KR960005505B1 - Apparatus and process for producing hydrogen - Google Patents

Apparatus and process for producing hydrogen Download PDF

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KR960005505B1
KR960005505B1 KR1019880002136A KR880002136A KR960005505B1 KR 960005505 B1 KR960005505 B1 KR 960005505B1 KR 1019880002136 A KR1019880002136 A KR 1019880002136A KR 880002136 A KR880002136 A KR 880002136A KR 960005505 B1 KR960005505 B1 KR 960005505B1
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outlet means
catalyst
tubes
inlet
convection
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KR880011009A (en
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디데리쿠스 데 그라프 요하네스
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셀 인터나쵸 나아레 레사아츠 마아츠샤피 비이부이
오노 알버어스
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    • C01B2203/0205—Processes for making hydrogen or synthesis gas containing a reforming step
    • C01B2203/0227—Processes for making hydrogen or synthesis gas containing a reforming step containing a catalytic reforming step
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    • C01B2203/0805—Methods of heating the process for making hydrogen or synthesis gas
    • C01B2203/0833—Heating by indirect heat exchange with hot fluids, other than combustion gases, product gases or non-combustive exothermic reaction product gases
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    • C01B2203/0844—Methods of heating the process for making hydrogen or synthesis gas by heat exchange with exothermic reactions, other than by combustion of fuel the non-combustive exothermic reaction being another reforming reaction as defined in groups C01B2203/02 - C01B2203/0294
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Abstract

내용 없음.No content.

Description

수소 제조 장치 및 방법Hydrogen Production Apparatus and Method

제1도는 본 발명에 따른 장치의 종단면도이다.1 is a longitudinal sectional view of the device according to the invention.

제2도는 제1도에 도시한 장치의 AA' 횡단면도이다.FIG. 2 is a cross-sectional view AA ′ of the apparatus shown in FIG. 1.

제3도는 제1도에 도시한 장치에 대해, 부가의 열교환 수단을 포함하는 장치의 종단면도이다.FIG. 3 is a longitudinal sectional view of the apparatus including additional heat exchange means for the apparatus shown in FIG.

* 도면의 주요부분에 대한 부호의 설명* Explanation of symbols for main parts of the drawings

1 : 하우징 2 : 대류부1 housing 2 convection part

5 : 분배부 8 : 촉매용기5: Distribution unit 8: Catalyst container

9 : 개방단부튜브 10 : 튜브판9: open end tube 10: tube plate

본 발명은 수소제조에 적당한 장치와, 수소함유 기체를 제조하기 위한 방법에 관한 것이다. 적절한 반응온도를 유지하는데 필요한 열을 재생하기 위해 연도 기체와 생성기체 사이에 열을 교환되는 장치에서 탄화수소류 공급물을 흡열성 증기로 리포밍(feforming)하므로써 합성기체(주로, 수소와 일산화탄소로 구성되고, 추가로 이산화탄소, 질소, 전환되지 않은 탄화수소 및 증기로 구성됨)와 같은 수소함유 기체를 제조하는 것은 널리 공지되어 있다. 그러나, 보통 매우 흡열적인 반응이 수행되는 반응부에서와 같이 열이 가장 많이 필요로 하는 장치에서는 재생되지 않는다.The present invention relates to a device suitable for producing hydrogen and a method for producing a hydrogen containing gas. Synthetic gas (mainly composed of hydrogen and carbon monoxide) by reforming hydrocarbon feeds into endothermic vapors in a device where heat is exchanged between flue gas and product gas to recover the heat required to maintain the appropriate reaction temperature. And additionally producing hydrogen-containing gases such as carbon dioxide, nitrogen, unconverted hydrocarbons and steam. However, it is not usually regenerated in devices that require the most heat, such as in the reaction zone where very endothermic reactions are performed.

