Note : Les descriptions sont présentées dans la langue officielle dans laquelle elles ont été soumises.
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METHOD A~D APPARATUS FOR GENERATING HYDRO(~EN
FIELD OF THE INVENTION
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This invention relates to a method of and
apparatus for instantaneously generating hydrogen from
water upon demand, where needed as needed. This inven-
tion also relates to systems which include the described
method and apparatus and which utilizes the generated
hydrogen.
B KGROUND OF THE INVENTION
There is a continuing cri~ica]. need to more
efficiently produce hydrogen in substantial quantities
for forming chemical products and in chemical processes.
Presently, large quantities of hydrogen are
consumed in the manufacture of ammonia and methanol,
and in producing other alcohols, nitrates and ami.nes.
Hydrogen also is used in the hydrogenation of organic
~ compounds, such as oils and fats to make margarine and
`~ vegetable shortening.
In the steel making industry hydrogen is being
used in increasing quantities in the direct reduction of
iron ores to produce metallic iron which may be fed to
steel making furnaces, open hearth furnaces, electric
furnaces and as part of the feed for blast furnaces.
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Further, llydrogen can be used for such diverse
uses as the gasification and liquification of coal, the
reduction of oxides of tungsten and molybdenum to the
metals, the providing of high protein foods through
biosynthesis of hydrogen and carbon dioxide, and in
total water management programs ~o pasteurize pathogens.
Apart from the growing need as a chemical,
hydrogen, for some time, has been considered as a
possible alternative to fossil fuels: oil, natural gas
and coal. Hydrogen is an excellent fuel available in
abundance. Water provides an undepletable supply of
hydrogen. When it burns, hydrogen produces extraordin-
ary quantities of heat and essentially pollution free
water vapor useful once again as a source of more hydrogen.
Prior to the present invention, however, hy-
drogen has not been produced upon demand in an Pconomic
manner.
Available systems, generally, do not provide
hydrogen for instantaneous use. Presently, existing
systems commonly require production and storage, or
substantial accumulation, before utilization. There
is no direct link between production and use. Storage,
a necessary element in such existing systems, prohibits
instantaneous use of hydrogen upon production.
This is not meant to say that storage is
necessarily detrimental. Generally, however, the con-
sumer has not had the option of either directly using
the hydrogen or storing the hydrogen and using it when
needed. Presently storage is required.
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In add;tion, available systems do not produce
hydrogen economically. The price for hydrogen is not
, competitive with available sources of energy. Also,
it often tak~s more energy to produce hydrogen than the
energy available from the produced hydrogen.
In sum, there is a need to more efficiently
produce large quantities of hydrogen for chemical pur-
poses, and there is a pressing need to make available
an economic, ecologically sound energy generating sys-
tem which produces hydrogen from wa~er adap~ed for
instantaneous use at the option of the consumer.
It is a primary object of the 1nvention, there-
fore, to provide a new and improved method of and appara-
tus for producing hydrogen for chemical and energy purposes.
It is another primary object of the invention
to provide a new generating system which economically
produces hydrogen from wat~r adapted to be used upon
demand where needed, as needed, and which is an improve-
ment of the system of my earlier patent, United States
Patent No. 3,967,589.
It is another object of the invention to pro-
vide a new system which produces hydrogen from water
without substantially depleting the supply of water or
polluting the environment.
It is still another object of ~he invention
to provide a new system which produces hydrogen ready
~ for instantan ous use without the need for an inter-
Li~ mediate storage facility.
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Another object of the invention is to provide
a new energy system which produces low-cost hydrogen.
Among the other objects 3f the invention is
~o provide hydrogen generating and utilizing systems
for direct applications which serve human needs, such
as commercial, industrial and home heating, propulsion
for land, marine and aerospace vehicles, and the gener
ation of electricity by utilities, by commercial and
industrial enterprises, as well as by the homeowner.
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It is still a further object of this inven~
tion to provide a new and improved hydrogen generating
system for wherever hydrogen is used chemically in form-
ing hydrogen containing products as well as for processeswhere hydrogen can be used advantageously.
Additional objects and advantages will be set
forth in part hereinafter and in part will be obvious
herefrom or may be learned with the practice of the in-
vention, the same being realized and obtained by means
of the systems and applications,recited in the appended
claims.
