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GB2034293A - Recovery of Ammonia - Google Patents

Recovery of Ammonia Download PDF

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Publication number
GB2034293A
GB2034293A GB7936522A GB7936522A GB2034293A GB 2034293 A GB2034293 A GB 2034293A GB 7936522 A GB7936522 A GB 7936522A GB 7936522 A GB7936522 A GB 7936522A GB 2034293 A GB2034293 A GB 2034293A
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United Kingdom
Prior art keywords
range
surface area
process according
ammonia
weight
Prior art date
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Granted
Application number
GB7936522A
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GB2034293B (en
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BP PLC
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BP PLC
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Publication date
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Priority to GB7936522A priority Critical patent/GB2034293B/en
Publication of GB2034293A publication Critical patent/GB2034293A/en
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Publication of GB2034293B publication Critical patent/GB2034293B/en
Expired legal-status Critical Current

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    • BPERFORMING OPERATIONS; TRANSPORTING
    • B01PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01JCHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J35/00Catalysts, in general, characterised by their form or physical properties
    • B01J35/60Catalysts, in general, characterised by their form or physical properties characterised by their surface properties or porosity
    • BPERFORMING OPERATIONS; TRANSPORTING
    • B01PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01JCHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J21/00Catalysts comprising the elements, oxides, or hydroxides of magnesium, boron, aluminium, carbon, silicon, titanium, zirconium, or hafnium
    • B01J21/18Carbon
    • CCHEMISTRY; METALLURGY
    • C01INORGANIC CHEMISTRY
    • C01CAMMONIA; CYANOGEN; COMPOUNDS THEREOF
    • C01C1/00Ammonia; Compounds thereof
    • C01C1/02Preparation, purification or separation of ammonia
    • C01C1/04Preparation of ammonia by synthesis in the gas phase
    • C01C1/0405Preparation of ammonia by synthesis in the gas phase from N2 and H2 in presence of a catalyst
    • C01C1/0411Preparation of ammonia by synthesis in the gas phase from N2 and H2 in presence of a catalyst characterised by the catalyst
    • CCHEMISTRY; METALLURGY
    • C01INORGANIC CHEMISTRY
    • C01CAMMONIA; CYANOGEN; COMPOUNDS THEREOF
    • C01C1/00Ammonia; Compounds thereof
    • C01C1/02Preparation, purification or separation of ammonia
    • C01C1/04Preparation of ammonia by synthesis in the gas phase
    • C01C1/0405Preparation of ammonia by synthesis in the gas phase from N2 and H2 in presence of a catalyst
    • C01C1/0458Separation of NH3
    • C01C1/0464Separation of NH3 by absorption in liquids, e.g. water
    • BPERFORMING OPERATIONS; TRANSPORTING
    • B01PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01JCHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J35/00Catalysts, in general, characterised by their form or physical properties
    • B01J35/60Catalysts, in general, characterised by their form or physical properties characterised by their surface properties or porosity
    • B01J35/61Surface area
    • B01J35/615100-500 m2/g
    • YGENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02PCLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
    • Y02P20/00Technologies relating to chemical industry
    • Y02P20/50Improvements relating to the production of bulk chemicals
    • Y02P20/52Improvements relating to the production of bulk chemicals using catalysts, e.g. selective catalysts

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  • Chemical & Material Sciences (AREA)
  • Organic Chemistry (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Engineering & Computer Science (AREA)
  • Materials Engineering (AREA)
  • Analytical Chemistry (AREA)
  • Inorganic Chemistry (AREA)
  • Catalysts (AREA)
  • Organic Low-Molecular-Weight Compounds And Preparation Thereof (AREA)

Abstract

A process for the production of ammonia comprises passing hydrogen and nitrogen over a catalyst disclosed in 45711/76 comprising a specified transition metal, e.g., ruthenium, and a modifying metal, e.g., an alkali metal, supported on a graphite-containing carbon support having specified surface area properties, the ammonia being recovered by washing the reaction product with water in an absorber to dissolve the ammonia produced.

