WO2018096018A1 - Réacteur à lits multiples comprenant un lit de catalyseur chauffé et adiabatique - Google Patents

Réacteur à lits multiples comprenant un lit de catalyseur chauffé et adiabatique Download PDF

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Publication number
WO2018096018A1
WO2018096018A1 PCT/EP2017/080157 EP2017080157W WO2018096018A1 WO 2018096018 A1 WO2018096018 A1 WO 2018096018A1 EP 2017080157 W EP2017080157 W EP 2017080157W WO 2018096018 A1 WO2018096018 A1 WO 2018096018A1
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Prior art keywords
catalyst
reactor
adiabatic
catalyst bed
heated
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PCT/EP2017/080157
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English (en)
Inventor
Per Juul Dahl
Helbo Anders HANSEN
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Topsoe AS
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Haldor Topsoe AS
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    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J8/00—Chemical or physical processes in general, conducted in the presence of fluids and solid particles; Apparatus for such processes
    • B01J8/02—Chemical or physical processes in general, conducted in the presence of fluids and solid particles; Apparatus for such processes with stationary particles, e.g. in fixed beds
    • B01J8/04—Chemical or physical processes in general, conducted in the presence of fluids and solid particles; Apparatus for such processes with stationary particles, e.g. in fixed beds the fluid passing successively through two or more beds
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J8/00—Chemical or physical processes in general, conducted in the presence of fluids and solid particles; Apparatus for such processes
    • B01J8/02—Chemical or physical processes in general, conducted in the presence of fluids and solid particles; Apparatus for such processes with stationary particles, e.g. in fixed beds
    • B01J8/04—Chemical or physical processes in general, conducted in the presence of fluids and solid particles; Apparatus for such processes with stationary particles, e.g. in fixed beds the fluid passing successively through two or more beds
    • B01J8/0446—Chemical or physical processes in general, conducted in the presence of fluids and solid particles; Apparatus for such processes with stationary particles, e.g. in fixed beds the fluid passing successively through two or more beds the flow within the beds being predominantly vertical
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J8/00—Chemical or physical processes in general, conducted in the presence of fluids and solid particles; Apparatus for such processes
    • B01J8/02—Chemical or physical processes in general, conducted in the presence of fluids and solid particles; Apparatus for such processes with stationary particles, e.g. in fixed beds
    • B01J8/04—Chemical or physical processes in general, conducted in the presence of fluids and solid particles; Apparatus for such processes with stationary particles, e.g. in fixed beds the fluid passing successively through two or more beds
    • B01J8/0446—Chemical or physical processes in general, conducted in the presence of fluids and solid particles; Apparatus for such processes with stationary particles, e.g. in fixed beds the fluid passing successively through two or more beds the flow within the beds being predominantly vertical
    • B01J8/0449—Chemical or physical processes in general, conducted in the presence of fluids and solid particles; Apparatus for such processes with stationary particles, e.g. in fixed beds the fluid passing successively through two or more beds the flow within the beds being predominantly vertical in two or more cylindrical beds
    • B01J8/0453—Chemical or physical processes in general, conducted in the presence of fluids and solid particles; Apparatus for such processes with stationary particles, e.g. in fixed beds the fluid passing successively through two or more beds the flow within the beds being predominantly vertical in two or more cylindrical beds the beds being superimposed one above the other
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J8/00—Chemical or physical processes in general, conducted in the presence of fluids and solid particles; Apparatus for such processes
    • B01J8/02—Chemical or physical processes in general, conducted in the presence of fluids and solid particles; Apparatus for such processes with stationary particles, e.g. in fixed beds
    • B01J8/04—Chemical or physical processes in general, conducted in the presence of fluids and solid particles; Apparatus for such processes with stationary particles, e.g. in fixed beds the fluid passing successively through two or more beds
    • B01J8/0446—Chemical or physical processes in general, conducted in the presence of fluids and solid particles; Apparatus for such processes with stationary particles, e.g. in fixed beds the fluid passing successively through two or more beds the flow within the beds being predominantly vertical