촉매입자를 포함한 환형공간을 형성하는 두개의 동심 튜브들로 이루어진 반응부를 사용하여 중앙튜브를 통해 생성기체를 재기하고 따라서 뜨거운 생성 기체와 촉매 사이에 열을 직접 교환함으로써 반응구역으로 부터 생기는 생성기체의 열함량을 이용하는 것도 공지되어 있다.The reaction part consisting of two concentric tubes forming an annular space containing catalyst particles is used to recover the product gas through the central tube and thus to directly exchange heat between the hot product gas and the catalyst, thereby producing the gas generated from the reaction zone. It is also known to use heat content.

동심 튜브들로 이루어진 반응부들 사용하는 것과 관련된 주요한 문제는, 그것으로 얻어질 수 있는 열교환 정도, 특히 800℃ 또는 심지어 1000℃ 온도의 생성기체가 냉각되어질 때의 열교환정도이다.The main problem associated with the use of reaction sections consisting of concentric tubes is the degree of heat exchange that can be obtained, especially when the product gas at 800 ° C or even 1000 ° C is cooled.

뜻밖에도, 촉매용기에는 배열되고 나선형으로 감긴 튜브들은 상기 튜브들을 경유하여 제기된 뜨거운 생성기체와 대류열교환에 의해 더욱 가열된 주변촉매 입자들 사이에 우수한 열전달을 한다는 것이 밝혀졌다.Unexpectedly, it has been found that the tubes arranged and spirally wound in the catalyst vessel have good heat transfer between the hot product gas raised via the tubes and the peripheral catalyst particles further heated by convective heat exchange.

그러므로 수소제조에 적당한 장치에 관한 본 발명은 다음을 포함한다.Therefore, the present invention relating to a device suitable for producing hydrogen includes the following.

(i) 가열매체용 입구 및 출구수단을 가지는 대류부를 포함한 하우징.(i) a housing comprising a convection portion having inlet and outlet means for the heating medium.

(ii) 프로세스 유체용 입구 및 출구수단을 가지며, 대류부속으로 인장되고 다수의 나선형으로 감겨진 개방단부 튜부들로 이루어진 촉매용기(들)로 된 반응부, 여기서 프로세스 유체 입구수단은 촉매용기(들)와 연통하고 프로세스 유체 출구수단은 튜브의 상단부와 연통한다.(ii) a reaction section having a catalyst vessel (s) having inlet and outlet means for the process fluid and which is tensioned into the convection and consists of a plurality of spirally wound open end tubs, wherein the process fluid inlet means is a catalyst vessel (s) ) And the process fluid outlet means is in communication with the upper end of the tube.

본 발명은 또한 상승온도 및 압력에서 증기 존재하의 탄화수소류 공급물을, 대류열전달에 의해 가열되는 리포밍 촉매와 접촉시키고, 이 리포밍 촉매내에 뻗은 나선형으로 감긴 튜브들을 통하여 수소함유 생성 기체를 제기하는 것을 포함하는 수소 함유기체의 제조방법에 관한 것이다.The present invention also provides a method for contacting a hydrocarbon feed in the presence of steam at elevated temperatures and pressures with a reforming catalyst heated by convective heat transfer and bringing hydrogen-containing product gas through spirally wound tubes extending within the reforming catalyst. It relates to a method for producing a hydrogen-containing gas comprising a.

이하 첨부도면을 참조하여 본 발명은 상세히 서술하면 다음과 같다.Hereinafter, the present invention will be described in detail with reference to the accompanying drawings.

제1도에 도시된 장치는 가열매체, 예컨대 뜨거운 액체나 기체, 심지어 입자 고체, 바람직하게 연소기체를 위한 입구수단(3)과 출구수단(4)을 가진 대류부(2)를 포함하는 하우징(1)으로 이루어진다.The apparatus shown in FIG. 1 comprises a housing comprising a convection part 2 having an inlet means 3 and an outlet means 4 for a heating medium, such as a hot liquid or gas, even particulate solids, preferably combustion gases. Consists of 1).

