon dioxide is mixed in the obtained gas. there were.
【００３１】本発明方法によれば、揮発分率の高い原料
を選択的に用い、所定の温度範囲で低酸素濃度雰囲気条
件下で熱分解反応を行うので、１段目の熱分解で発生し
た水とタール分を効率的に２段目の熱分解で反応させる
ことができ、高純度の水素と一酸化炭素を効率的に得る
ことができる。According to the method of the present invention, the raw material having a high volatile content is selectively used, and the pyrolysis reaction is carried out in a predetermined temperature range under a low oxygen concentration atmosphere. Water and tar can be efficiently reacted in the second-stage thermal decomposition, and high-purity hydrogen and carbon monoxide can be efficiently obtained.
【００３２】こうして、本発明方法によれば、熱分解で
発生するタール分がなく、熱分解で得られるガス中の水
素／一酸化炭素＝０．８〜３（体積比）、低位発熱量＞
１，５００ｋｃａｌ／Ｎｍ３ で、収率５０ｗｔ％以上
で水素と一酸化炭素ガスを回収することができる。Thus, according to the method of the present invention, there is no tar component generated by thermal decomposition, hydrogen / carbon monoxide in the gas obtained by thermal decomposition = 0.8 to 3 (volume ratio), lower calorific value>
At 1,500 kcal / Nm 3 , hydrogen and carbon monoxide gas can be recovered with a yield of 50 wt% or more.
【図１】ＲＤＦの熱分解生成物収支を示す温度と生成割
合の関係のグラフである。FIG. 1 is a graph showing the balance between the temperature and the production ratio showing the balance of the pyrolysis products of RDF.
【図２】ガスとタール生成割合を示す温度と生成割合の
関係のグラフである。FIG. 2 is a graph showing a relationship between a temperature and a production ratio indicating a gas and a tar production ratio.
【図３】ガス生成割合を示す温度と生成割合の関係のグ
ラフである。FIG. 3 is a graph showing a relationship between a temperature indicating a gas generation ratio and a generation ratio.
【図４】本発明方法の実施例を示すフローシートであ
る。FIG. 4 is a flow sheet showing an embodiment of the method of the present invention.
(1) ：第１段熱分解炉 (2) ：第２段熱分解炉 (3) 〜(5) ：温度制御ヒータ (6) ：ガスクロマトグラフ分析計 (7) ：真空ポンプ (8) ：ＲＤＦ投入フィーダー (1): First stage pyrolysis furnace (2): Second stage pyrolysis furnace (3) to (5): Temperature controlled heater (6): Gas chromatograph analyzer (7): Vacuum pump (8): RDF Input feeder
───────────────────────────────────────────────────── フロントページの続き (72)発明者 岸田 央範 大阪市住之江区南港北１丁目７番89号 日 立造船株式会社内 (72)発明者 荻野 悦生 大阪市住之江区南港北１丁目７番89号 日 立造船株式会社内 Ｆターム(参考） 4D004 AA46 AA50 BA03 BA06 CA27 DA03 DA06 DA10 4G040 BA02 BB01 BB02 BB03 ──────────────────────────────────────────────────続 き Continuing on the front page (72) Inventor Hironori Kishida 1-7-89, Minami Kohoku, Suminoe-ku, Osaka-shi Inside Tachibashi Shipbuilding Co., Ltd. No. 89 Date Tate Shipbuilding Co., Ltd. F-term (reference) 4D004 AA46 AA50 BA03 BA06 CA27 DA03 DA06 DA10 4G040 BA02 BB01 BB02 BB03
Claims (2)
燃性廃棄物を酸素濃度３ｖｏｌ％以下の低酸素濃度雰囲
気下で温度４００〜１，０００℃で１次熱分解した後、
酸素濃度３ｖｏｌ％以下の低酸素濃度雰囲気下で温度
１，０００〜１，５００℃で２次熱分解することを特徴
とする、可燃性廃棄物からの水素と一酸化炭素の製造方
法。Claims 1. After a primary pyrolysis of a combustible waste having a (volatile matter) / (fixed carbon) ratio of 1 or more at a temperature of 400 to 1,000 ° C in a low oxygen concentration atmosphere having an oxygen concentration of 3 vol% or less,
A method for producing hydrogen and carbon monoxide from combustible waste, comprising performing secondary pyrolysis at a temperature of 1,000 to 1,500 ° C. in a low oxygen concentration atmosphere having an oxygen concentration of 3 vol% or less.
の低酸素濃度雰囲気下で温度４００〜１，０００℃での
１次熱分解により、（水）／（タール分）比＝０．５〜
１．５の割合で水とタール分を生成するものである、請
求項１記載の可燃性廃棄物からの水素と一酸化炭素の製
造方法。2. The waste is subjected to primary thermal decomposition at a temperature of 400 to 1,000 ° C. in a low oxygen concentration atmosphere having an oxygen concentration of 3 vol% or less, whereby a (water) / (tar content) ratio = 0.5 ~
The method for producing hydrogen and carbon monoxide from combustible waste according to claim 1, wherein water and tar are generated at a ratio of 1.5.
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Cited By (1)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| KR20030025314A (en) * | 2001-09-20 | 2003-03-29 | 김현영 | Method of gasifying carbonaceous material and apparatus therefor |
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2000
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Cited By (1)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| KR20030025314A (en) * | 2001-09-20 | 2003-03-29 | 김현영 | Method of gasifying carbonaceous material and apparatus therefor |
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