US 20130015405A1

(19) United States

(12) Patent Application Publication (10) Pub. No.: US 2013/0015405 A1
Quintero et al.

(43) Pub. Date:

(54) ISOTHERMAL REACTOR FOR PARTIAL

(30)

Jan. 17, 2013

Foreign Application Priority Data

OXIDATION OF METHANE
Jan. 7, 2010

(75)

Inventors: Ruben Dario Rodriguez Quintero,

Aberdeen (GB); Ernesto Manuel
Santana Diaz, Aberdeen (GB); James
AndreW Banister, Aberdeen (GB)

(GB) ................................. .. 10001568

PllblicatiOIl ClaSSi?CatiOH

(51) Int- Cl
B01] 8/06
C013 3/38
(52)

(2006-01)
(2006.01)

US. Cl. ...................................... .. 252/373; 422/198

(73) Assignee: GAS2 LIMITED, Aberdeen (GB)

(57)
(21) Appl' N05

13/261,355

(22)

Jan. 7, 2011

(86)

PcT Filed:

ABSTRACT

There is herein described a process and apparatus for partial

oxidation of hydrocarbons. More particularly, there is
described a process and an isothermal reactor apparatus for

PCT No.:

PCT/GB2011/050015

371 (c)(1),
(2), (4) Date:

Sep. 14, 2012

the partial oxidation of methane Which comprises a heat

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transfer surface, a porous catalytic membrane and wherein

heat is disipated and/or removed through the heat transfer

surface.

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US 2013/0015405 A1

ISOTHERMAL REACTOR FOR PARTIAL

OXIDATION OF METHANE
FIELD OF THE INVENTION

[0001]

The present invention relates to a process and appa

ratus for partial oxidation of hydrocarbons. More particularly,

the present invention relates to a process and an isothermal

reactor apparatus for the partial oxidation of methane Which

uses a heat transfer surface.

BACKGROUND OF THE INVENTION

Jan. 17, 2013

With a pre-mixed feed comprising methane and oxygen (gas

molar ratio of 2: 1) the feed is preheated to at least 400 deg C.
such that good selectivity to carbon monoxide is achieved.
The temperature of the gases passing over the catalyst rapidly

rises and under adiabatic conditions (no heat loss) the product
gases leaving the reactor can be in excess of 900 deg C. It is
also bene?cial if the reaction can be performed at elevated
pressure since most of the processes that utilise syngas to
form another chemical do so at raised pressure and the costs

of compressing the component feed streams (comprising

methane and oxygen) is less than compressing the resultant
syngas. This is principally as a result of the increase in gas

[0002] There are three main technologies that are used for
the production of syngas from methane and they are steam

volumes that accompany the reaction. The partial oxidation of

reforming, autothermal reforming and partial oxidation (cata

have similar characteristics in that it is most bene?cially

carried out at elevated temperature and pressure.

lytic and non-catalytic). The most commonly used are auto

methane as described in US. Pat. No. 7,641,888 is found to

thermal and steam reforming or a combination of the tWo.

[0009]

Both these technologies require a large proportion of steam to

reaction in a simple adiabatic reactor is that there is no control

on the temperature of the ?uids Within the reactor and so there
is less ?exibility to operate the reactor at a temperature that is

be included With the methane feed to prevent coke formation

and reforming catalyst deactivation. In order to achieve high

energy ef?ciency the large amount of sensible and latent heat

The draWback of performing the partial oxidation

(>1200 deg C.) create energy e?iciency challenges of their

most bene?cial for maintaining a long catalyst life. With a

typical long contact time reactor this is a straightforWard
problem to solve by an engineer skilled in the art. Placing the
catalyst pellets Within the tube of a shell and tube type reactor
orusing a tube cooled reactors are bothpossibilities. A further
possibility useful in loWer temperature reactor is to operate

oWn.

the reaction in the liquid phase Where the heat capacity of the

contained Within the steam must be recovered and recycled to

the process.

[0003] Non-catalytic partial oxidation does not require the

high levels of steam but the very high process temperatures

[0004]

One more recent, non-commercial technology is the

catalytic partial oxidation of methane using rhodium cata

lysts. Rhodium has been found to be highly selective in the
oxidation With minimal coke formation alloWing the partial
oxidation process to be run at much loWer temperatures. The

liquid is able to absorb the heat of reaction.