하우징(1)은 반응부를 포함하고, 이 반응부는 또한 하나 또는 그 이상의 촉매용기(8)와, 증기 및 탄화수소 함유 기체(바람직하게 천연기체 혹은 메탄)의 공급 혼합물과 같은 프로세스 유체를 위한 입구수단(6)과 수소함유 생성기체 및 비전화된 공급기체의 혼합물과 같은 프로세스 유체를 위한 출구수단(7)을 가지는 분배부(5)를 포함한다.The housing 1 comprises a reaction section, which also comprises inlet means for a process fluid, such as a feed mixture of one or more catalyst vessels 8 and vapor and hydrocarbon containing gases (preferably natural gas or methane) ( 6) and a distribution section 5 having outlet means 7 for process fluids, such as mixtures of hydrogen containing gas and non-ignited feed gas.

촉매용기들(8)은 바람직하게 관모양으로 되어있으며, 적어도 부분적으로라도 나선형으로 감겨진 여러개의 개방단부 튜브들(9)의 최소한 주요부분을 둘러싸고 있다.The catalyst vessels 8 are preferably tubular and enclose at least a major part of several open end tubes 9 which are at least partially spirally wound.

바람직하게도, 하우징(1)안에 하나의 원형(제2도에 도시됨)으로 또는 그 이상의동심원 형태로 적당히 배열된 다수의 관형 촉매용기들(8)은 대류부(2)속에서 아래로 뻗어 있다.Preferably, a plurality of tubular catalyst vessels 8 suitably arranged in a circle (shown in FIG. 2) or more concentrically in the housing 1 extend down into the convection portion 2. .

분배부(5)는 튜브판(10)에 의해 대류부(2)로 부터 바람직하게 분리되어 있어서, 출구수단(11)을 통해 나오는 생성기체가 가열기체로 오염되는 것을 방지한다. 더우기 튜브판(10)에 의해 관형 촉매용기를 매달아놈으로써, 튜브가 양끝에서 입구 또는 출구수단에 연결되었을 때 쉽사리 발생될 수 있는 튜브 또는 튜브 접속부의 파괴와 같은 문제가 일어나지 않으면서 촉매용기들은 본 발명에 따른 장치의 시동중에 자유로이 확장할 수 있다.The distribution part 5 is preferably separated from the convection part 2 by the tube plate 10, thereby preventing the generation gas coming out through the outlet means 11 from being contaminated with the heating gas. Furthermore, by suspending the tubular catalyst vessel by the tube plate 10, the catalyst vessels can be seen without problems such as destruction of the tube or tube connection, which can easily occur when the tube is connected to the inlet or outlet means at both ends. It is possible to freely expand during startup of the device according to the invention.

촉매용기를 가능한 한 균일하게 가열하기 위해서, 대류부는 예를들어 제1도 및 제3도에 도시된 내화물질을 포함하는 디스크 모양의 격리수단과 같이 방사열 전달을 방지하기 위한 수단(12)을 바람직하게 포함한다.In order to heat the catalyst vessel as uniformly as possible, the convection portion preferably comprises means 12 for preventing radiant heat transfer, such as, for example, disk-shaped isolation means comprising the refractory material shown in FIGS. Include it.

프로세스 기체는 촉매용기의 상단부에 있는 입구 구멍(13)을 통하여서만 들어갈 수 있으며, 반응부에서 2 내지 200 바아의 압력과 400 내지 1200℃의 비교적 낮은 온도로 작동될 수 있도록 바람직하게 사용되는 입자 촉매를 통하여 아래로 진행한다.The process gas can only enter through the inlet hole 13 at the upper end of the catalyst vessel and is preferably used as a particle catalyst so that it can be operated at a pressure of 2 to 200 bar and a relatively low temperature of 400 to 1200 ° C in the reaction section. Proceed down through.

바람직하게도, 촉매용기(8)의 닫힌 하단부에는 촉매지지수단(14)이 마련되어 있어, 바람직하게 각 촉매용기에 있는 두 나선형 코일튜브의 개방하단부(15)속으로 촉매입자가 전달되는 것을 막는다. 이와더불어 촉매 지지 수단(14)은 나선형 코일튜브의 상기 하단부(15)를 위한 위치지정수단으로 작용할 수 있다.Preferably, a catalyst support means 14 is provided at the closed lower end of the catalyst vessel 8, preferably preventing the transfer of catalyst particles into the open lower end 15 of the two helical coil tubes in each catalyst vessel. In addition, the catalyst support means 14 can act as a positioning means for the lower end 15 of the helical coil tube.

작동중에 뜨거운 프로세스 기체는 제1도 및 제3도에 도시한 바와같이 하단부(15)를 통해 튜브(9)로 들어가 위로 흘러서, 주변촉매와 최적열교환을 한다.During operation, the hot process gas enters the tube 9 through the lower end 15 and flows upward, as shown in FIGS. 1 and 3, for optimum heat exchange with the surrounding catalyst.

열교환된 프뤄스 기체(500-1000℃의 온도를 계속가짐)는 촉매용기(8)의 상단부(29)에서 1쌍의 나선형으로 감겨진 튜브들과 소통하는 환형 채널(16)로 들어간다환형채널들(16)은 매니포울드 튜브들(17)을 경유하여 생성기체 출구수단(7)과 개방 소통한다.The heat exchanged Pruth gas (having a temperature of 500-1000 ° C.) enters the annular channel 16 in communication with a pair of spirally wound tubes at the upper end 29 of the catalyst vessel 8. (16) is in open communication with the product gas outlet means (7) via manifold tubes (17).

상술한 방식으로 각쌍의 나선형으로 감겨진 튜브들(9)의 상단부들은 하우징(1)의 상단부 거의 중심에 위치한 프로세스 유체용 단일 출구 매니포울드(7)에 연결된다. 그러한 배열은 구조적인 관점에서는 매우 유익한데, 그 이유는 밀폐와 팽창문제와 관련해서 각 촉매튜브에 대해 다수의 개별 출구수단을 사용할 필요가 없어지고 더우기, 모든 매니포울드 튜브(17)내의 압력은 거의 같을 것이며, 따라서 모든 촉매용기들에 걸쳐 처리기체의 최적 분배가 확실해지기 때문이다.In the manner described above the upper ends of each pair of spirally wound tubes 9 are connected to a single outlet manifold 7 for process fluid which is located about the center of the upper end of the housing 1. Such an arrangement is very advantageous from a structural point of view, since it eliminates the need to use multiple separate outlet means for each catalyst tube in connection with sealing and expansion problems, and furthermore, the pressure in all manifold tubes 17 It will be about the same, so the optimum distribution of treatment gas across all catalyst vessels is assured.

제1도 및 제3도에서 도시한 대로 하우징(1)의 기저부(18)에 있는 하나 또는 그 이상의 연소기 출구수단은 가열매체용 입구수단(3)으로 기능한다. 본 발명에 따른 장치의 바람직한 실시예에서, 다수의(예컨대, 3개)연소기 출구 수단은 회전 대칭적 방식 (도시안됨)으로 하우징에 예컨대 접선적으로 배열되어 있어서 대류부(2) 곳곳에 연소 기체가 최적으로 분배되게 한다.One or more combustor outlet means at the base 18 of the housing 1 as shown in FIGS. 1 and 3 function as inlet means 3 for the heating medium. In a preferred embodiment of the device according to the invention, the plurality of (e.g. three) combustor outlet means are arranged, for example, tangentially in the housing in a rotationally symmetrical manner (not shown) so that combustion gases are scattered throughout the convection part 2 Ensure optimal distribution.

제1도 및 제3도에 도시한 연소수단은(예컨대 산소가 푸우한)공기용 입구수단(19), 가연성 유동체(예컨대 탄화수소류의 기체, 액체 및/또는 석탄)용 입구수단(20), 그리고 선택적으로 가열 압력 스윙흡착(도면에 도시안됨)에 의해 수소 및 일산화탄소 함유 생성 기체로 부터 분리된 일산화탄소 함유 기체와 같은 재순환된 기체, 또는 재순환된 연도기체용 입구수단(21)을 포함한다.The combustion means shown in FIG. 1 and FIG. 3 include inlet means 19 for air (e.g. saturated with oxygen), inlet means 20 for combustible fluids (e.g., gases, liquids and / or coals of hydrocarbons), And optionally recycled gas, such as carbon monoxide containing gas separated from hydrogen and carbon monoxide containing product gas by heating pressure swing adsorption (not shown in the figure), or inlet means 21 for recycled flue gas.

제3도에서, 본 발명에 따른 장치의 좀더 복잡하고 좀더 효율적인 실시예가 도시되어 있으며, 여기서 출구수단(7)은 하우징(1)밖으로 연장된 열교환 유체(예컨대 비교적 냉각 팽창된 연도 기체 및/또는 열교환된 연도기체)용 입구수단(23) 및 출구수단(21)과 개방 소통하는 적어도 하나의 환형 공간(22)을 형성하는, 다수의 동심 배열 튜브를 포함한다.In FIG. 3, a more complex and more efficient embodiment of the device according to the invention is shown, wherein the outlet means 7 comprise a heat exchange fluid (eg a relatively cold expanded flue gas and / or heat exchanger extending out of the housing 1). A plurality of concentric array tubes, forming at least one annular space 22 in open communication with the inlet means 23 and outlet means 21 for the flue gas.

생성기체 출구수단(7)은 튜브판(10)을 통하여 대류부(2)속으로 연장한 관형 하우징(24)을 포함한다. 하우징(24)의 닫힌 하단부(25)는, 바람직하게 팽창 벨로우(제3도에 도시안됨)에 의해, 열교환 유체 입구수단(23)에 연결되어 있다. 매니포올드 튜브들(17)은 닫힌 하단부(28)을 가진 관형 열교환 수단(26)과 개방 소통하여, 상기 관형 수단(26)속으로 매니포울드 튜브(17)을 통하여 뻗은 개방단부 관형 출구 수단(11)안으로 환형 공간(28)을 통하여 작동중 생성기체의 하향흐름을 반전시킨다. 상기 서술한 출구수단으로, 매니포울드 튜브(17)로부터 발산하는 생성기체에 여전히 존재하는 열에너지의 상당부분이 회수될 수 있다.The product gas outlet means 7 comprise a tubular housing 24 which extends into the convection part 2 through the tube plate 10. The closed lower end 25 of the housing 24 is connected to the heat exchange fluid inlet means 23, preferably by expansion bellows (not shown in FIG. 3). Manifold tubes 17 are in open communication with tubular heat exchange means 26 having a closed lower end 28, so that open end tubular outlet means extend through the manifold tube 17 into the tubular means 26. Reverse the downward flow of the product gas during operation through the annular space 28 into (11). With the outlet means described above, a significant portion of the thermal energy still present in the product gas emanating from the manifold tube 17 can be recovered.

Claims (7)

