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WO2001037982A1 - Steam reforming apparatus - Google Patents

Steam reforming apparatus Download PDF

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Publication number
WO2001037982A1
WO2001037982A1 PCT/GB2000/004127 GB0004127W WO0137982A1 WO 2001037982 A1 WO2001037982 A1 WO 2001037982A1 GB 0004127 W GB0004127 W GB 0004127W WO 0137982 A1 WO0137982 A1 WO 0137982A1
Authority
WO
WIPO (PCT)
Prior art keywords
tube
reformer
inner tube
section
circular cross
Prior art date
Application number
PCT/GB2000/004127
Other languages
French (fr)
Inventor
Bernard John Crewdson
Raymond Davies
Peter William Farnell Farnell
Original Assignee
Imperial Chemical Industries Plc
Priority date (The priority date 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 date listed.)
Filing date
Publication date
Application filed by Imperial Chemical Industries Plc filed Critical Imperial Chemical Industries Plc
Priority to CA002392349A priority Critical patent/CA2392349A1/en
Priority to AU79368/00A priority patent/AU7936800A/en
Publication of WO2001037982A1 publication Critical patent/WO2001037982A1/en

Links

Classifications

    • 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
    • B01J8/008—Details of the reactor or of the particulate material; Processes to increase or to retard the rate of reaction
    • 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
    • B01J8/062—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 being installed in a furnace
    • 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
    • C01B3/02—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen
    • C01B3/32—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen by reaction of gaseous or liquid organic compounds with gasifying agents, e.g. water, carbon dioxide, air
    • C01B3/34—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen by reaction of gaseous or liquid organic compounds with gasifying agents, e.g. water, carbon dioxide, air by reaction of hydrocarbons with gasifying agents
    • C01B3/38—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen by reaction of gaseous or liquid organic compounds with gasifying agents, e.g. water, carbon dioxide, air by reaction of hydrocarbons with gasifying agents using catalysts
    • C01B3/384—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen by reaction of gaseous or liquid organic compounds with gasifying agents, e.g. water, carbon dioxide, air by reaction of hydrocarbons with gasifying agents using catalysts the catalyst being continuously externally heated
    • 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
    • B01J2208/00106—Controlling the temperature by indirect heat exchange
    • B01J2208/00115—Controlling the temperature by indirect heat exchange with heat exchange elements inside the bed of solid particles
    • B01J2208/00132—Tubes
    • 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
    • B01J2219/00049—Controlling or regulating processes
    • B01J2219/00051—Controlling the temperature
    • B01J2219/00157—Controlling the temperature by means of a burner
    • 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
    • C01B2203/08—Methods of heating or cooling
    • 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

