Europaisches Patentamt

(19) European Patent Office

Office europeen
peen des brevets
brevets EP 0 810 985 B1

(12) E U R O P E A N PATENT S P E C I F I C A T I O N

(45) Date of publication and mention (51) intci.6: C07C 17/156, C07C 1 9 / 0 4 5
of the grant of the patent:
08.12.1999 Bulletin 1999/49 (86) International application number:
PCT/IB96/00159
(21) Application number: 96902403.3
(87) International publication number:
(22) Date of filing: 01.02.1996 WO 96/26171 (29.08.1996 Gazette 1996/39)

(54) OXYCHLORINATION OF ETHYLENE IN TWO STAGE FIXED-BED REACTOR

OXYCHLORIERUNG VON ETHYLEN IN EINEM ZWEISTUFIGEN FESTBETT REAKTOR
OXYCHLORATION D'ETHYLENE EN REACTEUR A LIT FIXE ET A DEUX ETAGES

(84) Designated Contracting States: • FATUTTO, Pierluigi

BE GB ITSE 1-30171 Mestre(IT)
• MARSELLA, Andrea
(30) Priority: 22.02.1995 GB 9503541 1-31038 Paese (IT)
11.04.1995 GB 9507480
(74) Representative: Votier, Sidney David
(43) Date of publication of application: CARPMAELS & RANSFORD
10.12.1997 Bulletin 1997/50 43, Bloomsbury Square
London WC1A2RA (GB)
(73) Proprietor: EVC TECHNOLOGY AG
6300 Zug (CH) (56) References cited:
EP-A-0 146 925 DE-A- 1 493 213
(72) Inventors: FR-A- 1 563 882 FR-A- 2 318 135
• CARMELLO, Diego GB-A- 1 218 413
1-31021 Mogliano Veneto (IT)

