JPH02153801A - Production of hydrogen-containing gas - Google Patents
Production of hydrogen-containing gasInfo
- Publication number
- JPH02153801A JPH02153801A JP63304053A JP30405388A JPH02153801A JP H02153801 A JPH02153801 A JP H02153801A JP 63304053 A JP63304053 A JP 63304053A JP 30405388 A JP30405388 A JP 30405388A JP H02153801 A JPH02153801 A JP H02153801A
- Authority
- JP
- Japan
- Prior art keywords
- hydrogen
- concentration
- containing gas
- gas
- catalyst
- 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.)
- Pending
Links
- 239000007789 gas Substances 0.000 title claims abstract description 45
- 229910052739 hydrogen Inorganic materials 0.000 title claims abstract description 27
- 239000001257 hydrogen Substances 0.000 title claims abstract description 26
- UFHFLCQGNIYNRP-UHFFFAOYSA-N Hydrogen Chemical compound [H][H] UFHFLCQGNIYNRP-UHFFFAOYSA-N 0.000 title claims abstract description 25
- 238000004519 manufacturing process Methods 0.000 title claims description 5
- 239000003054 catalyst Substances 0.000 claims abstract description 21
- 238000006243 chemical reaction Methods 0.000 claims abstract description 19
- 229910002091 carbon monoxide Inorganic materials 0.000 claims abstract description 10
- 239000010931 gold Substances 0.000 claims abstract description 10
- 229910052760 oxygen Inorganic materials 0.000 claims abstract description 10
- 229910052737 gold Inorganic materials 0.000 claims abstract description 8
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 claims abstract description 7
- PCHJSUWPFVWCPO-UHFFFAOYSA-N gold Chemical compound [Au] PCHJSUWPFVWCPO-UHFFFAOYSA-N 0.000 claims abstract description 7
- 239000001301 oxygen Substances 0.000 claims abstract description 7
- 238000000034 method Methods 0.000 claims description 9
- UGFAIRIUMAVXCW-UHFFFAOYSA-N Carbon monoxide Chemical compound [O+]#[C-] UGFAIRIUMAVXCW-UHFFFAOYSA-N 0.000 claims description 7
- 239000007864 aqueous solution Substances 0.000 abstract description 5
- 239000002253 acid Substances 0.000 abstract description 3
- PNEYBMLMFCGWSK-UHFFFAOYSA-N aluminium oxide Inorganic materials [O-2].[O-2].[O-2].[Al+3].[Al+3] PNEYBMLMFCGWSK-UHFFFAOYSA-N 0.000 abstract description 2
- JEIPFZHSYJVQDO-UHFFFAOYSA-N iron(III) oxide Inorganic materials O=[Fe]O[Fe]=O JEIPFZHSYJVQDO-UHFFFAOYSA-N 0.000 abstract description 2
- 229910052593 corundum Inorganic materials 0.000 abstract 1
- 229910001845 yogo sapphire Inorganic materials 0.000 abstract 1
- VNWKTOKETHGBQD-UHFFFAOYSA-N methane Chemical compound C VNWKTOKETHGBQD-UHFFFAOYSA-N 0.000 description 11
- OKKJLVBELUTLKV-UHFFFAOYSA-N Methanol Chemical compound OC OKKJLVBELUTLKV-UHFFFAOYSA-N 0.000 description 9
- CURLTUGMZLYLDI-UHFFFAOYSA-N Carbon dioxide Chemical compound O=C=O CURLTUGMZLYLDI-UHFFFAOYSA-N 0.000 description 4
- 230000000052 comparative effect Effects 0.000 description 4
- 230000000694 effects Effects 0.000 description 3
- XEEYBQQBJWHFJM-UHFFFAOYSA-N iron Substances [Fe] XEEYBQQBJWHFJM-UHFFFAOYSA-N 0.000 description 3
- 239000003345 natural gas Substances 0.000 description 3
- 238000007254 oxidation reaction Methods 0.000 description 3
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 3
- UQSXHKLRYXJYBZ-UHFFFAOYSA-N Iron oxide Chemical compound [Fe]=O UQSXHKLRYXJYBZ-UHFFFAOYSA-N 0.000 description 2
- KDLHZDBZIXYQEI-UHFFFAOYSA-N Palladium Chemical compound [Pd] KDLHZDBZIXYQEI-UHFFFAOYSA-N 0.000 description 2