[0010] Where a reaction such as the partial oxidation of
methane requires a short contact time at high temperature,
typically using a very shalloW catalyst bed of pellets or gauZe,
then the removal of heat is more problematic. Unusual solu

process doesnt require steam to operate, although small

quantities (10 vol % of the methane feed) are frequently

tions can be found such as in the silver catalysed methanol to

described as a means of increasing the hydrogen to carbon

enlarged, sintered catalyst pellets alloWs conduction of the

monoxide ratio in the resultant syngas.

[0005] The simplicity of the system, With little or no steam,
a loWer temperature of operation and a highly active catalyst
promises a compact and e?icient process that is capable of

heat of reaction to the front of the bed, Which then acts as a

formaldehyde reactor Where good thermal contact betWeen

feed pre-heater producing an essentially isothermal catalyst

bed Within an adiabatic reactor.

[0011]

In the operation of a ?xed bed catalyst With pre

operating ef?ciently Without extensive steam recycles. HoW

mixed feed for the oxidation of methane to syngas there are

ever, the processes described in the literature prior to U. S. Pat.

No. 7,641,888 Gobina, utilise a pre-mixed feed Well Within

safety issues that are associated With operating in an explo

sive regime. These problems are exacerbated if heat exchange
function is required Within the reactor. Some have sought to
counteract this by stage Wise addition of oxygen to the feed
methane requiring a complex series of ?xed beds and gas
distributors (as described in Conoco US. Pat. No. 7,261,751

the explosive limits of the gases to produce a selective reac

tion. US. Pat. No. 7,641 ,888 is incorporated herein by refer

ence. This presents signi?cant safety problems particularly in
operation and preheating of the respective feeds. The safety of
the reaction relies on the gas velocities being maintained at a

Which is incorporated herein by reference) and this alloWs for

suf?ciently high speed that ?ash back to the inlet point does
not occur.

removal of some of the reaction heat betWeen catalyst beds as

the material contains little or no oxygen as it passes through

[0006]

the heat exchanger. HoWever, this is a complex and expensive

With the invention of a tWo chamber reactor sepa

rated by a porous, catalytic, membrane With mixing and reac

solution.

tion taking place simultaneously Within the reactor the safety

of the system Was greatly improved.
[0007] HoWever, there is another problem that is found
That is the problem of catalyst overheating. It has since been

[0012] A problem, found With rhodium partial oxidation

catalysts in a ?xed bed arrangement, is that despite the high
selectivity that is achievable With this form of catalyst very
high catalyst surface temperatures can form that far exceed
the adiabatic reaction temperature.
[0013] One option to reduce the catalyst surface tempera

found that a similar problem can also occur Within the tWo

tures Within the reactor is to operate the catalyst With a tur

chamber porous membrane reactor described. The steps to

mitigate this problem Within a multitubular reactor are the

bulent gas in contact With the catalyst. This is the subject of

the present invention.
[0014] The sloW partial oxidation of methane With oxygen

Within a ?xed bed partial oxidation reactor that is described in

the literature but not referred to in US. Pat. No. 7,641,888.

subject of this patent.

[0008] The partial oxidation of methane is a very rapid
reaction that takes place at temperatures in excess of 600 deg

C. Typically, When performed using a ?xed bed of catalyst

is knoWn to be a strongly exothermic reaction folloWed by an

endothermic reaction. After this initial discovery it Was dis
covered that the reaction Would still take place at very much

US 2013/0015405 A1

higher gas hourly space velocities (GHSV). The fast partial

oxidation of methane With oxygen using a ?xed bed of
rhodium on alumina Was thought to be effectively isothermal,
although there is still some debate on this. Published Work has

shoWn that the reaction pathWay still involves high heat

release in the initial part of the catalyst bed and endothermic

reactions later (e.g. Basini, Aasberg-Petersen, Guarinoni,

Ostberg, Catalysis Today 64 (2001), 9-20, Which is incorpo

Jan. 17, 2013

through to the second chamber and the second reactant gas to

diffuse into the porous catalytic membrane such that there is

reaction and products pass into the second chamber;

[0029] Wherein the heat of reaction formed from the reac
tion of the ?rst and second reactant gases is capable of being
dissipated and/or removed along the reaction Zone by pas sage
of the gas along the heat transfer surface substantially per
pendicular to the How of gases through the porous catalytic

rated herein by reference). Some have attributed this rise in

surface temperature to the superadiabatic effect that is related
to the higher diffusion rates of H2 and H in combustion pro

[0030] According to a third aspect of the present invention

there is provided apparatus for the oxidation of reactant gases,

cesses, others have suggested it is a consequence of compet

said apparatus comprising:

ing kinetics. HoWever, a satisfactory Way of managing the

heat pro?le of the catalyst bed has not been found.