DO
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00
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00 Note: Within nine months from the publication of the mention of the grant of the European patent, any person may give
notice to the European Patent Office of opposition to the European patent granted. Notice of opposition shall be filed in
o
a written reasoned statement. It shall not be deemed to have been filed until the opposition fee has been paid. (Art.
a.
99(1) European Patent Convention).
LU
Printed byJouve, 75001 PARIS(FR)
 1 EP 0 810 985 B1
Description
[0001] The present invention relates to the oxychlo-
rination of ethylene in a fixed bed reactor system to pro-
duce chlorinated hydrocarbons, particularly 1, 2-dichlo- 5
roethane (EDC).
[0002] It is well known that hydrocarbons such as eth-
ylene may be chlorinated by reacting them with hydro-
gen chloride and gases containing elemental oxygen,
particularly air or oxygen enriched air, in the presence 10
of a catalyst at elevated temperatures and pressures in
order to produce chlorinated hydrocarbons such as
EDC. The reaction may be carried out with two different
reactor technologies. The first is fluid bed reactor tech-
nology wherein a gaseous mixture of reactants is con- is
tacted with a fluidizable catalyst powder. The second is
fixed bed reactor technology, in which the gaseous re-
actants flow over a fixed catalyst inside the reactor.
[0003] Fluid bed reactors have a number of draw-
backs, such as potential stickiness of the catalyst pow- 20
der, unsteady operation, poor selectivity owing to the
gas and catalyst solids back mixing in the reactor, loss
of heat transfer owing to fouling of the cooler bundle and
limits in reagent velocity imposed by the need to avoid
catalyst loss by elutriation from the reactor.
[0004] Fixed bed reactor technology has been devel-
oped in order to overcome these problems (see US pat-
ent 3,892,816 and US patent 4,123,467).
[0005] Although the fixed bed reactor overcomes
many of the problems incurred with the fluid bed reactor so
system, a number of new problems have been encoun-
tered. A major problem is the difficulty, in the fixed bed
reactor, of transferring the heat developed by the exo-
thermic oxychlorination reaction away from the reactor
to prevent overheating. For this reason, all the neces- 35
sary reagents may not be fed in the correct stoichiomet-
ric ratio to the reactor. Moreover, because it can be un-
safe to have an oxygen concentration of above 8% in
the mixture feedingthe reactor, forflammability reasons,
the reaction is carried out in two or more subsequent 40
stages (usually three) such that the ethylene is intro-
duced into the first reactor while the HCI and oxygen
feeds are split between the reactors. Unreacted ethyl-
ene plus some inert gases are recycled back to the first
reactor.
[0006] In a further attempt to reduce the incidence of
hot spots and the like, it is known to alter the activity
profile of the catalyst within a fixed bed reactor such that
the activity increases in the direction of flow. For exam-
ple, see European patent application 0146925. Howev- so
er, in the prior art, even when a profiled catalyst is used
it has been deemed necessary to use a multi-reactor
system.
[0007] The three-reactor systems of the prior art have
a number of disadvantages. For example, because the 55
contact time decreases from the first to the third stage,
the partial pressure of the reagents is also decreased.
This means that the three reactors have to be operated
2
2
at different temperatures, requiring separate cooling
jackets. Moreover, in spite of these precautions, the pro-
ductivity of each reactor is different. This is particularly
notable in the third reactor, where productivity is about
50% of that in the first reactor.
[0008] Furthermore, as a result of the high pressure
drop which occurs across the whole catalytic bed sys-
tem in three reactors, the recycling of vent gases neces-
sitates an elevated energy consumption.
[0009] Moreover, it is self-evident that setting up and
maintaining a three reactor system is more costly that a
system involving a single or twin reactors.
[001 0] We have now developed a new process for the
catalytic oxychlorination of ethylene which makes use
of a twin reactor system. Owing to a particular catalytic
loading scheme, the same EDC productivity as a three
reactor system can be maintained, which means that to-
tal productivity, with respect to the volume of catalysis
involved, is 50% greater than that achievable in a three
reactor system.
[0011] According to a first aspect of the invention, we
provide a method for the oxychlorination of ethylene to
produce 1,2-dichloroethane (EDC), comprising reacting
ethylene, a chlorine source and an oxygen source in a
25 fixed-bed oxychlorination reactor in the presence of a
catalyst, characterised in that a two reactor system is
used and the catalyst is a cupric chloride catalyst whose
activity profile is arranged such that the reagent flow first
comes into contact with a first layer of high activity cat-
alyst, subsequently a second layer of low activity cata-
lyst and finally a third layer of high activity catalyst.
[0012] Preferably, the third layer of catalyst is a pro-
filed catalyst and comprises multiple catalyst layers ar-
ranged in order of increasing activity.
[001 3] Preferably, the catalyst loading pattern accord-
ing to the invention is applied to both reactors in the two
reactor system.
[0014] The catalyst loading pattern according to the
invention allows the reaction to start quickly as the rea-
gents come into contact with the first, highly active cat-
alyst layer. Before the temperature of the reacting rea-
gents exceeds 270 to 285°C, the reagents flow into con-
tact with the lower activity catalyst layer, thus decreasing
the rate and therefore the temperature of the reaction.
45 Advantageously, therefore, the first, highly active cata-
lyst layer is short. In any case, the ideal length of the
catalyst layer may be determined empirically, by deter-
mining the maximum length of catalyst layer which may
be used without the reaction exceeding 285°C.
[0015] The second, lower activity catalyst layer is ar-