- 229910002092 carbon dioxide Inorganic materials 0.000 description 2
- 239000001569 carbon dioxide Substances 0.000 description 2
- 238000011156 evaluation Methods 0.000 description 2
- FDWREHZXQUYJFJ-UHFFFAOYSA-M gold monochloride Chemical compound [Cl-].[Au+] FDWREHZXQUYJFJ-UHFFFAOYSA-M 0.000 description 2
- MVFCKEFYUDZOCX-UHFFFAOYSA-N iron(2+);dinitrate Chemical compound [Fe+2].[O-][N+]([O-])=O.[O-][N+]([O-])=O MVFCKEFYUDZOCX-UHFFFAOYSA-N 0.000 description 2
- 239000000203 mixture Substances 0.000 description 2
- BASFCYQUMIYNBI-UHFFFAOYSA-N platinum Chemical compound [Pt] BASFCYQUMIYNBI-UHFFFAOYSA-N 0.000 description 2
- 238000000629 steam reforming Methods 0.000 description 2
- 239000012670 alkaline solution Substances 0.000 description 1
- 238000000975 co-precipitation Methods 0.000 description 1
- 239000003245 coal Substances 0.000 description 1
- 239000010779 crude oil Substances 0.000 description 1
- 238000002309 gasification Methods 0.000 description 1
- 150000002431 hydrogen Chemical class 0.000 description 1
- 238000005470 impregnation Methods 0.000 description 1
- 229910052742 iron Inorganic materials 0.000 description 1
- 230000003472 neutralizing effect Effects 0.000 description 1
- 230000003647 oxidation Effects 0.000 description 1
- 229910052763 palladium Inorganic materials 0.000 description 1
- 229910052697 platinum Inorganic materials 0.000 description 1
- 238000002407 reforming Methods 0.000 description 1
- 238000006057 reforming reaction Methods 0.000 description 1
- 239000000243 solution Substances 0.000 description 1
Abstract
Description
【発明の詳細な説明】
〔産業上の利用分野〕
本発明は一酸化炭素の濃度が高り水素含有ガスから一酸
化炭素の濃度が低い水素含有ガスを製造する方法に関す
るものである。DETAILED DESCRIPTION OF THE INVENTION [Industrial Application Field] The present invention relates to a method for producing a hydrogen-containing gas having a low carbon monoxide concentration from a hydrogen-containing gas having a high carbon monoxide concentration.
水素含有ガスを製造する方法としては、原油、石炭など
のガス化の他、天然カス（メタンが主成分）の水蒸気改
質又はメタノールの改質などの反応が利用されるが、熱
力学の平衡上の制約から、生成ガス中に一酸化炭２８度
は１％〜５０俤と高くなる。例えば、メタノールの改質
反応の場合、次のような反応式で表わされる。Methods for producing hydrogen-containing gas include gasification of crude oil, coal, etc., as well as reactions such as steam reforming of natural gas (methane is the main component) or reforming of methanol. Due to the above constraints, the amount of carbon monoxide at 28 degrees Celsius in the generated gas is as high as 1% to 50 degrees. For example, in the case of methanol reforming reaction, it is expressed by the following reaction formula.
ＣＨ１０Ｈ＋ （ｎ＋ｍ ）Ｈ２０→（２＋ｎ ）Ｈ２
＋ （１−ｎ ）ＧＯ＋ｎＣ０１＋ｍＨ１０こ＼で０
（ｎ （言
ｍｈ。CH10H+ (n+m)H20→(2+n)H2
+ (1-n)GO+nC01+mH10 this\0
(n (word mh.
水素含有ガスを大量に製造する場合、一般に天然ガスの
水蒸気改質反応が用いられている。When producing a large amount of hydrogen-containing gas, a steam reforming reaction of natural gas is generally used.
生成ガス中の一酸化炭素（以下、ＣＯと略記する〕濃度
は、反応圧力、温度及び水蒸気／天然ガスのモル比など
の反応条件で決定される平衡ガス組成になり、通常水蒸
気改質炉の出口ガスは、次のようなガス組成（ドライベ
ース、モル％）Ｋなる。The concentration of carbon monoxide (hereinafter abbreviated as CO) in the produced gas is the equilibrium gas composition determined by reaction conditions such as reaction pressure, temperature, and steam/natural gas molar ratio. The outlet gas has the following gas composition (dry basis, mol %) K.
Ｈ，：１１〜８０％、Ｃｏ：１０〜３０％、Ｃｏ、：１
０〜５０％。H: 11-80%, Co: 10-30%, Co: 1
0-50%.
