U.S. patent number 3,856,658 [Application Number 05/404,281] was granted by the patent office on 1974-12-24 for slurried solids handling for coal hydrogenation.
This patent grant is currently assigned to Hydrocarbon Research Inc.. Invention is credited to Michael C. Chervenak, Ronald H. Wolk.
United States Patent |
3,856,658 |
Wolk , et al. |
December 24, 1974 |
SLURRIED SOLIDS HANDLING FOR COAL HYDROGENATION
Abstract
In the H-Coal process for coal hydrogenation, an initial step is
the preparation of a coal slurry for transfer by suitable means
into the pressurized reactor. This invention provides an improved
method for facilitating such slurry transfer by pumping, and uses a
recycled carried liquid to help provide a dilute easily pumpable
coal slurry which is pressurized to above reactor pressure and then
concentrated in solids content to a desired extent by centrifugal
separation means before passing the concentrated slurry to the
reaction zone. A clarified liquid stream withdrawn from the slurry
concentration step is recirculated back to the mixing step to
facilitate the pumping step.
Inventors: |
Wolk; Ronald H. (Trenton,
NJ), Chervenak; Michael C. (Pennington, NJ) |
Assignee: |
Hydrocarbon Research Inc. (New
York, NY)
|
Family
ID: |
26886676 |
Appl.
No.: |
05/404,281 |
Filed: |
October 9, 1973 |
Related U.S. Patent Documents
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Application
Number |
Filing Date |
Patent Number |
Issue Date |
|
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191035 |
Oct 20, 1971 |
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Current U.S.
Class: |
208/415; 208/419;
208/434; 208/425 |
Current CPC
Class: |
C10G
1/00 (20130101); C10G 1/065 (20130101) |
Current International
Class: |
C10G
1/00 (20060101); C10G 1/06 (20060101); C10g
001/06 () |
Field of
Search: |
;208/10 ;302/14 |
References Cited
[Referenced By]
U.S. Patent Documents
Primary Examiner: Gantz; Delbert E.
Assistant Examiner: Berger; S.
Parent Case Text
CROSS REFERENCE TO RELATED APPLICATIONS
This is a continuation-in-part of copending application, Ser. No.
191,035, filed Oct. 20, 1971 and now abandoned.
Claims
We claim:
1. A method for introducing particulate coal in liquid phase slurry
form into a high pressure reaction zone which comprises:
a. mixing said particulate coal with a hydrocarbon liquid to
produce a dilute slurry;
b. pressurizing said dilute slurry to a pressure above the reaction
zone pressure;
c. passing said pressurized slurry through liquid-solid centrifugal
type separator means without substantial loss of pressure to
produce a clarified liquid portion and a concentrated slurry
portion;
d. returning the clarified liquid portion from (c) through pressure
reducing means to the mixing step (a); and
e. passing the concentrated slurry portion of (c) to the high
pressure reaction zone.
2. The method of claim 1 wherein the particulate coal solids are
smaller than 20 mesh and the slurrying liquid is a light
hydrocarbon oil.
3. The method of claim 1 wherein the particulate solids are a
mixture of coal and catalyst and the liquid is oil.
4. The method of claim 1 wherein the initial slurry is formed under
ambient conditions and is pressurized to at least 500 psig and the
concentrated slurry is then heated to a temperature of at least
500.degree.F.
5. The method of claim 1 wherein the pressure drop across the
centrifugal separator means to effect the liquid-solids separation
is 50-200 psi.
6. The process of claim 1 wherein the slurry of step (b) has a
viscosity less than about 10 poise.
7. The method of claim 1 wherein the slurry pressurizing means is a
positive displacement reciprocating plunger type pump.
8. A liquid phase catalytic hydroconversion process for converting
coal to liquid hydrocarbons and gas which comprises:
a. slurry said coal with a hydrocarbon oil boiling above
400.degree.F recovered from the process in a ratio of from 0.5 part
of coal per part of oil to 3 parts coal per part of oil at
substantially ambient conditions;
b. pressurizing said slurry by positive displacement pumping means
to a pressure of 1,000-3,000 psig;
c. centrifugally separating at least a substantial part of the
liquid portion from the coal slurry by centrifugal force means to
provide a more concentrated solids slurry portion;
d. returning the clarified liquid from step (c) through pressure
reducing means to step (a);
e. heating the concentrated coal slurry to
600.degree.-950.degree.F; and
f. discharging said concentrated heat slurry to a high pressure
reaction zone wherein it is converted to hydrocarbon liquid and gas
products.
9. The process of claim 8 wherein said slurry liquid is a
hydrocarbon oil recovered from the process and having a nominal
boiling range above 400.degree.F.
10. The process of claim 8 wherein the pressure reducing means to
step (d) is a hydraulic turbine.