ranged such that the reaction, which has been initiated
at a high rate by the first catalyst layer, is not allowed to
exceed a hotspot temperature of 285°C.
[0016] The third, high activity catalyst layer is ar-
ranged such that the maximum conversion of reagents
is achieved, without exceeding 285°C. Advantageously,
the third catalyst layer is a profiled catalyst layer wherein
the activity increases in the direction of reagent flow.
 3 EP 0 810 985 B1
[0017] The choice of suitable specific catalyst loading
patterns will depend on the maximum forecast temper-
ature of the hotspot, and on the inside diameter and
length of the reactor being used, as well as the through-
put of reagents.
[0018] Catalysts of varying known activities for use in
the method of the invention are known in the art. Pref-
erably, the catalysts are supported catalysts with cupric
chloride as the active component and alumina, silica gel
or aluminosilicates as supports. The support material
may be in the form of the spheres, cubes, cones, hollow
cylinders, cylindrical pellets, multilobate pellets and the
like.
[0019] The copper content of the catalyst preferably
varies in accordance with the required activity, such that
the first, active catalyst layer has a high copper content,
the second, lower activity catalyst layer has a lower cop-
per content, and the third, high activity layer has a high
copper content. Where the third catalyst is a profiled cat-
alyst, the copper content of the catalyst may be similarly
profiled.
[0020] In addition to the cupric chloride active compo-
nent, the catalyst may also comprise promoters such as
the chlorides of potassium, magnesium, cesium, lithium,
sodium, calcium and cerium for improving the selectivity
to EDC.
[0021 ] The reactor type employed in the method of the
invention is a tubular reactor. Advantageously, it con-
sists of a plurality of tubes stacked together within a sin-
gle coolant jacket. The internal diameter of each tube is
preferably between 15 and 40 millimetres. Diameters of
less than 15 millimetres are disadvantageous as an ex-
cessive number of tubes is required in an industrial re-
actor in order to obtain a satisfactory throughput of ma-
terials, while diameters larger than 40 millimetres result
in excessively high hotspot temperatures inside the cat-
alytic bed, requiring a low specific throughput in order
to keep the temperatures low. A diameter of 20 to 30mm
is preferred.
[0022] The preferred length of the reactor is between
3 and 9 metres. A length of less than 3 metres results
in too short a residence time and therefore either low
reactant conversion or low specific throughput; a length
of more than 9 metres is not necessary in order to
achieve both high HCI and oxygen conversion and large
specific throughput. A length of 3.5-7m is preferred.
[0023] Preferably, all of the ethylene is fed intothefirst
reactor, together with from 40 to 100% of the chlorine
source. Preferably, the chlorine source is a HCI.
[0024] The oxygen source is preferably pure oxygen
and the volume of pure oxygen fed to the first reactor is
preferably between 2 and 6% by volume of the total fed
product in the first reactor, corresponding to between 40
and 60% of the total oxygen fed to the reaction.
[0025] In the second reactor, as a different reagent
mixture is used which has higher flammability limits, the
oxygen concentration may be increased to between 7
and 10% without hazard. The oxygen excess with re-
4
spect to the stoichiometric requirement in relation to the
chlorine source will range from 0 to 15%.
[0026] Preferably, unreacted gasses are recycled
from the second reactor back to the first reactor. The
5 composition of the recycled gas, which may include
some or all of the unreacted ethylene recovered after
standard cooling and condensation procedures, will
reach an equilibrium depending on combustion rate,
amounts of inert gases in the raw materials and the
10 purge rate. Ethylene concentration can accordingly vary
from 10% to nearly 90%. As a consequence, the excess
of ethylene in the reaction depends on the ethylene con-
centration in the recycle vent gas and on the recycle flow
rate.
is [0027] Where at least some of the vented ethylene,
or other gases, are not recycled, they may be used in
other processes, such as direct chlorination.
[0028] The recycle flow rate may be adjusted in order
to control oxygen concentration at the inlet of the first
20 reactor, thus controlling the hotspot temperature.
[0029] The hotspot temperature itself depends on
several parameters. Typically, hotspot temperatures of
between 230 and 260°C are preferred for a tubular re-
actor with an inside diameter of 27 millimetres, and 250
25 to 275°C for a tubular reactor with an inside diameter of
32 millimetres.
[0030] Preferably, reactants are preheated up to be-
tween 100-200°C. The pressure of the reaction can
range up to 20 barg, the preferred pressure in being be-
so tween 4 and 7 barg.
[0031] The performance of the two stage process is
excellent. HCI conversion is typically above 98% even
with very low oxygen excess and conversion beyond
99% can easily be achieved with an oxygen excess of
35 10% in the second stage. The selectivity of the reaction,
moreover, is high. The burning rate is low, less than 1%
of the ethylene being converted to carbon monoxide and
carbon dioxide. Byproducts such as ethyl chloride
amount to approximately 1500 to 3000 ppm in the EDC
40 produced.
[0032] The invention will now be described, for the
purpose of illustration only, in the following examples.
Figure 1 shows a schematic diagram of a two reactor
system according to the invention.
45
COMPARATIVE EXAMPLE 1
[0033] The reactors were three units composed of
313mm (1.25 inch) o.d. nickel tube, 14 BWG, 14 feet
so
50 long; inside each tube, on axis, there was a thermowell
of 6mm o.d. containing 4 sliding thermocouples with
which it was possible to record the thermal profile of the
reactor. The reactor was surrounded with an external
jacket in which steam at 210°C and 18 barg was used
55 to control the temperature of the reaction. The reactor
pressure was controlled with a pneumatic valve on an
effluent line.
[0034] The reagents were preheated in 18 barg steam
3
 5 EP 0 810 985 B1 6