SUMMARY OF THE INVENTION
In accordance with the present invention, there
is provided a hydrogen generating sys~em including a
plurality of reaction zones which contain catalys~ and
which are maintained at elevated temperatures. Steam
(or water~ is adapted to be conveyed to each catalyst
containing zone, wherein hydrogen is generated ~rom the
steam (or wa~er~, and wherein the generated hydrogen is
conveyed from the zone ready for use upon demand 9 where
needed, as needed. The invention lnclude~ forming adjacent
reaction zones in a reactor containing a catalyst in
each zone, and maintaining the zone at elevated tempera-
tures, to produce hydrogen from steam fed thereinto.
The zones in the reactor can be in the form of longitudinal
bores or tubes which extend along the length of the re-
actor about a heat aeneratina chamber~ At least one end of
the reactor includes transverse and radial passages, ~apted
to interconnect the lonaitudinal zones with each other,
with the surrou~ding atmosphere and with the source for
steam, all to ~aximize the generation of hydrogen by pro-
viding a reactor of maximum flexibility.
It is believed that hydrogen is generated by the
invention because of the interaction of the high tempera-
tures and the catalyst upon the steam (or water). At the
high tempera~ures, it is believed the the s~eam (or wat~r)
becomes super heated steam which tends to disassociate in
the presence of the catalyst, to produce hydrogen gas.
In any event, by practice of the invention, hydrogen is
produced from water which is instantaneously available for
use either as an essentially pollution free fuel, which,
when burned, again produces water, or as a chemical wherever
hydrogen is required in products or processes.
The catalyst of the system, generally, is metal-
lic and contains innumerable sites on its surface, which,
with the elevated temperature in each zone, effect the
generation of hydrogen. Illustratively, the catalyst is
formed of a web-like cellular structure defined by inter-
connected metal filaments comprising iron, copper, silver,
nickel, palladium, pla~inum, or iron-nickel and molybdenum.
Where the catalyst becomes deactivated because
of use in the present invention, it is regenerated, in situ.
For example, ~he innumerable reaction sites on a catalyst
` 35 surface of iron will become oxidized by the steam to produce
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hydrogen gas until the sites are oxidized. In such
instance, the catalyst sites become deactivated. To
reactivate the sites a reducing agent, such as hydrogen
or hydrocarbons or mix~ures thereof, can be used. Once
reactivated, steam can be fed to such ca~alyst to once
again generate hydrogen.
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As used herein, the term "deactivation" des-
cribes the condition of ~he catalyst when it is no longer
substantially effective as a catalyst in the production
of hydrogen, and ~he term "activated" describes the con-
dition of the catalyst when it is effective in the pro-
duction of substantial quantities of hydrogPn.
In this embodiment of the invention, the gen-
eratlng system includes control means, responsive to the
deactivation of the catalyst, adapted to halt ~he supply
of steam to the zone containing such catalyst and to
provide a catalyst regeneration agent which, once again?
activates the catalyst. At such time the control means
are adapted to reverse the process by halting the supply
of the regenerating agent and by supplying steam to the
reaction zone for the generation of hydrogen.
A conduit system at each end of the reac~or
and conn~cted to the zones or tubes conveys fluid to and
from the reactor. At one end, e.g., upstream of the re-
actor, a control conduit circuit selectively provides
to the tubes or zones steam from a s~eam generator for
~` 30 the production of hydrogen and a reducing agent, such
~` as hydrogen or hydrocarbon, to the tubes for the reactiva
tion of the catalyst. At the other end, e.g., downstream,
the conduit-system conveys fluids from the reactor, includ-
~ ing the hydrogen generated within the rPactor.
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Once the system is in full operation sel~cted
zon~s or tubes will con~ain an active catalyst whi.le
adjacent zones or tubes will contain deactivated catalyst.
Under such conditions the control conduit circuit con-
currently provides steam to each tube containing activecatalyst and a reducing agent, such as hydrogen, to each
tube containing deactivated ca~alyst. In each active
zone to which steam is supplied, the elevated tempera-
ture~ and catalyst decompose the steam to produce hydro-
gen gas. This reaction is endothermic in nature becausethe heat is absorbed by the reaction. Simultaneously,
in each deactivated zone to which hydrogen is supplied,
the reducing agent reacts with the o*idized catalyst to
remove the oxygen from the catalys~ surface to thereby
regenerate or reactivate the catalyst. This reaction
produces water and is exothermic in nature because heat
is generated by the reaction. By conducting the described
reactions in adjacent zones, the exothermic heat is used
to increase the production of hydrogen by further elevat-
ing the temperatures in a juxtaposed hydrogen generatingzone.