Description
BACKGROUND OF THE INVENTION
Hydrogenation of a coal-oil slurry by the upflow, liquid-phase,
random motion ebullated bed process known as H-Coal and described
in U.S. Pat. No. 3,519,555 to Keith et al., is accomplished at
temperatures in the range of 750.degree.-950.degree.F and pressures
in the range of 1,000-3,000 psig with coal throughputs ranging from
15 to 300 pounds per hour per cubic fool of reactor volume, and
results in yields in the order of four barrels of synthetic crude
oil per ton of coal. There are, of course, other variables
involved, primarily due to the rank of the coal to be converted and
to the end products desired.
The particulate coal is usually mixed with a carrying oil to form a
slurry, which is then pressurized and introduced into the reactor
along with heated hydrogen gas. However, introducing the relatively
viscous coal-oil slurry into the high pressure ebullated bed
reactor presents significant problems. Because the coal particles
are quite abrasive, they cause rapid erosion and wear in the
pumping equipment, particularly for positive displacement type
pumps which are usually used at the high discharge pressures
involved and which have close internal clearances.
SUMMARY OF THE INVENTION
It has been found that the economical introduction of coal into a
pressurized reactor is a function of the solids concentration in
the coal-liquid slurry, as well as a function of the viscosity and
temperature of the carrier liquid used. While it is essential to
provide a satisfactorily pumpable fluid slurry, any excessive
dilution used in preparing the slurry to facilitate the pumping
step has involved considerable excess investment costs for the rest
of the high pressure reaction system and much higher operating
costs. However, a coal-liquid slurry more concentrated in solids
becomes far more difficult to pump in that the coal solids tend to
settle out in the pump body and thus interfere with its normal
operation, and also to accelerate erosion of the pump inner
parts.
In accordance with the present invention, the pumping of the
coal-liquid slurry to high pressure is accomplished on a dilute
(low percentage of solids) slurry stream which is first pressurized
to super-atmospheric pressures, preferably to slightly above the
desired reactor pressure, following which a concentration of solids
in the slurry to the extent desired is accomplished by centrifugal
force means at substantially the same pressure level. This
concentrated slurry is then heated to near reactor temperature and
passed into the reaction zone without further pressurization.
In the slurry concentration step, the undesired liquid portion is
conveniently and substantially removed from the dilute slurry by
centrifugal force action using a liquid cyclone device, and such
liquid is recycled to the initial slurry preparation step.
Separating this undesired liquid portion by centrifugal force means
such as a liquid cyclone or hydroclone apparatus is quite
desirable, in that the apparatus is relatively simple and reliable
and no plugging problems ordinarily result due to the solids
portion of the slurry, such as would usually occur if filtration
means were used for the slurry concentration step. This liquid
recycle arrangement permits the pressurizing transfer pump to
advantageously handle a dilute slurry material only, with the
concentrated slurry material then being constituted so as to flow
freely through regular piping and through the remainder of the
system. While the carrier liquid used may be any hydrocarbon oil,
it is preferably a light hydrocarbon oil which may conveniently be
made in the coal hydrogenation process.
The principle advantage provided by this invention is that it
materially reduces the amount of diluent oil that must be handled
in the remainder of the system downstream of the liquid-solid
separation step, i.e., in the heater, reactor, heat exchangers,
distillation apparatus and such. Consequently, this arrangement
requires a smaller reactor and less heat exchange surface and
smaller piping for handling the excess liquid. Other advantages
include less wear on the slurry pump, which thus usually can be a
less expensive pump.
DESCRIPTION OF THE DRAWING
The drawing is a schematic view of certain process equipment for
the hydrogenation of coal.
DESCRIPTION OF THE PREFERRED EMBODIMENT
Referring to the attached drawing, particulate coal solids at 10
and a carrier liquid, which is preferably a light hydrocarbon oil,
at 12 are added to a slurry mixing tank 14 in a preferred ratio of
about 60 weight percent solids to 40 weight percent liquid. The
solids/liquid weight ratios of the slurry, however, may vary from
about 0.5:1 to 3:1 of coal to liquid depending on the properties of
the carrier liquid. The mixing tank 14 conveniently has a slurry
mixer 16 which is driven by motor 18, which may be either electric
or hydraulic and powered by recycle liquid.
The resulting coal-liquid slurry, diluted by a recycle liquid
stream as explained below and at a pressure between atmospheric and
about 15 psig, is withdrawn from the mixing tank through line 20 to
pump 22, wherein it is pressurized to above reactor pressure or
about 500-3250 psig, and preferably to 1000-3,000 psig. This high
pressure dilute slurry is then passed through line 24 to liquid
cyclone 26 for liquid-solids separation. In the liquid cyclone 26
the separation of the dilute slurry into a substantially clarified
liquid overflow and concentrated slurry underflow streams occurs by
centrifugal and centripetal force action induced by the pressure
drop developed through the static device. The liquid cyclone 26 is
selected and the pressure differential across it adjusted by the
flow rate therethrough so that about 30 weight percent of dilute
slurry stream 24 is returned as clarified liquid through line 28
under control of pressure reducing means 30 back to slurry mixing
tank 14 to help provide the dilute slurry therein. The pressure
drop across the liquid cyclone device will usually be 50-200 psi.