ＣＨ４： １〜Ｉ Ｏ’ｌｋ
上記ガスのＣＯ濃度を低下する方法としては、Ｃｏ シ
フト反応（ＣＯ＋Ｈ，Ｏ−＋ＣＯ鵞＋Ｈ雪）を利用し、
Ｃｏシフト触媒（Ｆｅ系又はＣｕ系）上で２００〜５０
０℃の温度範囲で行われるが、工業的に行われている条
件下では、ＣＯｇ度Ｆｉｔｓ前後であり、さらにＣＯ６
度を下ける丸めには炭酸ガスを除去した後、メタネーシ
ョン（ＣＯ＋５Ｈ。CH4: 1~I O'lk As a method to reduce the CO concentration of the above gas, use the Co shift reaction (CO + H, O - + CO + H snow),
200-50 on Co shift catalyst (Fe-based or Cu-based)
It is carried out in a temperature range of 0°C, but under industrial conditions, the COg degree is around Fits, and further CO6
To lower the degree, after removing carbon dioxide gas, methanation (CO + 5H) is used.
→ＣＨ４＋Ｈ，Ｏ） を利用し、Ｎｉ系触媒上で５５
（１〜５５０℃の温度範囲で行われる。→CH4+H,O) on Ni-based catalyst.
(Conducted at a temperature range of 1 to 550°C.
しかし、上記方法は反応温度が高いという欠点があるほ
か、ＣＯシフト反応の場合、スチームが多ｔｃ６！？要
になる点ま九メタネーション反応の場合、共存する炭酸
ガスをあらかじめ除去した後、昇温させて反応させる必
要がある点などの問題点がある。However, the above method has the disadvantage that the reaction temperature is high, and in the case of the CO shift reaction, a large amount of steam is generated. ? Key points 9. In the case of the methanation reaction, there are problems such as the need to remove coexisting carbon dioxide gas beforehand and then raise the temperature to carry out the reaction.
前述した方法以外でＣｏＩＩｌｌ度を低減させる方法と
しては、ＣＯを酸化させてＣｏ、にする方法が考えられ
るが、既存の酸化触媒（白金又はパラジウムを含有する
触媒）を用いた場合、水素の方が燃焼速度が速（、Ｃｏ
９度はあまり低くならないという問題がある。A possible method for reducing the CoIIll degree other than the method described above is to oxidize CO to Co, but when using existing oxidation catalysts (catalysts containing platinum or palladium), hydrogen has a fast burning rate (, Co
The problem is that 9 degrees doesn't get very low.
本発明者らは上記の問題点を解決すべく、鋭意実験検討
を重ねた結果、ＣＯ濃度が高い水素含有ガスに空気など
の酸素含有ガスを混合したガスを適当な反応温度で金を
含有する触媒と接触させることくより水素の酸化反応を
抑制し、ＣＯ酸化反応を極めて選択性よく進行させ得る
ことを見出し、本発明を完成させるに至った。In order to solve the above-mentioned problems, the present inventors conducted intensive experimental studies and found that a hydrogen-containing gas with a high CO concentration and an oxygen-containing gas such as air were mixed with gold at an appropriate reaction temperature. The present inventors have discovered that it is possible to suppress the hydrogen oxidation reaction and allow the CO oxidation reaction to proceed with extremely high selectivity without bringing it into contact with a catalyst, and have completed the present invention.
すなわち、発明ＢＡは、ＣＯ濃度が１優（モル悌、以下
チはモル饅である）以下の水素含有ガスを製造する方法
において、ＣＯ濃度が高い水素官有ガスに酸素含有ガス
を混合したガスを、反応温度２００℃以下で金を含有す
る触媒と接触させることを特徴とする水素含有ガスの製
造方法である。That is, the invention BA is a method for producing a hydrogen-containing gas with a CO concentration of 1 mole or less (hereinafter referred to as mole), which is a gas in which a hydrogen-containing gas with a high CO concentration is mixed with an oxygen-containing gas. is brought into contact with a catalyst containing gold at a reaction temperature of 200° C. or less.
本発明でいうＣａ２度が高い水素含有ガスとは、水素濃
度が少なくとも１０係以上でかつ、ＣＯ濃度が少なくと
も１０１％以上のガスを指し、例えばメタノール改質後
のガスなどがある。In the present invention, the hydrogen-containing gas having a high Ca2 degree refers to a gas having a hydrogen concentration of at least 10% or higher and a CO concentration of at least 101% or higher, such as a gas after methanol reformation.
また、本発明でいう酸素含有ガスとは酸素濃度が少なく
とも（ＬＩＪ以上のガスを指し、例えば空気などである
。Further, the oxygen-containing gas in the present invention refers to a gas having an oxygen concentration of at least LIJ or higher, such as air.
なお、本発明における好ましい反応条件は次の通りであ
る。In addition, preferable reaction conditions in the present invention are as follows.