Definitions

  • This invention relates to steam reforming apparatus and in particular to the design of steam reforming tubes
  • a process gas i e a mixture of a hydrocarbon feedstock and steam, and in some cases also carbon dioxide
  • a suitable heating medium generally a hot gas mixture
  • the catalyst is normally in the form of shaped units, e g cylinders, rings, saddles, and cylinders having a plurality of through holes, and are typically formed from a refractory support material e g alumina, calcium aluminate cement, magnesia or zirconia impregnated with a suitable catalytically active material which is often nickel or ruthenium
  • the reformer tubes are of a double-tube design, having an outer tube and a concentric inner tube thus providing a space between the inner and outer tubes
  • the catalyst units are disposed in this space, normally random packed as a result of pouring the catalyst units into the space from one end
  • the outer tube is often closed at one end and the process gas passes through the space between the interior surface of the outer tube and the exterior surface of the inner tube, and then returns through the inner tube
  • the tubes normally have a circular cross-section and have a length of several metres, e g 5 to 15 m, and the outer tube typically has an outer diameter in the range 7 to 20 cm
  • the tubes are generally disposed vertically In operation the tubes are heated to a high temperature, typically to a maximum temperature in the range 700°C to 900°C by a suitable medium flowing past the exterior of the outer tubes This heating necessarily means that the tubes are subject to considerable thermal expansion, both longitudinally and radially, as the tubes are heated
  • the circular cross-section of the outer tubes is dictated by the need for the tubes to withstand a substantial pressure differential between the pressure of the process gas within the tubes and the pressure of the heating medium
  • the heating medium is at a pressure in the range 1 to 4 bar abs while the process gas may be at a pressure in the range 20 to 80 bar abs While this pressure differential may be decreased if the pressure of the heating medium is increased, for example where the heating medium is the process gas after further treatment, e g secondary reforming as described in the aforesaid US 4 690 690, there is still liable to be a pressure differential of several bar between the process gas and the heating medium
  • the present invention provides a reformer tube of the double-tube configuration having an outer tube of substantially circular cross-section and an inner tube disposed within the outer tube, said inner tube having a non-circular cross-section
  • the invention also provides the use in a double-tube reformer of an inner tube having a non-circular cross-section
  • the inner tube is more capable, than a tube of circular cross-section, of local deflection and so can deflect to accommodate settled catalyst units, thereby decreasing the crushing forces to which the catalyst units are subject
  • the cross-section of the inner tubes is non-circular in particular the maximum cross- sectional dimension of the inner tubes is at least 1 2, and preferably at least 1 4, times the minimum dimension
  • the cross-section is preferably polygonal, particularly a regular polygon having 3 to 6 sides, preferably 4 to 5 sides While the sides of the polygon may be straight, so that the cross-sections are those of e g an equilateral triangle, square, regular pentagon or hexagon, the sides of the polygon are preferably inwardly curved
  • the curve may be an arc of a circle or in particular is in the form of a catenary (hyperbolic cosine curve)
  • the inner tube is formed by welding, e g by electrical resistance or laser seam welding, together the edges of metal strips of substantially uniform thickness that are curved across their width
  • the strips are preferably relatively thin, thus the maximum thickness of the walls of the inner tube, i e at the seam-welded edges in the aforesaid form of construction, is preferably less than 5%
  • Figure 1 is a diagrammatic section of a double-tube reformer tube assembly and Figure 2 is a section along line II - II of Figure 1
  • the reformer tube assembly comprises an outer reformer tube 10 of circular cross- section, closed at its lower end 11 , and suspended from a tube-sheet 12 Surrounding tube 10 for the major part of its length is a sheath tube 13, also of circular cross-section, open at both ends and suspended from a second tube-sheet 14 beneath tube sheet 12
  • Tube 15 is made by seam-welding together the long edges of four elongated strips of metal 16a, 16b, 16c and 16d, each having a substantially uniform thickness but curved across its width so that the outer surface of the welded structure has an inwardly curved, i e concave, cross-section
  • the upper end 17 of tube 15 is flared to a circular cross- section, for ease of connection to a process gas outlet conduit (not shown)
  • a perforate mesh 18 (not shown in
  • a heating gas is supplied to the exterior of the lower end 11 of tube 10 and passes up through the space 23 between the inner surface 24 of the sheath tube 13 and the outer surface 25 of tube 10 This heating gas then leaves sheath tube 13 at the upper end thereof and is collected from the space between tube-sheets 12 and 14
  • the concave sides of the inner tube are able to reduce their radius of curvature under force from the catalyst units much more easily, i e at much lower force, than if the inner tube has a circular cross-section
  • the inner tube becomes progressively inwardly deformed with each expansion/contraction cycle resulting from heating and cooling the assembly
  • the resulting decrease in the cross-sectional area of the inner tube has no significant detrimental effect on the gas flow through the inner tube

Landscapes

  • 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)

Abstract

A reformer tube, for a steam reformer, having a double-tube configuration with an outer tube (10) of substantially circular cross section and an inner tube (15) of non-circular cross section disposed within the outer tube (10).