heated exchangers. Ethylene, HCI and nitrogen were first reactor was 5.9% (-4.5% with respect to stoichio-
mixed together and oxygen was added to the mixture in metric); at the inlet of the second reactor the oxygen
a special mixer where the velocity of the gases was high- concentration was 6.05% (+4.22% with respect to stoi-
er than the eventual ethylene flame propagation veloc- chiometric).
ity. The catalyst used was a normal industrial catalyst 5 The results were:
for a three stage fixed bed process consisting of hollow
cylinders containing copper and potassium chloride ar- Oxygen conversion to crude EDC 96.00%
ranged as follows: HCI conversion to crude EDC 98.20%
[0035] In the first reactor, 60% of the volume was filled EDC production 84.15 moles/h
with a catalytic bed containing Cu 3.2%w/w, K 1.3%w/
w and Cs 1.4%w/w. The other 40% was filled with a cat-
alytic bed containing Cu 5.5%w/w, K 1.8%w/w and Cs Hotspot 1° 316°C
2.0%w/w. In the second reactor 60% of the volume was 2° 313°C
filled with a catalyst containing Cu 3.7%w/w, K 1.4%w/ Pressure drop 1.2 bar
w, 20% of the volume filled with a catalyst containing Cu
6%w/w, K 1%w/w and the last 20% filled with a catalyst
As we can see the hotspot temperature was too high.
containing Cu 7%w/w, K 1%w/w. The third reactor had
only one type of catalyst containing Cu 7%w/w, K 1%w/
COMPARATIVE EXAMPLE 3
w.
[0036] The first reactor was fed a mixture of 212 20
moles/h of ethylene, 85.7 moles/h of HCI, 17.5 moles/h [0039] The reaction was carried out with the same
conditions as Example 2 but with a loading pattern ar-
of oxygen and 31 moles/h of nitrogen. The second re-
ranged to lower the hotspot up to 270°C. In this case
actor was fed 85.7 moles/h of HCI and 17.5 moles of
the catalyst activity was profiled to increase from top to
oxygen. The third reactor was fed 8.75 moles/h of oxy- the bottom, in the direction of reagent flow. The loading
gen. At the inlet of the first reactor the oxygen concen- 25
tration was 5% (-18% with respect to stoichiometric); at pattern was:
the inlet of the second reactor, the oxygen concentration
First reactor: 7% graphite; 48% of a catalyst con-
was 4.6% (-30 % with respect to stoichiometric); at the
taining Cu 2.7w/w, K 0.8%w/w, Cs 1%w/w; 23% of
inlet of the third reactor the oxygen concentration was
a catalyst containing Cu 3.3w/w K 1.1%w/w; and
3% (+9.6% with respect to stoichiometric). The overall
22% of a catalyst containing Cu 7.8%w/w, K0.8%w/
oxygen excess was 2.1%. The inlet pressure of the first
w.
reactor was 6.3 bar and the outlet pressure at the third
reactor was 4.25 bar. The temperature of the cooling
Second reactor: 7% graphite; 42% of a catalyst con-
jacket was held at 210°C.
taining Cu 2.7%w/w, K 0.9%w/w; 30% of a catalyst
[0037] The outlet stream, consisting of a mixture of
containing Cu 5.5%w/w, K 0.6%w/w; and 21% of a
ethylene, oxygen, HCI, EDC, water, COx and byprod-
catalyst containing Cu 7.8%w/w, K 0.8%w/w.
ucts, was analyzed and the overall results were:
[0040] The oxygen concentration at the inlet of the re-
Oxygen conversion to crude EDC 97.70%
actors was the same as in Example 2.
HCI conversion to crude EDC 99.70%
The results were:
EDC production 85.55 moles/h
EDC production 82.50 moles/h
HCI conversion 96.23%
Hotspot 1° 272 C°
Oxygen conversion 94.08%
2° 264 C° 45
3° 255 C°
Pressure drop0 2.05 bar Hotspots1° 275°C
2° 275°C
COMPARATIVE EXAMPLE 2 50 Pressure drop 1.25 bar