[0031] a ?rst chamber forming a passageWay for a ?rst

reactant gas;
[0032] a second chamber forming a passageWay for a sec
ond reactant gas;

[0015] We also refer to WO 2004/098750, Which is incor

porated herein by reference, Which relates to a membrane and
a method of preparing the membrane, said membrane being
used in a process to produce hydrogen gas via a partial oxi
dation of methane.
[0016] It is an object of at least one aspect of the present
invention to obviate or mitigate at least one or more of the

aforementioned problems.
[0017] It is a further object of at least one aspect of the
present invention to provide an improved process and appa
ratus for partial oxidation of methane.
[0018] It is a further object of at least one aspect of the
present invention to provide an improved process and appa

ratus for partial oxidation of methane Which enables catalyst

in the reaction Zone to be cooled and thereby overcome the

problem of a reaction catalyst overheating.

[0019] It is a yet further object of at least one aspect of the
present invention to provide an improved process and appa
ratus for partial oxidation of methane Which alloWs higher
temperatures to be used Which increases the thermal e?i
ciency of the process and Which also alloWs higher pressures

of operation.
SUMMARY OF THE INVENTION

Zone.

[0033]

a porous catalytic membrane separating the ?rst and

second chambers, said membrane being capable of alloWing

the ?rst reactant gas to permeate from the ?rst chamber
through to the second chamber and the second reactant gas to
diffuse into the porous catalytic membrane such that there is

reaction and products pass into the second chamber;

[0034] Wherein the heat of reaction formed from the reac
tion of the ?rst and second reactant gases is capable of being
dissipated and/or removed along the reaction Zone by pas sage
of the gas along the heat transfer surface substantially per
pendicular to the How of gases through the porous catalytic
Zone, Where the heat transfer surface is separated by than
5mm the porous catalytic Zone. The present invention there
fore relates to dissipating and/or removing thermal energy
formed from the heat of reaction from the ?rst and second
reactant gases and reducing surface temperatures in the reac
tion Zone. The ?rst and second reactant gases may react
together With one another in a partial oxidation to form a

partially oxidised product such as a synthetic gas (e.g. CO and

H2).
[0035]

Utilising a cylindrical geometry rather than ?xed

bed increases the surface area of catalyst bed that can be

[0020] According to a ?rst aspect of the present invention

there is provided apparatus for the oxidation of reactant gases,

thermal radiation in a cost effective manner. The heat of

said apparatus comprising:

reaction can then be removed by providing a heat transfer

[0021] a ?rst chamber forming a passageWay for a ?rst

reactant gas;
[0022] a second chamber forming a passageWay for a sec
ond reactant gas;

surface Within, for example, line of sight of this catalyst Zone

such that thermal radiation, and convection, from the reaction

[0023]

a porous catalytic membrane separating the ?rst and

second chambers, said membrane being capable of alloWing

the ?rst reactant gas to permeate from the ?rst chamber
through to the second chamber and the second reactant gas to
diffuse into the porous catalytic membrane such that there is

exposed to a heat transfer, particularly by the mechanism of

Zone is capable of transferring some of the heat of reaction

from the catalyst surface to the heat transfer surface. The heat
transfer surface may be maintained at the desired temperature
through the use of ?oWing gas across, for example, the reverse
side. The catalytic porous Zone is maintained at a more uni

form temperature by ensuring a good thermal conductivity.