Description

Steam reforming apparatus
This invention relates to steam reforming apparatus and in particular to the design of steam reforming tubes
In the steam reforming process a process gas, i e a mixture of a hydrocarbon feedstock and steam, and in some cases also carbon dioxide, is passed at an elevated pressure through catalyst-filled tubes which are externally heated by means of a suitable heating medium, generally a hot gas mixture The catalyst is normally in the form of shaped units, e g cylinders, rings, saddles, and cylinders having a plurality of through holes, and are typically formed from a refractory support material e g alumina, calcium aluminate cement, magnesia or zirconia impregnated with a suitable catalytically active material which is often nickel or ruthenium
In one form of reformer design, the reformer tubes are of a double-tube design, having an outer tube and a concentric inner tube thus providing a space between the inner and outer tubes The catalyst units are disposed in this space, normally random packed as a result of pouring the catalyst units into the space from one end In this arrangement, the outer tube is often closed at one end and the process gas passes through the space between the interior surface of the outer tube and the exterior surface of the inner tube, and then returns through the inner tube An example of such a construction is described in US 4 690 690 The tubes normally have a circular cross-section and have a length of several metres, e g 5 to 15 m, and the outer tube typically has an outer diameter in the range 7 to 20 cm The tubes are generally disposed vertically In operation the tubes are heated to a high temperature, typically to a maximum temperature in the range 700°C to 900°C by a suitable medium flowing past the exterior of the outer tubes This heating necessarily means that the tubes are subject to considerable thermal expansion, both longitudinally and radially, as the tubes are heated from ambient temperature at which the catalyst is normally loaded and the operating temperature and likewise to thermal contraction as the tube is cooled upon shut down of the process The thermal expansion permits the catalyst units to settle down the space between the tubes and subsequent contraction, particularly that in the radial direction, subjects the catalyst units to severe crushing forces, often leading to catalyst breakage
The circular cross-section of the outer tubes is dictated by the need for the tubes to withstand a substantial pressure differential between the pressure of the process gas within the tubes and the pressure of the heating medium For example in many applications, the heating medium is at a pressure in the range 1 to 4 bar abs while the process gas may be at a pressure in the range 20 to 80 bar abs While this pressure differential may be decreased if the pressure of the heating medium is increased, for example where the heating medium is the process gas after further treatment, e g secondary reforming as described in the aforesaid US 4 690 690, there is still liable to be a pressure differential of several bar between the process gas and the heating medium
On the other hand, where the process gas passes through the catalyst and then back through the inner tube, the pressure differential across the walls of the inner tube can be relatively small and so the inner tube can be made from relatively light gauge material We have now realised that because the inner tube does not have to withstand such large mechanical stresses as the outer tube, it need not be of circular cross-section and indeed advantages may result from the use of a non-circular cross-section Accordingly the present invention provides a reformer tube of the double-tube configuration having an outer tube of substantially circular cross-section and an inner tube disposed within the outer tube, said inner tube having a non-circular cross-section
The invention also provides the use in a double-tube reformer of an inner tube having a non-circular cross-section As a result of the use of an inner tube of non-circular cross-section, the inner tube is more capable, than a tube of circular cross-section, of local deflection and so can deflect to accommodate settled catalyst units, thereby decreasing the crushing forces to which the catalyst units are subject