反応温度＝２００℃以下、特に好ましくｈａ〜 １００
℃
ＧＨ８Ｖ ： １０〜１０１ｈ−１、％に好ましくは
１０１〜１０４ ｈ−１
混合ガス中の０２ ／ Ｃｏモル比 ＝Ｉ１５〜５、特
に好ましくは１〜３
亥た、本発明でいう金を含有する触媒とは、金を１１〜
５０重ｔｓ％特に好ましくは１〜１０重童慢含有する触
媒を指す。全以外の成分としてはＦｅ！０３． ｃｏｏ
、 Ｎｉｐ、 Ａ４０３． Ｔｉ０１ 、 ＺｒＯ＊ｓ
８１０ｘからなる群の一種以上の酸化物が用いられる
。Reaction temperature = 200°C or less, particularly preferably ha~100
°C GH8V: 10 to 101 h-1, preferably 101 to 104 h-1 02/Co molar ratio in mixed gas = I15 to 5, particularly preferably 1 to 3 Contains gold as referred to in the present invention Catalyst means gold from 11 to
It refers to a catalyst containing 50% by weight, particularly preferably 1 to 10% by weight. The other components are Fe! 03. coo
, Nip, A403. Ti01, ZrO*s
One or more oxides from the group consisting of 810x are used.
触媒の調製方法としては次のような方法がある。There are the following methods for preparing the catalyst.
（１） 含浸方法：例えｌｌ１Ｆｅ、Ｏ，又は＊２＝
０＝ などの担体を塩化金酸の水溶液に浸漬し、乾燥後
焼成する。(1) Impregnation method: For example, ll1Fe, O, or *2=
A carrier such as 0= is immersed in an aqueous solution of chloroauric acid, dried, and then fired.
（２） 共沈方法：例えば硝酸鉄と塩化金ａ２を含む
水溶液をアルカリ水溶液で中和して生成する共沈物を水
洗・乾燥後焼成する。(2) Co-precipitation method: For example, a coprecipitate produced by neutralizing an aqueous solution containing iron nitrate and gold chloride a2 with an alkaline aqueous solution is washed with water, dried, and then fired.
以下、実施例によｐ本発明を具体的に説明する。Hereinafter, the present invention will be specifically explained with reference to Examples.
〔実施例１〕
所定濃度の硝酸鉄と塩化金ｒＲ′ｆｒ：含む水溶液を所
定の比率（ＡｕとＦｅ（Ｆ）原子比＝５：９５）で混合
し九ｇ、をアルカリ水溶液で中和して生成する共沈物を
水洗・乾燥後、４００℃で焼成して触媒１を調製した。[Example 1] An aqueous solution containing a predetermined concentration of iron nitrate and gold chloride rR'fr was mixed at a predetermined ratio (atomic ratio of Au and Fe (F) = 5:95), and 9 g was neutralized with an aqueous alkaline solution. The resulting coprecipitate was washed with water, dried, and then calcined at 400°C to prepare catalyst 1.
樅ＩＫ示す条件で活性評価試験を行い表２の結果を得た
。An activity evaluation test was conducted under the conditions shown in Fir IK, and the results shown in Table 2 were obtained.
表 １
水素含有ガス（Ｈａ ： ７２９６％Ｃｏ ： １．５
％、ＣＯＩ：２５％、ＣＨ４： １．５％ ） ： ６
０〜１８０ Ｎｌ／ ｈ空気＝５〜１５ Ｎｔ／ｈ
触媒：１００ｃｃ
反応温度： ０〜ｇＯ℃ （比較例 ２５０１１：）
表 ２
以上のように比較例（反応温度：２５０℃）では、出口
ガス中のＣｏ濃度（入口混合ガス中のＣｏ濃度１．５４
％）は、１％を越えるのに対し、本発明の実施例では１
％以下となっている。Table 1 Hydrogen-containing gas (Ha: 7296%Co: 1.5
%, COI: 25%, CH4: 1.5%): 6
0-180 Nl/h Air = 5-15 Nt/h Catalyst: 100cc Reaction temperature: 0-gO℃ (Comparative example 25011:)
Table 2 As shown above, in the comparative example (reaction temperature: 250°C), the Co concentration in the outlet gas (Co concentration in the inlet mixed gas was 1.54
%) exceeds 1%, whereas in the embodiment of the present invention it exceeds 1%.
% or less.
なお、Ｒｕｎ ２の反応条件で１０００時間連続試験を
行ったが、出口ガス中のＣｏｆｌｌ度は安定していた。Although a continuous test was conducted for 1000 hours under the reaction conditions of Run 2, the degree of Coflu in the outlet gas was stable.
〔実施例２〕
酸化鉄（α−Ｆｅ２０３ ）及びアルミナを各々所定濃
度の塩化金酸水浴液に浸漬し、乾燥後４００℃で焼成を
行い触媒２ （Ａｕ／Ｆｅ１０３．全Ｘｔ中のＡｕ５重
量襲）、触媒５ （Ａｕ／Ａ４０ｓ Ｉ全憲童中のＡｕ
１重ｉｔ％）をそれぞれａｔａ＋製した。[Example 2] Iron oxide (α-Fe203) and alumina were each immersed in a chloroauric acid water bath solution with a predetermined concentration, dried, and then calcined at 400°C to prepare catalyst 2 (Au/Fe103. ), catalyst 5 (Au/A40s I
1 weight it%) were each made from ata+.
表５に示す条件で活性評価試＠を行い、表４の結果を得
た。An activity evaluation test @ was conducted under the conditions shown in Table 5, and the results shown in Table 4 were obtained.
なお、比較触媒としてＡｔ、Ｏ，担体にｐｔ’ｌ＋重ｆ
％担持し次触媒についても同様の試験を行った。In addition, as a comparative catalyst, At, O, pt'l + heavy f on the carrier
A similar test was conducted for the catalyst with % loading.
表 ３
水素含有ガス（Ｈ鵞：５０％、ＣＯ：２％、Ｎ！：４Ｂ
％）：５ＯＮ ｔ／ ｈ
空気：１ＯＮｔ／ｈ
触媒： ２０ｃｃ、 反応温度＝ ９０℃表 ４
以上のように比較触媒（ｐｔ系）ではＣｏ濃度はめまり
低下しない。Table 3 Hydrogen-containing gas (H: 50%, CO: 2%, N!: 4B
%): 5 ON t/h Air: 1 ON t/h Catalyst: 20 cc, Reaction temperature = 90°C Table 4 As described above, with the comparative catalyst (PT type), the Co concentration does not decrease.
以上の実施例からも明らかなように、本発明を用いるこ
とにより、一酸化炭素の濃度が高い水素含有ガスから、
Ｃｏ濃度が１％以下の水素含有ガスを製造することがで
きる。As is clear from the above examples, by using the present invention, hydrogen-containing gas with a high concentration of carbon monoxide can be
A hydrogen-containing gas with a Co concentration of 1% or less can be produced.
Claims (1)
方法において、一酸化炭素の濃度が高い水素含有ガスに
酸素含有ガスを混合したガスを、反応温度２００℃以下
で金を含有する触媒と接触させることを特徴とする水素
含有ガスの製造方法。In a method for producing a hydrogen-containing gas with a carbon monoxide concentration of 1% or less, a hydrogen-containing gas with a high carbon monoxide concentration mixed with an oxygen-containing gas is mixed with a gold-containing catalyst at a reaction temperature of 200°C or less. A method for producing a hydrogen-containing gas, the method comprising bringing it into contact with a hydrogen-containing gas.
Priority Applications (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP63304053A JPH02153801A (en) | 1988-12-02 | 1988-12-02 | Production of hydrogen-containing gas |
Applications Claiming Priority (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP63304053A JPH02153801A (en) | 1988-12-02 | 1988-12-02 | Production of hydrogen-containing gas |
Publications (1)
| Publication Number | Publication Date |
|---|---|
| JPH02153801A true JPH02153801A (en) | 1990-06-13 |
Family
ID=17928475
Family Applications (1)
| Application Number | Title | Priority Date | Filing Date |
|---|---|---|---|
| JP63304053A Pending JPH02153801A (en) | 1988-12-02 | 1988-12-02 | Production of hydrogen-containing gas |
Country Status (1)
| Country | Link |
|---|---|
| JP (1) | JPH02153801A (en) |
Cited By (2)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| KR100440907B1 (en) * | 2001-11-29 | 2004-07-21 | (주)에너피아 | Process for Selectively Removing Carbon Monoxide Contained in Hydrogen-enriched Reformate Gas Using Natural Manganese Ore |
| JP2009046388A (en) * | 1998-10-12 | 2009-03-05 | Toyota Motor Corp | Carbon monoxide removing device |
-
1988
- 1988-12-02 JP JP63304053A patent/JPH02153801A/en active Pending
Cited By (2)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| JP2009046388A (en) * | 1998-10-12 | 2009-03-05 | Toyota Motor Corp | Carbon monoxide removing device |
| KR100440907B1 (en) * | 2001-11-29 | 2004-07-21 | (주)에너피아 | Process for Selectively Removing Carbon Monoxide Contained in Hydrogen-enriched Reformate Gas Using Natural Manganese Ore |
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