This can be achieved, for example by the use of a sintered

reaction and products pass into the second chamber;

support Whereby sintering of the component particles

[0024] Wherein the heat of reaction formed from the reac

tion of the ?rst and second reactant gases is capable of being
dissipated and/ or removed along the reaction Zone.
[0025] According to a second aspect of the present inven
tion there is provided apparatus for the oxidation of reactant

enhances thermal conductivity as a result of intimate contact

gases, said apparatus comprising:

[0026] a ?rst chamber forming a passageWay for a ?rst
reactant gas;
[0027] a second chamber forming a passageWay for a sec
ond reactant gas;

[0028]

a porous catalytic membrane separating the ?rst and

second chambers, said membrane being capable of alloWing

the ?rst reactant gas to permeate from the ?rst chamber

betWeen the constituent particles. One possibility is that this

?oWing gas may be one of the feed gases. This has the bene?t
of simplicity in that the heat transfer surface is not a pres sure

containing surface. For example, literature shoWs that While

the temperature of the gas typically rises from about 400 C.
to about 850 C., inlet to outlet for the stoichiometric reaction
in a ?xed bed, it may be found that surface catalyst tempera
tures reach up to about 1100 C. We have found that utilisia
tion of a heat transfer surface in line of sight of the reaction
Zone for the partial oxidation of methane is able to loWer the

peak surface catalyst temperature by about 50-300 C. or

typically about 100 C.

US 2013/0015405 A1

Jan. 17, 2013

[0036] The amount of heat that can be removed depends

upon the How rate, exothermicity of the reaction and resultant
surface temperatures. At a surface temperature of about 1000
C. the thermal radiation given off is approximately 60

may be about 600 lpmin.

[0041] Typically, the ?rst chamber may be in the form of a
sleeve Which may be cylindrical in shape.

kW/m2. The amount that can be removed at this temperature

Without severe detrimental effect to the selectivity of the

sageWay through Which the ?rst reactant gas may ?oW along.

process depends strongly on the operating parameters includ

ing the amount of complete oxidation, the How rates, the

The ?rst chamber may also form a reaction chamber in Which

the ?rst and second reactant gases may react.

pressure etc. The upper limit is set by the amount of surface

area and temperature and hence it can be seen that making
more surface area visible is advantageous for heat transfer. In

[0043] Typically, the second chamber may be in the form of

a sleeve Which may be cylindrical in shape. The second cham
ber may have a larger diameter than the ?rst chamber and may
therefore form an outer sleeve. Typically, the second chamber

particular embodiments, the heat of reaction may be removed

by coupling the apparatus to an endothermic reaction such as

steam reforming of methane. An additional option may be

that the heat transfer surface may be in the form of a tube,

either surrounding the cylindrical catalyst support or placed

betWeen cylindrical support in an array, typical of shell and
tube type heat exchanger units. In both these arrangements
the heat transfer surface can form a pressure containing vessel
that may noW utilise a separate ?uid to maintain the desired

surface temperature of the heat transfer surface. Furthermore,

the heat transfer tube may even contain catalyst and reacting
?uids. For example, if the heat transfer tube contains a steam
reforming catalyst and suitable reacting gases then, as steam
reforming is a strongly endothermic reaction, some of the
heat of reaction from the partial oxidation of methane Will be
transferred by convection and radiation to drive the steam
reforming of methane. Preferably, the reaction Zone in the
second chamber Where the ?rst and second reactant gases

[0040]

[0042]

The How rate of the ?rst and second reactant gases

The ?rst chamber may therefore have a central pas

may form an enclosure around or at least partially encompass

the ?rst chamber. The second chamber may therefore form a
passageway for a second reactant gas.

[0044] The ?rst reactant gas may permeate from the ?rst
chamber through the porous catalytic membrane at high tem
peratures into the second chamber to react With the second
reactant gas. The rate of permeation of the ?rst reactant gas
may be such that the pressure drop from one chamber to
another is maintained at a suitable level, typically less than

about 1 bar. The pressure drop can be reduced by increasing

the pores siZe of the support. Typically this pore siZe may be
in the region of about 200 to 20,000 nm With the thickness of

the layer being adjusted to balance the pressure drop and

permeation rate. Conveniently, the ?rst reactant gas may
therefore be predominantly fed via the ?rst chamber and the
second reactant gas may be predominantly fed via the second
chamber.

may react may be directly connected to an endothermic reac

[0045]

tion. The endothermic reaction preferably may have a heat of

reaction in the region of 200 kJ/mol. The reaction Zone in the
second chamber Where the ?rst and second reactant gases
may react may also be directly connected to an exothermic
reaction to deal With the situation When the oxidation reaction

and may, for example, be oxygen.

[0046] Typically, the ?rst reactant gas may be pre-heated to
a temperature of about 200 C. using any suitable type of

becomes endothermic. The exothermic reaction preferably

may have a free energy reaction AH from about 40 to 900

kJ/mol depending on the level of complete and partial oxida

tion.