One consequence of the use of an inner tube of non-circular cross-section within an outer tube of circular cross-section is that the width of the space between the tubes varies round the perimeter of the reformer tube, leading to differing radial depths of catalyst in this space However, calculation has shown that such a variation in the depth of the catalyst space has negligible effect on the degree of reforming that will occur
The cross-section of the inner tubes is non-circular in particular the maximum cross- sectional dimension of the inner tubes is at least 1 2, and preferably at least 1 4, times the minimum dimension The cross-section is preferably polygonal, particularly a regular polygon having 3 to 6 sides, preferably 4 to 5 sides While the sides of the polygon may be straight, so that the cross-sections are those of e g an equilateral triangle, square, regular pentagon or hexagon, the sides of the polygon are preferably inwardly curved The curve may be an arc of a circle or in particular is in the form of a catenary (hyperbolic cosine curve) In a preferred arrangement, the inner tube is formed by welding, e g by electrical resistance or laser seam welding, together the edges of metal strips of substantially uniform thickness that are curved across their width The strips are preferably relatively thin, thus the maximum thickness of the walls of the inner tube, i e at the seam-welded edges in the aforesaid form of construction, is preferably less than 5% of the maximum cross-section dimension of the inner tube
The invention is illustrated by the accompanying drawings wherein Figure 1 is a diagrammatic section of a double-tube reformer tube assembly and Figure 2 is a section along line II - II of Figure 1
The reformer tube assembly comprises an outer reformer tube 10 of circular cross- section, closed at its lower end 11 , and suspended from a tube-sheet 12 Surrounding tube 10 for the major part of its length is a sheath tube 13, also of circular cross-section, open at both ends and suspended from a second tube-sheet 14 beneath tube sheet 12
Disposed within tube 10 is an inner tube 15 open at its lower end and having a non- circular cross-section Tube 15 is made by seam-welding together the long edges of four elongated strips of metal 16a, 16b, 16c and 16d, each having a substantially uniform thickness but curved across its width so that the outer surface of the welded structure has an inwardly curved, i e concave, cross-section The upper end 17 of tube 15 is flared to a circular cross- section, for ease of connection to a process gas outlet conduit (not shown) At the lower end of outer tube 10 is disposed a perforate mesh 18 (not shown in
Figure 2) which serves as a restraint for the catalyst units
In use shaped catalyst units, e g pellets or rings, are charged to the space 19 above mesh 18 between the inner surface 20 of the outer tube 10 and the exterior, inwardly curved, surface 21 of inner tube 15 Process gas, e g a mixture of natural gas and steam, is fed to the space above tube-sheet 12 and passes down through the catalyst-filled space 19, where it undergoes reforming The reformed process gas passes through mesh 18 and flows up through the space 22 inside inner tube 15 and leaves the reformer tube assembly at the top of tube 15 via the process gas outlet conduit (not shown)
To provide the heat required for the endothermic reforming reaction, a heating gas is supplied to the exterior of the lower end 11 of tube 10 and passes up through the space 23 between the inner surface 24 of the sheath tube 13 and the outer surface 25 of tube 10 This heating gas then leaves sheath tube 13 at the upper end thereof and is collected from the space between tube-sheets 12 and 14
In use the concave sides of the inner tube are able to reduce their radius of curvature under force from the catalyst units much more easily, i e at much lower force, than if the inner tube has a circular cross-section By equilibrium this results in a lower reaction force on the catalyst units and thus the catalyst units are less liable to breakage As a result the inner tube becomes progressively inwardly deformed with each expansion/contraction cycle resulting from heating and cooling the assembly However the resulting decrease in the cross-sectional area of the inner tube has no significant detrimental effect on the gas flow through the inner tube