[0038] This example was carried out with only two re- [0041] In this case the hot spot temperature was ac-
actors and with a catalytic loading scheme as in reactors
ceptable but the conversions of the oxygen and HCI
1 and 2 of Example 1. A mixture of ethylene (212 moles/
were too low.
h), (HCI 85.7 moles/h), oxygen (20.5 moles/h) and 31 55
moles of nitrogen was fed to the first stage. In the second EXAMPLE 4
stage, 85.7 moles/h of HCI and 23.25 moles/h of oxygen
were fed. The oxygen concentration at the inlet of the [0042] This Example was carried out with the same

4
 7 EP 0 810 985 B1 8

reactors and the same amount of reagents as in Exam- (continued)

ple 2 but with the following catalytic scheme:
First reactor: The loading pattern was: 7% graphite;
3% of a catalyst containing Cu 6.5%w/w, K 2.2%w/
w; 40% of a catalyst containing Cu 2.7%w/w, K
0.8%w/w; 22% of a catalyst containing Cu 3.75%w/
w, K 1.2%w/w; and 28%w/w of a catalyst containing
Cu 7.8%w/w, K 0.8%w/w.
10
Second reactor: The loading pattern was: 3% of a
catalyst containing Cu 6.5%w/w, K 2.2%w/w; 31%
of a catalyst containing Cu 2.9%w/w, K 1.2%w/w;
18% of a catalyst containing Cu 3.9%w/w, K 1.3%w/
w; and 48% of a catalyst containing Cu 7.8%w/w, K 15
0.8%w/w.
[0043] The results were:
Oxygen conversion to crude EDC 96.80% 20
HCI conversion to crude EDC 99.00%
EDC production 85.00 moles/h
2° 268°C
Pressure drop 1.25 bar
[0047] Conversions and hotspots were good. Note
the lowering of the pressure drop using the two stage
system.
Claims
1. A method for the oxychlorination of ethylene to pro-
duce 1,2-dichloroethane (EDC), comprising react-
ing ethylene, a chlorine source and an oxygen
source in a fixed-bed oxychlorination reactor in the
presence of a catalyst, characterised in that a two
reactor system is used and the catalyst is a cupric
chloride catalyst whose activity profile is arranged
such that the reagent flow first comes into contact
with a first layer of high activity catalyst, subse-
quently a second layer of low activity catalyst and
finally a third layer of high activity catalyst.

Hotspots 1°after 2. 1m 270°C 25 2. A method according to claim 1 wherein the third cat-
2° " " 272° C alyst layer is a profiled catalyst comprising multiple
Pressure drop 1.25 bar catalyst layers wherein the activity increases in the
direction of reagent flow.

[0044] Conversion and hotspots were good. 30 3. A method according to claim 1 or claim 2 wherein
the activity of the catalyst is profiled in each of the
EXAMPLE 5 two reactors.

[0045] This example was carried out with the same
apparatus and throughput in Example 3 but with the fol-
lowing loading scheme.
First reactor: 7% graphite, 3% of a catalyst contain-
ing Cu 6.5%w/w, K2.2%w/w; 45% of a catalyst con-
taining Cu 2.7% w/w, K 0.8%w/w; 28% of a catalyst
containing Cu 3.75%w/w, K 1.2%w/w; and 22% of
a catalyst containing Cu 7.8%w/w, K 0.8%w/w.
Second reactor: 3% of a catalyst containing Cu
6.5%w/w, K 2.2%w/w; 31% of a catalyst containing
Cu 2. 9% w/w, K 1.2%w/w; 20% of a catalyst contain-
ing Cu 3.9%w/w, K 1.3%w/w and 46% of a catalyst
containing Cu 7.8%w/w.
[0046] The results were:
Oxygen conversion to crude EDC 96.50%
HCI conversion to crude EDC 98.70%
EDC production 84.75 moles/h
Hotspot 1° 270°C
4. A method according to any preceding claim wherein
35 the temperature of the reaction does not exceed
285°C.
5. A method according to any preceding claim wherein
the catalyst also comprises promoters such as the
40 chlorides of potassium, magnesium, cesium, lithi-
um, sodium, calcium and cerium.
6. A method according to any preceding claim wherein
between 40 and 60% of the total oxygen source fed
45 to the reaction is fed to the first reactor.
7. A method according to any preceding claim wherein
between 40 and 100% of the total chlorine source
fed to the reaction is fed to the first reactor.
50
8. A method according to any preceding claim wherein
exhaust gases vented from the second reactor are
recycled, at least in part, to the first reactor.
55 9. A method according to any preceding claim wherein
the reaction proceeds at a pressure between 4 and
7 barg.