[0037]

The ?rst reactant gas fed at a rate of about 300 lpmin

pre-heater.
[0047]

The ?rst reactant gas may be fed into the ?rst cham

ber using any suitable means such as an inlet.

[0048]

The porous catalytic membrane may form a porous

sleeve-type region containing a catalyst. The porous sleeve

type region may be of any suitable shape and may comprise a

Heat may therefore be dissipated and/or removed

holloW core forming a passageWay for the second reactant

from the reaction Zone in the second chamber to the ?rst

chamber at a rate of about 0-50 kW/m2 or typically about 20
kW/m2. The temperature in the reaction Zone may reach an
upper surface temperature of about 1000 C. and a loWer

gas. For example, the sleeve-type region may be cylindrical or

temperature of about 750 C. It is preferred to maintain the

reaction Zone at a temperature of about 950 C. by using
externally connected exothermic and/or endothermic reac
tions.
[0038] The reaction Zone may be de?ned as any part of or
all of the area of the second chamber Where reaction is occur
ring betWeen the ?rst and second reactant gases. The reaction

reactant gas may also be pre-heated to a temperature of about

Zone may have a length of about 200 cm, may be at a tem

perature of about 900 C. With higher temperatures near to the

feed inlet points and loWer temperatures near the product
outlet point and/or may have an operating pressure of about

substantially cylindrical in shape.

[0049]

The second reactant gas may be fed at a rate of about

600 lpmin and may, for example, be methane. The second

600 C. using any suitable type of pre-heater. In particular

embodiments, a heat exchange surface may be used.
[0050] The ?rst and second reactant gases may react to
form a synthetic gas (i.e. syngas) giving a total outlet ?oW rate
of about 1800 lpmin
[0051] In particular embodiments Where the ?rst reactant
gas is oxygen and the second reactant gas is methane the
folloWing partial oxidation reaction may occur to form syn
thetic gas:

100-2000 kPa. The diameter of the cylinder forming the

chamber may be in the region of 40 mm. At higher turbulent
?oW Within the second chamber the temperature pro?le is

[0052] The porous catalytic membrane may be made from

any suitable porous material but particularly is made from

more even and the peak surface temperatures can occur more

alumina and has pore siZes of about 0.2 to 20 pm. The porous

than half Way through the reactor hoWever the heat transfer
surface is still able to effectively loWer the catalytic surface

catalytic membrane may therefore form a porous support in,

for example, a cylindrical form. The porous catalytic mem

temperatures.

brane may comprise structured voids (i.e. not packed With

catalyst pellets). A preferred catalytic material is rhodium or

[0039] The ?rst and second reactant gases may be pre

heated in the region of the reaction Zone in the apparatus.

platinum. The catalyst may be impregnated throughout the

US 2013/0015405 A1

Whole of the porous region or may be deposited on either one

of or both of the inner and outer surfaces of the porous region.

[0053]

The function of the porous catalytic membrane may

be to alloW the ?rst reactant gas once entering the ?rst cham
ber to permeate toWards the second reactant chamber and the
second reactant gas to diffuse into the porous catalytic mem

brane Whereupon they react. The presence of the catalytic

Jan. 17, 2013

any of the folloWing: less than about 300 mm; less than about
100 mm; or less than about 50 mm.

[0062]

lyst containing Zone Where:

[0063] a. The Reynolds number in the chamber compris
ing oxygen is maintained loWer than in the channel

comprising methane

metal Within the Zone Where the gases mix may enable the

correct stoichiometry at the catalyst surface for good selec

tivity to be maintained While also maintain separation of the
reactant gases as they enter the reactor.

[0054] The pressure in the central passageWay in the second

chamber may be about 500 kPa. The pressure in the ?rst
chamber may be about 550 kPa.
[0055] Using heat exchange to maintain a heat transfer
surface temperature from 800 to 10000 C. may modify the

catalyst surface temperature. By modifying the catalyst sur

face temperature Will maintain a more even catalyst surface

temperature of about 900 C. This has the advantageous fea

tures of increasing catalyst life. The thermal e?iciency of the
process may also increased because heat can be used inter
nally Within the reactor for pre-heating of the feed gases to a

higher temperature than With just simple preheating.