    • B01J8/0461—Chemical or physical processes in general, conducted in the presence of fluids and solid particles; Apparatus for such processes with stationary particles, e.g. in fixed beds the fluid passing successively through two or more beds the flow within the beds being predominantly vertical in two or more cylindrical annular shaped beds
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J8/00—Chemical or physical processes in general, conducted in the presence of fluids and solid particles; Apparatus for such processes
    • B01J8/02—Chemical or physical processes in general, conducted in the presence of fluids and solid particles; Apparatus for such processes with stationary particles, e.g. in fixed beds
    • B01J8/06—Chemical or physical processes in general, conducted in the presence of fluids and solid particles; Apparatus for such processes with stationary particles, e.g. in fixed beds in tube reactors; the solid particles being arranged in tubes
    • B01J8/067—Heating or cooling the reactor
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
    • C01B3/00—Hydrogen; Gaseous mixtures containing hydrogen; Separation of hydrogen from mixtures containing it; Purification of hydrogen; Reversible storage of hydrogen
    • C01B3/02—Production of hydrogen; Production of gaseous mixtures containing hydrogen
    • C01B3/32—Production of hydrogen; Production of gaseous mixtures containing hydrogen by reaction of gaseous or liquid organic compounds with gasifying agents, e.g. water, carbon dioxide or air
    • C01B3/34—Production of hydrogen; Production of gaseous mixtures containing hydrogen by reaction of gaseous or liquid organic compounds with gasifying agents, e.g. water, carbon dioxide or air by reaction of hydrocarbons with gasifying agents
    • C01B3/38—Production of hydrogen; Production of gaseous mixtures containing hydrogen by reaction of gaseous or liquid organic compounds with gasifying agents, e.g. water, carbon dioxide or air by reaction of hydrocarbons with gasifying agents using catalysts
    • C01B3/384—Production of hydrogen; Production of gaseous mixtures containing hydrogen by reaction of gaseous or liquid organic compounds with gasifying agents, e.g. water, carbon dioxide or air by reaction of hydrocarbons with gasifying agents using catalysts with external heating of the catalyst
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J2208/00—Processes carried out in the presence of solid particles; Reactors therefor
    • B01J2208/00008—Controlling the process
    • B01J2208/00017—Controlling the temperature
    • B01J2208/00522—Controlling the temperature using inert heat absorbing solids outside the bed
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J2208/00—Processes carried out in the presence of solid particles; Reactors therefor
    • B01J2208/00743—Feeding or discharging of solids
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J2208/00—Processes carried out in the presence of solid particles; Reactors therefor
    • B01J2208/00796—Details of the reactor or of the particulate material
    • B01J2208/00805—Details of the particulate material
    • B01J2208/00814—Details of the particulate material the particulate material being provides in prefilled containers
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J2208/00—Processes carried out in the presence of solid particles; Reactors therefor
    • B01J2208/00796—Details of the reactor or of the particulate material
    • B01J2208/00884—Means for supporting the bed of particles, e.g. grids, bars, perforated plates
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J2208/00—Processes carried out in the presence of solid particles; Reactors therefor
    • B01J2208/02—Processes carried out in the presence of solid particles; Reactors therefor with stationary particles
    • B01J2208/023—Details
    • B01J2208/024—Particulate material
    • B01J2208/025—Two or more types of catalyst
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J2219/00—Chemical, physical or physico-chemical processes in general; Their relevant apparatus
    • B01J2219/00002—Chemical plants
    • B01J2219/00018—Construction aspects
    • B01J2219/00024—Revamping, retrofitting or modernisation of existing plants
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J8/00—Chemical or physical processes in general, conducted in the presence of fluids and solid particles; Apparatus for such processes
    • B01J8/02—Chemical or physical processes in general, conducted in the presence of fluids and solid particles; Apparatus for such processes with stationary particles, e.g. in fixed beds
    • B01J8/04—Chemical or physical processes in general, conducted in the presence of fluids and solid particles; Apparatus for such processes with stationary particles, e.g. in fixed beds the fluid passing successively through two or more beds
    • B01J8/0496—Heating or cooling the reactor
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
    • C01B2203/00—Integrated processes for the production of hydrogen or synthesis gas
    • C01B2203/02—Processes for making hydrogen or synthesis gas
    • 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
    • C01B2203/0233—Processes for making hydrogen or synthesis gas containing a reforming step containing a catalytic reforming step the reforming step being a steam reforming step