5
 9 EP 0 810 985 B1
Patentanspriiche
1. Verfahren fur die Oxychlorierung von Ethylen zur
Herstellung von 1,2-Dichlorethan (EDC), umfas-
send reagierendes Ethylen, eine Chlorquelle und
eine Sauerstoffquelle in einem Oxychlorierungs-
Festbettreaktor in Gegenwart eines Katalysators;
dadurch gekennzeichnet, dal3 ein System mit zwei
Reaktoren verwendet wird und dal3 der Katalysator
ein Kupfer(ll)-chlorid-Katalysator ist, dessen Aktivi-
tatsprofil so eingerichtet ist, dal3 der Reagenzstrom
zuerst mit einer ersten Schicht eines Katalysators
mit hoher Aktivitat, danach mit einer zweiten
Schicht eines Katalysators mit niedriger Aktivitat
und zum SchluB mit einer dritten Schicht eines Ka-
talysators mit hoher Aktivitat in Kontakt gerat.
2. Verfahren gemaB Anspruch 1, wobei die dritte Ka- 2.
talysatorschicht ein profilierter Katalysator umfas-
send mehrere Katalysatorschichten ist, wobei die 20
Aktivitat in Richtung des Reagenzstroms ansteigt.
3. Verfahren gemaB Anspruch 1 oder Anspruch 2, wo-
bei die Aktivitat des Katalysators in jedem der zwei
Reaktoren profiliert ist.
4. Verfahren gemaB irgendeinem der vorangehenden
Anspruche, wobei die Temperatur der Reaktion
285°C nicht ubersteigt.
5. Verfahren gemaB irgendeinem der vorangehenden
Anspruche, wobei der Katalysator auBerdem Pro-
motoren wie die Chloride von Kalium, Magnesium,
Casium, Lithium, Natrium, Kalzium und Cerium ent-
halt.
6. Verfahren gemaB irgendeinem der vorangehenden
Anspruche, wobei zwischen 40 und 60% der ge-
samten der Reaktion zugefuhrten Sauerstoffquelle
dem ersten Reaktor zugefuhrt wird.
7. Verfahren gemaB irgendeinem der vorangehenden
Anspruche, wobei zwischen 40 und 100% der ge-
samten der Reaktion zugefuhrten Chlorquelle dem
ersten Reaktor zugefuhrt wird.
8. Verfahren gemaB irgendeinem der vorangehenden
Anspruche, wobei die vom zweiten Reaktor abge-
zogenen Abgase zumindest teilweise zum ersten
Reaktor zuruckgeleitet werden.
9. Verfahren gemaB irgendeinem der vorangehenden
Anspruche, wobei die Reaktion bei einem Druck
zwischen 4 und 7 Bar ablauft.
10
Revendications
1. Procede pour I'oxychloration d'ethylene afin de pro-
duire du 1,2-dichlorethane (EDC), comprenant les
5 operations consistant a faire reagir de I'ethylene,
une source de chlore et une source d'oxygene dans
un reacteur d'oxychloration a lit fixe en presence
d'un catalyseur, caracterise en ce qu'on utilise un
systeme a deux reacteurs et le catalyseur est un
10 catalyseur de chlorure cuprique dont le profil d'ac-
tivite est amenage de telle sorte que le flux de reac-
tifs vienne d'abord en contact avec une premiere
couche d'un catalyseur a activite elevee, puis avec
une deuxieme couche d'un catalyseur a faible acti-
os vite et enfin avec une troisieme couche d'un cata-
lyseur a activite elevee.
Procede selon la revendication 1, dans lequel la
troisieme couche de catalyseur est un catalyseur
profile comprenant des couches catalytiques multi-
ples dans lesquelles I'activite augmente dans la di-
rection d'ecoulement des reactifs.
3. Procede selon la revendication 1 ou 2, dans lequel
25 I'activite du catalyseur est profilee dans chacun des
deux reacteurs.
4. Procede selon I'une quelconque des revendications
precedentes, dans lequel la temperature de la reac-
30 tion ne depasse pas 285°C.
5. Procede selon I'une quelconque des revendications
precedentes, dans lequel le catalyseur comprend
egalement des promoteurs tels que les chlorures
35 de potassium, de magnesium, de cesium, de li-
thium, de sodium, de calcium et de cerium.
6. Procede selon I'une quelconque des revendications
precedentes, dans lequel entre 40% et 60% de la
40 source d'oxygene totale acheminee a la reaction
sont achemines au premier reacteur.
7. Procede selon I'une quelconque des revendications
precedentes, dans lequel entre 40% et 100% de la
45 source de chlore totale acheminee a la reaction
sont achemines au premier reacteur.
8. Procede selon I'une quelconque des revendications
precedentes, dans lequel les gaz d'echappement
so echappees du second reacteur sont recycles, au
moins en partie, au premier reacteur.
9. Procede selon I'une quelconque des revendications
precedentes, dans lequel la reaction se fait a une
55 pression comprise entre 4 et 7 bars manometri-
ques.
6
 3

r-

r-