Claims

Claims
1 A reformer tube of the double-tube configuration having an outer tube of substantially circular cross-section and an inner tube disposed within the outer tube, said inner tube having a non-circular cross-section
2 A reformer tube according to claim 1 wherein the inner tube has a maximum cross- sectional dimension that is at least 1 2 times the cross-sectional minimum dimension
3 A reformer tube according to claim 1 or claim 2 wherein the inner tube has a polygonal cross-section
4 A reformer tube according to claim 3 wherein the polygon has 4 or 5 sides
5 A reformer tube according to claim 3 or claim 4 wherein the sides of the polygon are concave
6 A reformer tube according to any one of claims 3 to 5 wherein the inner tube comprises a plurality of metal strips of substantially uniform thickness seam-welded together along their edges
7 A reformer tube according to any one of claims 1 to 6 wherein the maximum thickness of the walls of the inner tube is less than 5% of the maximum dimension of the inner tube
8 A double-tube reformer including reformer tubes according to any one of claims 1 to 7 having shaped catalyst units randomly packed in the space between the inner and outer tubes
9 The use in a double-tube reformer of an inner tube of non-circular cross-section
PCT/GB2000/004127 1999-11-26 2000-10-27 Steam reforming apparatus WO2001037982A1 (en)

Priority Applications (2)

Application Number Priority Date Filing Date Title
CA002392349A CA2392349A1 (en) 1999-11-26 2000-10-27 Steam reforming apparatus
AU79368/00A AU7936800A (en) 1999-11-26 2000-10-27 Steam reforming apparatus

Applications Claiming Priority (2)

Application Number Priority Date Filing Date Title
GB9927817.8 1999-11-26
GBGB9927817.8A GB9927817D0 (en) 1999-11-26 1999-11-26 Steam reforming apparatus

Publications (1)

Publication Number Publication Date
WO2001037982A1 true WO2001037982A1 (en) 2001-05-31

Family

ID=10865087

Family Applications (1)

Application Number Title Priority Date Filing Date
PCT/GB2000/004127 WO2001037982A1 (en) 1999-11-26 2000-10-27 Steam reforming apparatus

Country Status (4)

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AU (1) AU7936800A (en)
CA (1) CA2392349A1 (en)
GB (1) GB9927817D0 (en)
WO (1) WO2001037982A1 (en)

Cited By (2)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
WO2004092060A1 (en) * 2003-04-15 2004-10-28 Shell Internationale Research Maatschappij B.V. Reactor for performing a steam reforming reaction and a process to prepare synthesis gas
KR101478821B1 (en) 2010-11-05 2015-02-04 미드렉스 테크놀리지스, 인코오포레이티드 Reformer tube apparatus having variable wall thickness and associated method of manufacture

Citations (3)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
FR841008A (en) * 1937-09-01 1939-05-09 Krupp Ag temperature exchanger intended for the synthesis of hydrocarbons, in particular for the manufacture of pressurized gasoline
US2662911A (en) * 1948-10-01 1953-12-15 Metallgesellschaft Ag Temperature control in the catalytic hydrogenation of carbon monoxide
DE2405606A1 (en) * 1969-01-15 1975-08-07 Gerhard Martens Reaction element for catalytic hydrocarbon conversion - has several spiral inner tubes inside straight outer tube

Patent Citations (3)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
FR841008A (en) * 1937-09-01 1939-05-09 Krupp Ag temperature exchanger intended for the synthesis of hydrocarbons, in particular for the manufacture of pressurized gasoline
US2662911A (en) * 1948-10-01 1953-12-15 Metallgesellschaft Ag Temperature control in the catalytic hydrogenation of carbon monoxide
DE2405606A1 (en) * 1969-01-15 1975-08-07 Gerhard Martens Reaction element for catalytic hydrocarbon conversion - has several spiral inner tubes inside straight outer tube

Cited By (5)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
WO2004092060A1 (en) * 2003-04-15 2004-10-28 Shell Internationale Research Maatschappij B.V. Reactor for performing a steam reforming reaction and a process to prepare synthesis gas
US7462209B2 (en) 2003-04-15 2008-12-09 Shell Oil Company Reactor for performing a steam reforming reaction and a process to prepare synthesis gas
US7550635B2 (en) 2003-04-15 2009-06-23 Shell Oil Company Process for the preparation hydrogen and a mixture of hydrogen and carbon monoxide
US8986631B2 (en) 2003-04-15 2015-03-24 Shell Oil Company Reactor vessel for performing a steam reforming reaction and a process to prepare synthesis gas
KR101478821B1 (en) 2010-11-05 2015-02-04 미드렉스 테크놀리지스, 인코오포레이티드 Reformer tube apparatus having variable wall thickness and associated method of manufacture

Also Published As

Publication number Publication date
AU7936800A (en) 2001-06-04
GB9927817D0 (en) 2000-01-26
CA2392349A1 (en) 2001-05-31

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