[0056]

The temperature may be maintained by using a com

bination of exothermic and/or endothermic reactions in a heat

transfer process to maintain the catalyst at an optimum oper

ating temperature of, for example, about 9000 C. The present

invention therefore provides a heat exchange transfer surface

capable of allowing heat to be removed from the catalytic

surface Where the exothermic reaction is most intense and
optionally heat to be added to the reaction Where the endot
hermic reactions become more dominant. Heat may therefore
be dissipated by use of an endothermic reaction such as steam

reforming of methane. In alternative embodiments, heat may

be added by use of an exothermic reaction such as complete or

partial combustion.
[0057]

It is also bene?cial for the length of the membrane,

the diameter of the channels Within the membrane and the

diameter of the surrounding heat transfer surface to be chosen
such that the Reynolds number of the ?uid ?oW Within the
chamber containing the methane reactant gas is greater than
500.
[0058] The ?rst chamber may therefore have a length and
diameter such that the Reynolds number of the ?rst reactant

gas passing along the length of the ?rst chamber has a Rey
nolds number greater than about 500. The Reynolds number
in the ?rst chamber may be selected from any of the folloW

ing: greater than about 1,000; greater than about 5,000; or

greater than about 10,000. Alternatively, the Reynolds num
ber in the ?rst chamber may be from about 500-20,000 or

about 1,000 to 20,000.

[0059]

To obtain the required Reynolds number the length

Typically, the oxygen may be fed to the reactor

through a porous Zone that is separate from the porous cata

[0064] b. Where the oxygen porous distributor is open

ended.
[0065] In particular embodiments, a fraction of the gas is
alloWed to pass from one chamber to another Without passage

through the catalytic membrane.

[0066] The reactor may be refractory lined. Therefore, a
shell of the reactor may have an internal refractory material

capable of self containing heat giving the reactor adiabatic

features that Will alloW the recovery of heat after passing
through the reactor. The energy from the hot gases can then be
used to generate energy or pre heat gases at the beginning.
[0067] Typically, the reaction may use air or any combina
tion of oxygen enriched air.

[0068] The reactor may also alloW for cleaning in situ by

means of Introduction of, for example, steam to improve gas

inlet velocity, decrease carbon formation and improve hydro

gen yields.
[0069] The reactor may also alloW introduction of nitrogen
to enhance reactor performance and reduce the requirement
for heat transfer.
[0070] The reactor may also alloW gas product extraction
on both sides of the membrane, in other Words the adiabatic
reactor enables recovery of the syngas produced through the
middle of the reactor on the membrane side or through the
shell of the adiabatic reactor.

[0071]

The reactor may also alloW for in situ regeneration

of catalyst.
[0072] The reactor may be used for producing syngas in
ratios of about 2:1 H2/CO all the Way to about 6:1 if desired.
[0073] The reactor may therefore be used for handling;
Natural gas, Coal Bed Methane and Biogas.
[0074] According to a fourth aspect of the present invention

there is provided a method of dissipating and/or removing

heat along a reaction Zone of an apparatus used for the oxi

dation of reactant gases, said method comprising:

[0075] providing a ?rst chamber forming a passageWay for
a ?rst reactant gas;

[0076]

providing a second chamber forming a passageWay

for a second reactant gas;

[0077] providing a porous catalytic membrane separating

the ?rst and second chambers, said membrane being capable
of alloWing the ?rst reactant gas to permeate from the ?rst
chamber through to the second chamber and the second reac
tant gas to diffuse into the porous catalytic membrane such
that there is reaction and products pass into the second cham

of the ?rst chamber may be selected from any of the folloW

ber;

ing: longer than about 400 mm; longer than about 600 mm;
longer than about 1,200 mm; longer than about 2,000 mm; or
longer than about 5,000 mm.

[0078] Wherein the heat of reaction formed from the reac

tion of the ?rst and second reactant gases is capable of being
dissipated and/or removed along the reaction Zone.

[0060]

To obtain the required Reynolds number the hydrau

lic mean diameter of the ?rst chamber may be selected from

[0079]

any of the folloWing: greater than about 2 mm; greater than

BRIEF DESCRIPTION OF THE DRAWINGS

about 5 mm; greater than about 10 mm; or greater than about

20 mm.

[0061]

[0080]

To obtain the required Reynolds number the hydrau

lic mean diameter of the ?rst chamber may be selected from

The method may use any of the above described

apparatus.

Embodiments of the present invention Will noW be

described, by Way of example only, With reference to the

accompanying draWings in Which: