US20040067174A1 - Reactor for chemical conversion of a feedstock with heat inputs and feedstock/catalyst cross-circulation - Google Patents

Reactor for chemical conversion of a feedstock with heat inputs and feedstock/catalyst cross-circulation Download PDF

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US20040067174A1
US20040067174A1 US10/432,773 US43277303A US2004067174A1 US 20040067174 A1 US20040067174 A1 US 20040067174A1 US 43277303 A US43277303 A US 43277303A US 2004067174 A1 US2004067174 A1 US 2004067174A1
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feed
reactor
catalyst
extraction
catalytic
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US10/432,773
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Eric Lenglet
Nicolas Boudet
Frederic Hoffmann
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IFP Energies Nouvelles IFPEN
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IFP Energies Nouvelles IFPEN
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Assigned to INSTITUT FRANCAIS DU PETROLE reassignment INSTITUT FRANCAIS DU PETROLE ASSIGNMENT OF ASSIGNORS INTEREST (SEE DOCUMENT FOR DETAILS). Assignors: BOUDET, NICOLAS, HOFFMANN, FREDERIC, LENGLET, ERIC
Publication of US20040067174A1 publication Critical patent/US20040067174A1/en
Priority to US11/442,328 priority Critical patent/US7357855B2/en
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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
    • B01J8/0496—Heating or cooling the reactor
    • 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
    • B01J8/0403—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 fluid flow within the beds being predominantly horizontal
    • B01J8/0423—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 fluid flow within the beds being predominantly horizontal through two or more otherwise shaped beds
    • B01J8/0438—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 fluid flow within the beds being predominantly horizontal through two or more otherwise shaped beds the beds being placed next to each 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
    • B01J8/08—Chemical or physical processes in general, conducted in the presence of fluids and solid particles; Apparatus for such processes with moving particles
    • B01J8/12—Chemical or physical processes in general, conducted in the presence of fluids and solid particles; Apparatus for such processes with moving particles moved by gravity in a downward flow