Description

SPECIFICATION Process for the Production of Ammonia This invention relates to a process for the production of ammonia.
With increased pressure on the world's food resources the demand for nitrogen-containing fertilisers based on ammonia has grown rapidly in recent years. Current Haber processes using nitrogen and hydrogen as feedstock generally use a potassium promoted iron catalyst, usually with other promoters such as alumina. These catalysts are reduced in situ from bulk iron oxides before use and operate under severe conditions, e.g., pressures of up to 300 bars and temperatures of 4500--5000C.
The reaction N2+3H2=2NH3 is highly exothermic and thus the equilibrium is moved to the right at lower temperatures. However, present day commercial catalysts are not sufficiently active at lower temperatures to enable the reaction to reach equilibrium within the short time the reactants are in contact with the catalyst. Activity increases with temperature and therefore a compromise has to be reached.
Recent work by Aika et al, Journal of Catalysis, 27, 424-431(1972), on the synthesis of ammonia discloses that synthesis over a ruthenium catalyst is promoted by the addition of an alkali metal, particularly when the ruthenium is supported by active carbon or alumina.
Similarly, British Patent Specification 1 367112 to to Sagami Chemical Research Centre discloses a complex catalyst for ammonia synthesis which comprises (a) at least one alkali metal belonging to Group 1 A of the Periodic Table, (b) at least one compound, preferably a halide, oxide or sulphide, of transition metal selected from the group consisting of Group 4B, Group 5B, Group 6B, Group 7B and Group 8 of the Periodic Table and graphite. The Periodic Table referred to by Sagami is that given in the "Handbook of Chemistry", edited by Norbert Adolf Lange; McGraw-Hill, 1961; pages 56 to 57.
The complex comprises an alkali metal as the electron donor, graphite as the electron acceptor and a transition metal compound. The alkali metal and the transition metal compound are present as intercalates in the graphite lattice. Aika and Sagami both disclose the use of free alkali metal or precursors thereof, such as azides, as electron donors.
Our copending British Patent Application No. 45711/76 discloses a catalyst comprising (i) as support a graphite-containing carbon having (a) a basal plane surface area of at least 100 m2/g. (b) a ratio of BET surface area to basal plane surface area of not more than 8:1, preferably not more than 5:1 and (c) a ratio of basal plane surface area to edge surface area of at least 2:1 and preferably at least 5::1 and (ii) as active component (a) 0.1 to 50%, preferably 130%, most preferably 510%, by weight of a transition metal of the 4th, 5th and 6th horizontal Periods of Groups VB, VIB, VIIB and VIII of the Periodic Table expressed as % by weight of total catalyst and (b) 0.1 to 4 times by weight of (a) of a modifying metal ion selected from Groups IA or IIA of the Periodic Table or the lanthanides or actinides, the modifying metal ion being actively associated with the transition metal rather than the support.
Unless otherwise indicated the Periodic Table referred to in the present specification is the Periodic Table published on page B-4 of the Handbook of Chemistry and Physics, 57th Edition, 1 976- 1977, published by CRC Press, Cleveland, Ohio.
Such a catalyst is suitable for the production of ammonia from hydrogen and nitrogen.
It is distinguished from the prior art in that it is neither an electron donor-acceptor complex nor is it an intercalate compound.
Ammonia is at present recovered cryogenically from current processes and the cost of refrigeration represents a considerable proportion of total cost. Furthermore, recovery by this method is incomplete since a proportion of the ammonia remains in the vapour form arid is recycled together with unconverted hydrogen and nitrogen. This, of course, reduces the conversion per pass of the reactor.
We have now discovered that because of the relatively high tolerance of the catalyst described in British Patent Application No. 45711/76 to water, ammonia can be recovered economically by washing the reaction product with water.
Thus according to the present invention there is provided a process for the production of ammonia which process comprises passing a feedstock containing hydrogen and nitrogen over a catalyst comprising (i) as support a graphite-containing carbon having (a) a basal plane surface area of at least 100 m2/g, (b) a ratio of BET surface area to basal plane surface area of not more than 8:1, preferably not more than 5:1, and (c) a ratio of basal plane surface area to edge surface area of at least 2:1 and preferably, at least 5::1, and (ii) as active component (a) 0.1 to 50% preferably 130%, most preferably 510%, by weight of a transition metal of the 4th, 5th and 6th horizontal Periods of Groups VB, VIB, VIIB and VIII of the Periodic Table, expressed as % by weight of total catalyst, and (b) 0.1 to 4 times by weight of (a) of a modifying metal ion selected from Groups IA or IIA of the Periodic Table or the lanthanides or actinides, the modifying metal ion being actively associated with the transition metal rather than the support, under conditions of temperature, pressure and space velocity such that conversion to ammonia is effected, washing the reaction product with water in an absorber to dissolve the ammonia produced, separating aqueous ammonia from unreacted hydrogen and nitrogen and recycling the unreacted hydrogen and nitrogen to the reactor.
Broad and preferred ranges of process conditions are as follows:- Broad Range Preferred Range Temperature OC 250-600 300-500 Pressure bars Atmospheric-300 20--1 30 Space velocity v/v/hr 1,000-100,000 5,000--30,000 The ammonia is produced in the form of a concentrated solution from which the water may be removed if desired, e.g., in a stripper.
The unconverted hydrogen and nitrogen separated after the water wash are substantially saturated with water vapour. As stated previously, the catalyst has a relatively high tolerance to water vapour but, even so, it may be desirable to remove some of the water vapour from the recycled gases.
This may be done by conventional methods such as drying over a molecular sieve.
It is not, however, necessary to dry the gases as thoroughly as would be the case if they were to be recycled to a process employing a conventional catalyst.
The absorber may be operated under the following conditions provided that there is a minimum ammonia concentration at the absorber inlet of 5% by weight.
Broad Range Preferred Range Pressure bars Atmospheric-300 20-130 Temperature OC 5-55 15 vi 5 Conditions in the stripper are not critical. However, the pressure may be in the range 10-30 bar and the temperature in the range 500--1500C.
The invention is illustrated with reference to the accompanying drawing which is a flow diagram.
Products from a reactor containing ammonia, unreacted nitrogen and hydrogen are supplied by line 1 to absorber 2 in which they are contacted with water supplied by line 3.
In the absorber, ammonia dissolves in the water and the resulting aqueous solution of ammonia is removed by line 4, heated in heat exchanger 5 and passed to a stripper 6. Unreacted nitrogen and hydrogen do not dissolve in the water in the absorber 2 and are removed by line 7 and passed to a molecular sieve drier (not shown) before being recycled to the reactor (not shown).
In the stripper 6, gaseous ammonia is stripped from the aqueous solution and removed from the stripper by line 8. It then passes through a cooler 9 and leaves through line 10 as a gaseous or liquid product. Stripped solvent, i.e., water, leaves the base of the stripper by line 11, passes through heat exchanger 5 where it gives up heat to the feed to the stripper and returns to the absorber by line 3.