(i) 가열매체용 입구 및 출구수단이 있는 대류부를 포함하는 하우징과 ; (ii) 프로세스 유체용 입구수단 및 출구수단이 있는 반응부로서, 대류부안으로 뻗어있고 다수의 나선형으로 감겨진 개방단부 튜브들로 이루어진 촉매용기(들)를 포함하는 반응부로 구성되는 수소 제조 장치로서, 프로세스 유체 입구수단의 촉매용기(들)와 소통하며, 프로세스 유체 출구수단이 튜브들의 상단부와 소통하는 수소 제조 장치.(i) a housing comprising a convection portion having inlet and outlet means for the heating medium; (ii) a reaction section having inlet and outlet means for a process fluid, the apparatus for producing hydrogen comprising a reaction section comprising a catalyst vessel (s) consisting of a plurality of spirally wound open end tubes extending into the convection section; And a hydrogen production apparatus in communication with the catalyst vessel (s) of the process fluid inlet means, the process fluid outlet means in communication with the upper ends of the tubes. 제1항에 있어서, 상기 대류부는 촉매용기로의 방사열 전달을 방지하기 위한 수단을 포함하는 장치.The apparatus of claim 1 wherein the convection portion comprises means for preventing radiant heat transfer to the catalyst vessel. 제1항 또는 제2항에 있어서, 대류부와 반응부가 튜브판에 의해 분리되는 장치.The device according to claim 1 or 2, wherein the convection portion and the reaction portion are separated by a tube plate. 제3항에 있어서, 다수의 관형 촉매 용기가 튜브판을 통하여 대류부로 아래로 뻗는 장치.4. The apparatus of claim 3, wherein the plurality of tubular catalyst vessels extend down into the convection through the tube plate. 제1항 또는 제2항에 있어서, 각 쌍의 나선형으로 감겨진 튜브들의 상단부는 하우징의 상단부 거의 중심에 배열된 프로세스 유체용 단일 출구수단에 연결되어 있는 장치.The device of claim 1 or 2, wherein the upper end of each pair of spirally wound tubes is connected to a single outlet means for process fluid arranged about the upper end of the housing. 제5항에 있어서, 상기 출구수단은, 하우징 밖으로 연장된 열교환 유체용 입구 및 출구수단과 소통하는 환형공간을 적어도 하나 형성하는 다수의 동심 배열 튜브들을 포함하는 장치.6. The apparatus of claim 5, wherein the outlet means comprises a plurality of concentric array tubes forming at least one annular space in communication with the inlet and outlet means for the heat exchange fluid extending out of the housing. 상승 온도와 압력에서 중기 존재하의 탄화수소류 공급물을, 대류 열전달에 의해 가열되는 리포밍(reforming) 촉매와 접촉시키는 단계와, 리포밍 촉매내에 뻗어있는 나선형으로 감겨진 튜브들을 통하여 수소함유 생성기체를 제거하는 단계를 포함하는 수소함유 기체 제조 방법.Contacting the hydrocarbon feed in the presence of medium to elevated temperature and pressure with a reforming catalyst heated by convective heat transfer, and through the spirally wound tubes extending within the reforming catalyst, Method for producing a hydrogen-containing gas comprising the step of removing.
KR1019880002136A 1987-03-03 1988-02-29 Apparatus and process for producing hydrogen KR960005505B1 (en)

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GB8704959A GB2201903B (en) 1987-03-03 1987-03-03 Apparatus and process suitable for producing hydrogen
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JP2835851B2 (en) * 1989-06-23 1998-12-14 ヤマハ発動機株式会社 Reformer for fuel cell
GB2238487A (en) * 1989-11-25 1991-06-05 Methan Limited Reforming apparatus
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IT1283877B1 (en) * 1996-01-12 1998-05-07 Kinetics Technology ISOTHERMAL CATALYTIC REACTOR FOR HIGH TEMPERATURE ENDOTHERMIC REACTIONS
EP0911076A1 (en) * 1997-10-23 1999-04-28 Haldor Topsoe A/S Reformer furnace with internal recirculation
CA2357960C (en) * 2000-10-10 2007-01-30 Tokyo Gas Co., Ltd. Single-pipe cylinder type reformer
WO2009003647A1 (en) 2007-07-05 2009-01-08 Saudi Basic Industries Corporation Process for performing an endothermic reaction
DE102011118217A1 (en) * 2011-11-11 2013-05-16 L'Air Liquide, Société Anonyme pour l'Etude et l'Exploitation des Procédés Georges Claude Reformer tube with internal heat exchange
EP3266739B1 (en) 2016-07-07 2018-12-05 L'air Liquide, Société Anonyme Pour L'Étude Et L'exploitation Des Procédés Georges Claude Corrosion protected reformer tube with internal heat exchanger
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