Definitions

  • Multi bed reactor comprising an adiabatic and a heated catalyst bed
  • prereforming reactors During the last 25 years use of separate prereforming reactors has become common part of the steam reforming section in synthesis gas preparation plants. In the begin- ning this was driven by the need to reform feed stocks with content of higher hydrocarbons.
  • Today prereforming is also used to reduce the size of the downstream primary reformer and to protect the catalyst in the primary reformer even in case of feedstocks with low content of hydrocarbon.
  • a prereforming step is an excellent catalyst guard removing for example all Sulphur components quantitatively.
  • the prereforming - primary reforming concept is a well-established concept in the industry
  • Prereforming protects the primary reforming catalyst typically increasing the expected lifetime from 3-5 to 10 years. Over a 10 years' period 1 to 2 primary reformer catalyst exchanges are thus avoided. As it is time consuming to change primary reformer catalyst this is a huge economic benefit, more than covering the cost of having a prereform- ing step.
  • Heat exchange reformers where a hot gas stream is used as heat source for the reforming process through heat exchange, are typical very compacts designs where catalyst is even more difficult to change than in a primary reformer. It is therefore very rel- evant to have a prereforming step before a heat exchange reformer. Heat exchange reformers are often used for revamps to increase the reforming capacity. This is also feasible for ammonia plants, which typically have no prereforming step and where it typically will not be economically feasible to install a separate prereforming step. In a first aspect of the present invention is provided a reactor which provides reduced equipment/piping cost.
  • a reactor which provides reduced plot space requirement thereby enabling cost savings and increased versatility of the reactor.
  • a rector comprising a guard layer and/or adiabatic catalyst layer and a heated catalyst bed.
  • a single reactor comprising a heated catalyst bed as well as a guard layer and/or adiabatic catalyst layer is provided whereby significant CAPEX savings may be achieved compared to known multi reactor setups.
  • the present invention thus combines prereforming and heat exchange reforming in a single reactor with no or minimal impact on the reactor dimensions.
  • the added cost of having a prereforming step protecting the heat exchange reforming step is therefore merely the catalyst cost making the combined solution economically feasible against a solution with no prereforming step, considering the heat exchange reformer catalyst exchange cost.
  • the heated catalyst bed is downstream the guard layer and/or adiabatic catalyst layer.
  • the outlet from the guard layer and/or adiabatic catalyst layer is the inlet to the heated catalyst bed. This way the reaction gas which enters the reactor first passes the guard layer and/or adiabatic catalyst layer and thereafter the heated catalyst bed.
  • the reaction gas first passes the guard layer and/or adiabatic catalyst layer i.e. when the adiabatic catalyst layer is arranged upstream the heated catalyst bed the lifetime of the catalyst in the heated catalyst bed may be significantly increased.
  • the heated catalyst bed is an exchange reformer, the process of changing the catalyst in the heated cata- lyst bed is relatively demanding in which case it may be highly desirable to be able to enhance the life time of the heated catalyst by adding the guard layer and/or adiabatic catalyst layer which furthermore may be simpler/faster/easier to change.
  • the guard layer and/or adiabatic catalyst layer may e.g. be a Sulphur guard, a hydro- carbon desulphurisation catalyst and/or a hydrocarbon steam reforming catalyst.
  • the catalyst in the heated catalyst bed may preferably be a hydrocarbon steam reforming catalyst.
  • the present reactor may be specifically designed and provided from new to comprise the heated catalyst bed as well as the guard layer and/or adiabatic catalyst layer.
  • the present reactor may alternatively be provided as a revamp solution to existing reactors comprising one or more heated catalyst beds.
  • the present reactor may be provided as a revamp to existing exchange reformers.
  • a heated catalyst bed is present in the reactor.
  • Above the heated catalyst bed is a hollow in known setups due to gas distribution requirements. The applicant has shown that this free space above the heated catalyst bed in a revamp solution advantageously may used for a guard layer and/or adiabatic catalyst layer.
  • the inventions is not limited to the prereforming - primary reformer concept but can also be used for other processes where a combination of an adiabatic/guard reactor and a heat exchange reactor is used.
  • An example of this could be a steam fired reverse shift reactor in combination with a chlorine/Sulphur guard layer.
  • the invention is valid for process combinations where the first step is the heat exchange reactor and the second step a guard/catalyst layer.
  • the heat exchange reactor has inherently also an empty room in the outlet head providing room for a guard/catalyst layer.
  • the guard/catalyst layer can for example be used to remove/convert bi-products formed in the heat exchange reactor step
  • Table 1 shows a typical set of process conditions for a heat exchange reformer.
  • the REACTOR INLET stream is send through a number of reforming catalyst containing tubes. These tubes are heated from outside by cooling the HEAT SOURCE gas. Before leaving the reactor the outlet gas from the catalyst containing tubes is mixed with the cooled heat source gas to form the final PRODUCT gas.
  • Table 2 shows the effect of sending the INLET REACTOR gas through an adiabatic pre-reforming catalyst layer before it is send through the heated reforming catalyst con- taining tubes.
  • the INTERMEDIATE shows the outlet stream from the adiabatic pre-reforming catalyst layer. It is seen that no higher hydrocarbons are present in this stream. Furthermore, Sulphur components in the INLET REACTOR stream will be absorbed by the pre reforming catalyst. These two effects increase the lifetime of the reforming catalyst in the tubes from approximate 3 years to 10 years. As a secondary effect the ca- pacity can be increased.
  • Figure 1 b) - f) show various examples of how a guard/adiabatic catalyst layer (1 ) can be integrated in a heat exchange reformer (2) with no or minimum change of the reactor dimensions.
  • the adiabatic catalyst layer (1 ) is placed in the entrance head of the heat exchange reformer (2), where there typically is an empty room, such that the incoming gas is send through this adiabatic catalyst layer 1 before entering the catalyst tubes (3).
  • Figure 1 b) provides example of a simple solution placing the guard/catalyst layer directly on the top of the tube sheet only separated by a grid (4) preventing catalyst from falling into the tubes.
  • Figure 1 c) - f) provides various examples of one or more cassette's (5) which easily can be taken in and out of the reactor for quick catalyst exchange.
  • Figure 1 shows a standard heat exchange reformer without an adiabatic catalyst layer.