Thus, the remaining concentrated slurry at substantially the same
pressure level and preferably containing about 60 weight percent
solids and 40 weight percent carrier liquid, is now passed by line
32 through heater 34. Herein it is heated to at least 500.degree.F
and preferably to 600.degree.-800.degree.F and then passed on to
the hydrogenation reactor 36.
As an example of this reactor 36, reference is made to U.S. Pat.
No. 3,519,555 previously mentioned. In such case, by appropriate
control of liquid and coal and hydrogen supplied in line 38, an
ebullated bed hydroconversion condition can be provided in the
reactor with the ultimate removal of gaseous products at 40 and
liquid products at 42. Carrier liquid 12 is preferably a light
hydrocarbon oil boiling in the range of fuel oil, that is, having a
nominal boiling range above 400.degree.F, illustratively, one
having a nominal boiling range of 400.degree.-975.degree.F and
recovered from the process by conventional processing steps (not
shown) downstream of liquid stream 42.
It is also within the contemplation of this invention that the
solid particulate matter may be catalyst rather than, or together
with, the coal, such as also disclosed in U.S. Pat. No.
3,519,555.
In a coal hydrogenation system of this type, the dilute slurry is
pumped to a high pressure, following which the clarified liquid
obtained after passing through the liquid cyclone separator is
recycled back through pressure reducing means 30 to the slurry
mixing tank. If desired, the dissipation of the pressure of this
recycled liquid stream may be accomplished by a hydraulic turbine,
with the power output therefrom used in the system either for
driving the slurry mixer motor 18 or assisting in driving high
pressure pump 22. The concentrated slurry stream at substantially
the high pressure level is passed to the process reactor 36.
In this system utilizing high pressure pump 22, which is preferably
a positive displacement reciprocating plunger type pump, the pump
operates only on dilute slurry. Furthermore, the more dilute the
slurry, the less the pump wear and greater the pump reliability. No
wasteful diluent is required in the remainder of the system and
such avoidance of excess liquid processing and additional heat
exchange surface is highly beneficial in reducing equipment
investment and operating costs. For example, in a coal
hydrogenation process as normally operated with high pressure
slurry pump 22, as much as 50-60 weight percent diluent liquid is
required in the process. Using this invention, only about half of
this diluent liquid is required for transfer of the coal slurry
downstream of liquid cyclone 26 through the associated piping,
heater, etc., to the reactor.
The significance of this coal slurry handling method for ebullated
bed coal hydrogenation is evident from the determination that
viscosity of coal-oil slurry increases appreciably for each percent
increase in solids in the slurry. It is usually preferred practice
to limit the viscosity of slurries to be pumped in this pressure
range (up to 3,500 psig) to about 3 poise and not more than 10
poise. Pumping concentrated slurries is therefore quite difficult
and expensive.
Normal conditions for coal hydrogenation have been established
using a start-up coal-oil slurry of about 20 weight percent solids
at about 100.degree.F (ambient). which is pressurized to reactor
pressure by one or more pumping stages, then concentrated to about
50 weight percent solids. This slurry material will flow readily
through regular piping in the heater and to the reactor.
EXAMPLE
From the established data, it is found that for coal hydrogenation,
the coal-oil dilute slurry may have the following initial
properties:
1. Slurry formed of pulverized coal finer than 20 mesh (U.S. Sieve
Series) and hydrocarbon oil boiling in the range of fuel oil, i.e.,
having a nominal boiling range above 400.degree.F.
2. Temperature of 100.degree.-250.degree.F.
3. Viscosity of 3-10 poise.
4. Materials added to the slurry mixing tank in 60/40-solids/liquid
weight ratio.
The dilute slurry is pressurized to 1,000-3,000 psig, then
concentrated by centrifugal force means using a liquid cyclone
apparatus, after which the clarified liquid portion is removed for
return to the mixing tank. The remaining concentrated slurry for
reactor feed contains about 60/40-solids/liquid ratio. Such a
slurry material will flow through pipes and heat exchanger passages
to the reactor.
While we have shown and described a preferred form of embodiment of
the invention, we are aware that modifications may be made thereto
within the scope and spirit of the disclosure herein and of the
claims appended thereto. For example, while a single liquid cyclone
device has been shown, it is understood that multiple cyclone units
connected in parallel could advantageously be used in systems where
the flow rate exceeded the desired capacity of a single cyclone
unit.
* * * * *