Definitions

  • One method for obtaining a high conversion consists of introducing heating surfaces into the catalytic bed, or using a plurality of catalytic beds separated by zones for re-heating the reaction fluid.
  • the catalyst is at least partially deactivated during the reaction, for example by coking, and must be extracted, continuously or at distinct time intervals, and replaced by new or regenerated catalyst.
  • Processes such as catalytic hydrocarbon reforming are known in which the reaction feed successively traverses a plurality of catalytic bed reactors, with intermediate re-heating between the reactors to compensate for cooling of the reaction fluid due to the endothermic nature of the reaction.
  • the catalyst moves from one reactor to another, as a co-current or as a counter-current to the feed before being regenerated and recycled.
  • the catalyst is used efficiently and homogeneously coked before being regenerated.
  • a first aim of the invention is to provide a reactor for carrying out a chemical conversion process in catalytic beds with means for supplying heat integrated into said reactor, and thus with a very compact reaction zone, combined with efficient use of the catalyst.
  • a further aim of the invention is to provide a process for converting a feed (usually a hydrocarbon feed) undergoing an endothermic reaction using said reactor.
  • the scope of the present invention also encompasses using a series of reactors at least one of which is in accordance with the present invention.
  • the invention concerns a reactor for chemical conversion of a feed, said chemical conversion reactor containing a substantially vertical catalytic bed between an upper end and a lower end, and comprising in combination:
  • said reactor comprises, close to its lower end, at least one means for extraction of the catalyst, which extraction is differentiated between an upstream portion and a downstream portion of said catalytic bed, with respect to the direction of flow of said feed.
  • the reactor can be a reactor-exchanger with heating surfaces immersed in the catalytic bed; it can also comprise a plurality of catalytic beds separated by non-catalytic zones for heating the reaction feed. In each of these zones, the reaction feed traverses a heat exchanger, supplied with a heat transfer fluid.
  • Heat transfer fluids that can be used include pressurised steam, for example between 0.5 MPa and 1.20 MPa, preferably between 0.6 MP and 1 MPa absolute, limits included, hydrogen or a hydrogen-containing gas such as a hydrogen-rich recycle gas, such as that used in certain processes to dilute the reaction feed to protect the catalyst. It is also possible to use the unconverted feed itself, or liquids such as molten salts or liquid sodium.
  • the differentiated catalyst extraction means is normally selected from the group formed by continuous and discontinuous extraction means.
  • the catalytic bed comprises a plurality of catalytic zones separated by noncatalytic zones for heating the feed.
  • the most upstream catalyst extraction means differs from at least one downstream extraction means, and particularly that located the furthest downstream, in its lower extraction capacity (the concepts of upstream and downstream being with respect to the direction of flow of the feed).
  • the invention also proposes a process for chemical conversion of a feed using a reactor as described above.
  • the feed is a hydrocarbon feed, often with an added diluent (for example steam, hydrogen, nitrogen or a mixture of these gases).
  • an added diluent for example steam, hydrogen, nitrogen or a mixture of these gases.
  • the chemical conversion process is a process for catalytic dehydrogenation of a paraffinic hydrocarbon feed.
  • FIG. 1 is a non-limiting representation of a reactor R in accordance with the invention used to carry out an endothermic reaction.
  • the reaction feed is introduced into reactor R via a line 1 ; it traverses, in succession, a catalytic bed 3 a, then a heat exchanger 4 a, then a second catalytic bed 3 b, then a second heat exchanger 4 b, then a third and last catalytic bed 3 c, before leaving the reactor via a line 2 .
  • the catalyst is introduced into the reactor at the head thereof via a line 9 . It is distributed into the three catalytic beds 3 a, 3 b, 3 c in which they flow under gravity in downflow mode.
  • Each catalytic bed has a separate hopper for evacuating the catalyst: 7 a for bed 3 a, 7 b for bed 3 b and 7 c for bed 3 c.
  • Extraction valves 8 a, 8 b, 8 c at the bottom of each of the catalytic beds can separately extract used catalyst flowing in each of the catalytic beds in series.
  • the catalyst is evacuated via lines 80 a, 80 b and 80 c.
  • Heat exchangers 4 a and 4 b are fed by heat transfer fluid introduced via lines 5 , 5 a and 5 b, this fluid leaving the exchanger via lines 6 a, 6 b and 6 .
  • a substantially inert gas is introduced via lines 10 , 10 a and 10 b.
  • the function of the gas is to provide a barrier gas to prevent feed passing from bed 3 a to bed 3 b and by-passing exchanger 4 a, and similarly preventing feed passing from bed 3 b to bed 3 c and by-passing exchanger 4 b.
  • this gas can be a diluent for the fed, for example steam or a hydrogen-rich recycle gas.
  • the feed pre-heated to the reaction temperature, traverses the three catalytic beds (or zones) 3 a, 3 b, 3 c in series, with two intermediate re-heating steps.
  • the catalyst, introduced via line 9 , is extracted continuously or discontinuously via lines 80 a, 80 b, 80 c.
  • the catalyst flowing in bed 3 c is preferably renewed more rapidly than that in bed 3 a.
  • the catalyst ages more rapidly and deactivates and cokes more rapidly at the end of the reaction zone, i.e., in the downstream bed 3 c more than in the upstream bed 3 a.
  • 3 c is renewed more rapidly than 3 b, which is itself renewed more rapidly than bed 3 a.
  • the invention thus enables the catalyst to be used efficiently, which catalyst is extracted in a relatively constant state of deactivation.
  • valves 8 a, 8 b, 8 c can be used to adjust the differentiated catalyst extraction.
  • the reactors of the invention can contain 2 to about 20 catalytic zones separated by heat exchange zones.
  • reaction fluid can also be introduced laterally and flow horizontally, as a crosswise current with the feed.
  • the reactor of the invention can carry out chemical conversion of a feed in the presence of a catalyst while providing each of the catalytic zones with the necessary amount of heat. It also enables the at least partially deactivated catalyst to be extracted in a differentiated manner.
  • the reactor of the invention can maintain a high catalytic activity and/or productivity for the desired product.
  • the invention can in particular be employed for hydrocarbon reforming, for dehydrogenating ethylbenzene, and for dehydrogenating paraffins such as propane, n-butane, isobutane, primarily linear paraffins containing 10 to 14 carbon atoms, and for the production of olefins for the production of alkylbenzenes, or for other chemical reactions.
  • paraffins such as propane, n-butane, isobutane, primarily linear paraffins containing 10 to 14 carbon atoms, and for the production of olefins for the production of alkylbenzenes, or for other chemical reactions.

Abstract

A chemical conversion reactor contains a substantially vertical catalytic bed between an upper end and a lower end and comprises, in combination: close to its upper end, at least one means for introducing a solid catalyst, means for introducing and evacuating said feed allowing its flow in a substantially horizontal direction through the catalytic bed, means for heating said feed integrated into said reactor, said reactor comprising, close to its lower end, at least one means for extraction of the catalyst, which extraction is differentiated between an upstream portion and a downstream portion of said catalytic bed, with respect to the direction of flow of said feed.

Description

  • The chemical, petroleum and petrochemical industries employ many endothermic chemical reactions, for example cracking reactions, dehydrogenation reactions or hydrocarbon reforming reactions. [0001]
  • Certain of those reactions are reversible and limited by a thermodynamic equilibrium. In that case, the cooling occurring in the catalytic bed due to the endothermic nature of the reaction limits the reactant conversion. [0002]
  • One method for obtaining a high conversion consists of introducing heating surfaces into the catalytic bed, or using a plurality of catalytic beds separated by zones for re-heating the reaction fluid. [0003]
  • In many cases, in particular for hydrocarbon dehydrogenation, the catalyst is at least partially deactivated during the reaction, for example by coking, and must be extracted, continuously or at distinct time intervals, and replaced by new or regenerated catalyst. [0004]
  • Processes such as catalytic hydrocarbon reforming are known in which the reaction feed successively traverses a plurality of catalytic bed reactors, with intermediate re-heating between the reactors to compensate for cooling of the reaction fluid due to the endothermic nature of the reaction. The catalyst moves from one reactor to another, as a co-current or as a counter-current to the feed before being regenerated and recycled. The catalyst is used efficiently and homogeneously coked before being regenerated. [0005]
  • A first aim of the invention is to provide a reactor for carrying out a chemical conversion process in catalytic beds with means for supplying heat integrated into said reactor, and thus with a very compact reaction zone, combined with efficient use of the catalyst. A further aim of the invention is to provide a process for converting a feed (usually a hydrocarbon feed) undergoing an endothermic reaction using said reactor. The scope of the present invention also encompasses using a series of reactors at least one of which is in accordance with the present invention. [0006]
  • To this end, the invention concerns a reactor for chemical conversion of a feed, said chemical conversion reactor containing a substantially vertical catalytic bed between an upper end and a lower end, and comprising in combination: [0007]
  • close to its upper end, at least one means for introducing a solid catalyst; [0008]
  • means for introducing and evacuating said feed allowing its flow in a substantially horizontal direction through the catalytic bed; [0009]
  • means for heating said feed integrated into said reactor; [0010]
  • in which said reactor comprises, close to its lower end, at least one means for extraction of the catalyst, which extraction is differentiated between an upstream portion and a downstream portion of said catalytic bed, with respect to the direction of flow of said feed. [0011]
  • The reactor can be a reactor-exchanger with heating surfaces immersed in the catalytic bed; it can also comprise a plurality of catalytic beds separated by non-catalytic zones for heating the reaction feed. In each of these zones, the reaction feed traverses a heat exchanger, supplied with a heat transfer fluid. [0012]
  • Heat transfer fluids that can be used include pressurised steam, for example between 0.5 MPa and 1.20 MPa, preferably between 0.6 MP and 1 MPa absolute, limits included, hydrogen or a hydrogen-containing gas such as a hydrogen-rich recycle gas, such as that used in certain processes to dilute the reaction feed to protect the catalyst. It is also possible to use the unconverted feed itself, or liquids such as molten salts or liquid sodium. [0013]
  • The differentiated catalyst extraction means is normally selected from the group formed by continuous and discontinuous extraction means. [0014]
  • Preferably, the catalytic bed comprises a plurality of catalytic zones separated by noncatalytic zones for heating the feed. [0015]
  • In a preferred feature of the invention, the most upstream catalyst extraction means differs from at least one downstream extraction means, and particularly that located the furthest downstream, in its lower extraction capacity (the concepts of upstream and downstream being with respect to the direction of flow of the feed). [0016]
  • The invention also proposes a process for chemical conversion of a feed using a reactor as described above. [0017]
  • Typically, the feed is a hydrocarbon feed, often with an added diluent (for example steam, hydrogen, nitrogen or a mixture of these gases). [0018]
  • In a particular implementation of the invention, the chemical conversion process is a process for catalytic dehydrogenation of a paraffinic hydrocarbon feed.[0019]
  • We shall now refer to FIG. 1, which is a non-limiting representation of a reactor R in accordance with the invention used to carry out an endothermic reaction.[0020]
  • The reaction feed is introduced into reactor R via a line [0021] 1; it traverses, in succession, a catalytic bed 3 a, then a heat exchanger 4 a, then a second catalytic bed 3 b, then a second heat exchanger 4 b, then a third and last catalytic bed 3 c, before leaving the reactor via a line 2. The catalyst is introduced into the reactor at the head thereof via a line 9. It is distributed into the three catalytic beds 3 a, 3 b, 3 c in which they flow under gravity in downflow mode. Each catalytic bed has a separate hopper for evacuating the catalyst: 7 a for bed 3 a, 7 b for bed 3 b and 7 c for bed 3 c.
  • [0022] Extraction valves 8 a, 8 b, 8 c at the bottom of each of the catalytic beds can separately extract used catalyst flowing in each of the catalytic beds in series. The catalyst is evacuated via lines 80 a, 80 b and 80 c.
  • [0023] Heat exchangers 4 a and 4 b are fed by heat transfer fluid introduced via lines 5, 5 a and 5 b, this fluid leaving the exchanger via lines 6 a, 6 b and 6.
  • At the upper portion of [0024] beds 3 a and 3 b, a substantially inert gas is introduced via lines 10, 10 a and 10 b. The function of the gas is to provide a barrier gas to prevent feed passing from bed 3 a to bed 3 b and by-passing exchanger 4 a, and similarly preventing feed passing from bed 3 b to bed 3 c and by-passing exchanger 4 b.
  • Typically, this gas can be a diluent for the fed, for example steam or a hydrogen-rich recycle gas. [0025]
  • The unit functions as follows. [0026]
  • The feed, pre-heated to the reaction temperature, traverses the three catalytic beds (or zones) [0027] 3 a, 3 b, 3 c in series, with two intermediate re-heating steps.
  • The catalyst, introduced via line [0028] 9, is extracted continuously or discontinuously via lines 80 a, 80 b, 80 c.
  • In the reactor, in accordance with the invention, the catalyst flowing in [0029] bed 3 c is preferably renewed more rapidly than that in bed 3 a. Typically, the catalyst ages more rapidly and deactivates and cokes more rapidly at the end of the reaction zone, i.e., in the downstream bed 3 c more than in the upstream bed 3 a. Preferably, 3 c is renewed more rapidly than 3 b, which is itself renewed more rapidly than bed 3 a.
  • The invention thus enables the catalyst to be used efficiently, which catalyst is extracted in a relatively constant state of deactivation. [0030]
  • When operation is continuous, [0031] valves 8 a, 8 b, 8 c can be used to adjust the differentiated catalyst extraction.
  • When operation is discontinuous, varying quantities of catalyst can be extracted at intervals depending on the catalytic zones (higher extraction rates in the downstream zones in the direction of feed flow). [0032]
  • It is also possible to carry out more frequent catalyst extraction in the [0033] downstream zone 3 c than in zone 3 b and/or in zone 3 b than in zone 3 a. It is also possible to modulate the frequency and quantities of catalyst extracted.
  • Finally, it is possible to carry out limited extraction of the used catalyst (for example 10% to 33% by volume of each bed) or to renew the entire volume of an individual bed (or zone): [0034] 3 a, 3 b or 3 c. In this case, the catalyst in zone 3 c is preferably renewed more frequently than that in zone 3 a.
  • The reactors of the invention can contain 2 to about 20 catalytic zones separated by heat exchange zones. [0035]
  • The reaction fluid can also be introduced laterally and flow horizontally, as a crosswise current with the feed. [0036]
  • It is possible to use thin beds, for example 5 to 10 cm thick, or of medium thickness, for example between 10 and 80 cm, and if the process demands it, low or high space velocities (for example 10 to 250 h[0037] −1). The temperatures depend on the process but are frequently in the range 250° C. to 950° C., preferably between about 400° C. and about 700° C. These values do not limit the invention.
  • The scope of the invention also encompasses the case wherein there is but a single catalytic bed, or beds in parallel, with a crosswise feed/catalyst flow. [0038]
  • The reactor of the invention can carry out chemical conversion of a feed in the presence of a catalyst while providing each of the catalytic zones with the necessary amount of heat. It also enables the at least partially deactivated catalyst to be extracted in a differentiated manner. [0039]
  • The reactor of the invention can maintain a high catalytic activity and/or productivity for the desired product. [0040]
  • The invention can in particular be employed for hydrocarbon reforming, for dehydrogenating ethylbenzene, and for dehydrogenating paraffins such as propane, n-butane, isobutane, primarily linear paraffins containing 10 to 14 carbon atoms, and for the production of olefins for the production of alkylbenzenes, or for other chemical reactions. [0041]