Claims (12)

Claims
1. A process for the production of ammonia which process comprises passing a feedstock containing hydrogen and nitrogen over a catalyst comprising (i) as support a graphite-containing carbon having (a) a basal plane surface area of at least 100 m2/g, (b) a ratio of BET surface area to basal plane surface area of not more than 8:1, and (c) a ratio of basal plane surface area to edge surface area of at least 2::1 and (ii) as active component (a) 0.1 to 50% by weight of a transition metal of the 4th, 5th and 6th horizontal Periods of Groups VB, VIIB and VIII of the Periodic Table, expressed as % by weight of total catalyst, and (b) 0.1 to 4 times by weight of (a) of a modifying metal ion selected from Groups IA or IIA of the Periodic Table or the lanthanides or actinides, the modifying metal ion being actively associated with the transition metal rather than the support, under conditions of temperature, pressure and space velocity such that conversion to ammonia is effected, washing the reaction product with water in an absorber to dissolve the ammonia produced, separating aqueous ammonia from unreacted hydrogen and nitrogen and recycling the unreacted hydrogen and nitrogen to the reactor.
2. A process according to Claim 1 wherein the graphite-containing carbon has a ratio of BET surface area to basal plane surface area of not more than 5:1 and a ratio of basal plane surface area to edge surface area of at least 5:1.
3. A process according to either of Claims 1 or 2 wherein the transition metal is present in amount 1 to 30% by weight expressed as % by weight of total catalyst.
4. A process according to any of the preceding claims wherein the transition metal is ruthenium.
5. A process according to any of the preceding claims wherein the modifying metal ions are rubidium or potassium ions.
6. A process according to any of the preceding claims wherein the feedstock is passed over the catalyst at a temperature in the range 2500 to 6000C, a pressure in the range atmospheric to 300 bars and a space velocity in the range 1,000 to 100,000 v/v/hr.
7. A process according to Claim 6 wherein the feedstockis passed over the catalyst at a temperature in the range 3000 to 5000C, a pressure in the range 20 to 200 bars and a space velocity in the range 5,000 to 30,000 v/v/hr.
8. A process according to any of the preceding claims wherein the wash water supplied to the absorber inlet contains a minimum ammonia concentration of 5% by weight and the absorber is operated under a pressure in the range atmospheric to 300 bar and a temperature in the range 50 to 550C.
9. A process according to Claim 8 wherein the absorber is operated under a pressure in the range 20 to 300 bar and a temperature in the range 1 50 to 450C.
1 0. A process according to any of the preceding claims wherein the stripper is operated under a pressure in the range 10 to 30 bar and a temperature in the range 50 to 1 500C.
11. A process as hereinbefore described with reference to the accompanying drawing.
12. Ammonia whenever prepared by a process according to any of the preceding claims.
GB7936522A 1978-10-25 1979-10-22 Recovery of ammonia Expired GB2034293B (en)

Priority Applications (1)

Application Number Priority Date Filing Date Title
GB7936522A GB2034293B (en) 1978-10-25 1979-10-22 Recovery of ammonia

Applications Claiming Priority (2)

Application Number Priority Date Filing Date Title
GB7841923 1978-10-25
GB7936522A GB2034293B (en) 1978-10-25 1979-10-22 Recovery of ammonia

Publications (2)

Publication Number Publication Date
GB2034293A true GB2034293A (en) 1980-06-04
GB2034293B GB2034293B (en) 1982-10-27

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Cited By (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
EP0058531A1 (en) * 1981-02-13 1982-08-25 The British Petroleum Company p.l.c. Process for the production of ammonia

Cited By (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
EP0058531A1 (en) * 1981-02-13 1982-08-25 The British Petroleum Company p.l.c. Process for the production of ammonia

Also Published As

Publication number Publication date
GB2034293B (en) 1982-10-27

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