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  • Chemical & Material Sciences (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Organic Chemistry (AREA)
  • Health & Medical Sciences (AREA)
  • General Health & Medical Sciences (AREA)
  • Engineering & Computer Science (AREA)
  • Combustion & Propulsion (AREA)
  • Inorganic Chemistry (AREA)
  • Hydrogen, Water And Hydrids (AREA)
  • Devices And Processes Conducted In The Presence Of Fluids And Solid Particles (AREA)

Abstract

La présente invention concerne un réacteur comprenant un lit de catalyseur chauffé et une couche de protection et/ou un catalyseur adiabatique, ainsi qu'un procédé de modernisation d'un acteur existant ayant au moins un lit de catalyseur chauffé.
PCT/EP2017/080157 2016-11-24 2017-11-23 Réacteur à lits multiples comprenant un lit de catalyseur chauffé et adiabatique Ceased WO2018096018A1 (fr)

Applications Claiming Priority (2)

Application Number Priority Date Filing Date Title
DKPA201600727 2016-11-24
DKPA201600727 2016-11-24

Publications (1)

Publication Number Publication Date
WO2018096018A1 true WO2018096018A1 (fr) 2018-05-31

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Citations (6)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US5464606A (en) * 1994-05-27 1995-11-07 Ballard Power Systems Inc. Two-stage water gas shift conversion method
US5928614A (en) * 1996-06-19 1999-07-27 Daimler Benz Ag Reforming reactor, particularly for the water vapor reforming of methanol
CN2621805Y (zh) * 2003-06-03 2004-06-30 华东理工大学 管壳外冷—绝热复合式固定床催化反应器
WO2007000244A1 (fr) * 2005-06-28 2007-01-04 Haldor Topsøe A/S Réacteur de réformage compact
CN102649564A (zh) * 2011-02-25 2012-08-29 中国石油化工股份有限公司 含co混合气体原料借助催化氧化反应脱氢的方法
CN105536654A (zh) * 2015-12-15 2016-05-04 惠生工程（中国）有限公司 一种大型轴向多段混合换热式丁烯氧化脱氢反应器

Patent Citations (6)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US5464606A (en) * 1994-05-27 1995-11-07 Ballard Power Systems Inc. Two-stage water gas shift conversion method
US5928614A (en) * 1996-06-19 1999-07-27 Daimler Benz Ag Reforming reactor, particularly for the water vapor reforming of methanol
CN2621805Y (zh) * 2003-06-03 2004-06-30 华东理工大学 管壳外冷—绝热复合式固定床催化反应器
WO2007000244A1 (fr) * 2005-06-28 2007-01-04 Haldor Topsøe A/S Réacteur de réformage compact
CN102649564A (zh) * 2011-02-25 2012-08-29 中国石油化工股份有限公司 含co混合气体原料借助催化氧化反应脱氢的方法
CN105536654A (zh) * 2015-12-15 2016-05-04 惠生工程（中国）有限公司 一种大型轴向多段混合换热式丁烯氧化脱氢反应器

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