Claims (7)

1. A chemical conversion reactor, containing a substantially vertical catalytic bed between an upper end and a lower end, and comprising in combination:
close to the upper end of said reactor, at least one means for introducing a solid catalyst;
means for introducing and evacuating said feed allowing its flow in a substantially horizontal direction through the catalytic bed;
means for heating said feed integrated into said reactor;
characterised in that said reactor comprises, close to its lower end, at least one means for extraction of the catalyst, which extraction is differentiated between an upstream portion and a downstream portion of said catalytic bed, with respect to the direction of flow of said feed.
2. A reactor according to claim 1, in which the means for differentiated catalyst extraction is selected from the group formed by continuous and discontinuous extraction means
3. A reactor according to claim 1 or claim 2, in which the catalytic bed comprises a plurality of catalytic zones separated by non-catalytic zones for heating the feed.
4. A reactor according to any one of claims 1 to 3, in which the most upstream catalyst extraction means differs from the most downstream extraction means in its lower extraction capacity.
5. A process for chemical conversion of a feed using a reactor according to any one of claims 1 to 4.
6. A chemical conversion process according to claim 5, in which the feed is a hydrocarbon feed.
7. A chemical conversion process according to claim 5 or claim 6, in which catalytic dehydrogenation of a paraffinic hydrocarbon feed is carried out.
US10/432,773 2000-11-29 2001-11-07 Reactor for chemical conversion of a feedstock with heat inputs and feedstock/catalyst cross-circulation Abandoned US20040067174A1 (en)

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FR0015426A FR2817172B1 (en) 2000-11-29 2000-11-29 CHEMICAL CONVERSION REACTOR OF A LOAD WITH HEAT SUPPLIES AND CROSS CIRCULATION OF THE LOAD AND A CATALYST
FR00/15426 2000-11-29
PCT/FR2001/003458 WO2002043851A1 (en) 2000-11-29 2001-11-07 Reactor for chemical conversion of a feedstock with heat inputs and feedstock/catalyst cross-circulation

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DE (1) DE60110625T2 (en)
ES (1) ES2242790T3 (en)
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Cited By (2)

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WO2006034551A1 (en) * 2004-09-28 2006-04-06 The University Of Queensland Magnetic field dosimeter
KR20210073562A (en) * 2018-10-15 2021-06-18 유오피 엘엘씨 Dehydrogenation method with improved uptime

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AU2009303608B2 (en) * 2008-10-13 2013-11-14 Shell Internationale Research Maatschappij B.V. Using self-regulating nuclear reactors in treating a subsurface formation
JP6327888B2 (en) * 2013-03-07 2018-05-23 新日鐵住金株式会社 Hydrogen gas production apparatus and hydrogen gas production method from coal dry distillation gas
KR101831507B1 (en) * 2016-01-05 2018-04-05 주식회사 효성 Self heat supply dehydrogenation reactor for inducing isothermal reaction
KR101815750B1 (en) * 2016-01-29 2018-01-31 주식회사 효성 Moving bed reactor for dehydrogenation process

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US2534859A (en) * 1946-04-18 1950-12-19 Socony Vacuum Oil Co Inc Method and apparatus for hydrocarbon conversion
US2865848A (en) * 1952-09-24 1958-12-23 Socony Mobil Oil Co Inc Temperature control in hydrocarbon conversion processes
US4525482A (en) * 1983-03-23 1985-06-25 Toyo Engineering Corporation Process for producing a gas containing methane
US4622210A (en) * 1984-08-13 1986-11-11 Standard Oil Company (Indiana) Sulfur oxide and particulate removal system
US5525311A (en) * 1994-05-02 1996-06-11 Uop Process and apparatus for controlling reaction temperatures
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Publication number Priority date Publication date Assignee Title
WO2006034551A1 (en) * 2004-09-28 2006-04-06 The University Of Queensland Magnetic field dosimeter
KR20210073562A (en) * 2018-10-15 2021-06-18 유오피 엘엘씨 Dehydrogenation method with improved uptime
KR102533922B1 (en) * 2018-10-15 2023-05-17 유오피 엘엘씨 Dehydrogenation method with improved run-time

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CA2430246A1 (en) 2002-06-06
US7357855B2 (en) 2008-04-15
JP2010051960A (en) 2010-03-11
EP1339483B1 (en) 2005-05-04
JP2004531361A (en) 2004-10-14
MXPA03004591A (en) 2004-05-05
JP4875283B2 (en) 2012-02-15
EP1339483A1 (en) 2003-09-03
CA2430246C (en) 2009-10-13
WO2002043851A1 (en) 2002-06-06
FR2817172A1 (en) 2002-05-31
ES2242790T3 (en) 2005-11-16
DE60110625T2 (en) 2005-11-10
US20060216218A1 (en) 2006-09-28
FR2817172B1 (en) 2003-09-26

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