To provide these concurrent reactions in adjacent
æones, initially, the steam can be supplied to one zone
while noth~ng is supplied to the adjacent zone. Once the
catalyst is deactivated in the one zone, concurrent opera-
tion can be commenced. For example, when there are eight
zones positioned circumferentially about the heat generat-
ing chamber, initially steam can be supplied to every other
zone (a set of four zones)~ Once the catalyst in such
every other zone becomes deactivated., then concurrent
operations are commenced so that the exothermic reactivat-
ing reaction occurs in such every o~her zone while the
endothermic hydrogen reaction occurs in the alternate
adjacent 30nes (a seconQ set of four zones) with the aid
of the exothermic heat.
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Preferably, means are provided at the other
end (downstream) of the reaction zones which can deter-
mine when ~he tubes are no longer producing hydrogen
because of deactiva~ion of the catalyst. At this time
the control conduit circuit can cease providing s~eam
to the non-productive tubes and begin providing the
hydrogen or hydrocarbons to such tubes to reactivate
them. Once the catalyst has been reg~nerated the means
will determine that regnerating hydrogen is being con-
veyed through that tube so that the control conduitcircuit can reverse the d~scribed procedur~ and begin
to supply steam to the reactivated catalyst.
In the embodiment of the invention where the
catalyst is not deactivated by the steam~ e.g., a
catalyst formed from a platinum type of metal, the con-
duit system can continuously supply steam to each re-
; actor tube and continuously convey the generated hydrogen
therefrom.
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In each embodimen~ of the invention the generat-
ing system can include downstream cooling means for re-
ducing the temperature of hydrogen and other fluids con-
veyed from the reactor. In doing so meaningful reforma-
tion of thP hydrogen and ox~gen to form water is prohibited
and the temperature of the ~luids is reduced to make them
easier to handle by components o~the system which separate
and collect fluids, as hereafter described in more detail.
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In addition, as hereafter explained in more detail,
;, the method and apparatus of the present invention can be
included in systems which utilize hydrogen to form chemical
products and in chemical processes, as well as in systems
which use hydrogen as a fuel for such diverse applications
~ 35 as heating, propulsion and electricity.
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BRIEF DESCRIPTION OF THE DRAWINGS AND
ILLUSTRATIVE EMBODIMENT OF THE INVENTION
The following is a detailed description together
with accompanying drawings of preferred and illustrative
embodiments of the invention. It is to be understood
that the inventlon is capable of modification and varia-
tion apparent to those skilled in the art within the
spirit and scope of the invention.
In the Drawings:
FIGURE 1 is a perspective view of one embodi~
ment of the invention.
FIGURE 2 is an exploded, perspective view of
the embodiment of the invention shown in Figure 1, wherein
structure of several components of the system have been
partially broken away to show details thereof.
FIGURE 3 is a cross-sec~ional view of the up-
stream end of the reactor.
FIGURE 4 is a cross-sectional view of the down-
stream end of the reactor, taken along the lines 4-4
i of Figure 1.
FIGURE 5 is a longitudinal sectional view of
a tube of the reactor containing one embodiment of the
catalyst system of the invention.
2~ FIGURE 6 is a longitudinal sectional view of
a tube of the reactor containing another embodiment of
the catalyst system of the invention.
FIGURE 7 ls a magnified view of a portion of
the catalyst of either Figures 5 or 6.
FIGURE 8 is a longitudinal sectional view of a
tube of the reactor containing stlll another embodiment
of the catalyst system of the invention.
FIGURE g is a longitudinal sectional view of
a tube of the reactor containing still another embodi-
~ ment of the catalyst system of the invention.
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FIGURE 10 is a longitudinal sectional view
of a tube of the reactor containing still another em-
bodiment of the catalyst system of the invention.
FIGURE 11 is an end view of the ups~ream end
of the reactor of the hydrogen generating system.
FIGURE 12 is an end view of the do~str2am
end of the cooling means of the hydrogen generating
system.
FIGURE 13 is a cross-sectional view of the
cooling means of the hydrogen generating system taken
along the lines 13-13 of Figure 12.
FIGURE 14 is a planar view, diagrammatically
illustrating the interrelationship between the compon-
ents and operation of the system shown in Figures 1-2,
and includes metering devices at the upstream end at
each of the reaction tubes.
FIGURE 15 is a perspective view of another
embodiment of a hydrogen generating system of the pres-
ent invention.
FIGURE 16 is a cross-sectional view of the
reactor of Figure 15, taken along the lines 16-16,
wherein a second set of transverse passages are shown
for interconnection o the illustrated reactor tubes.
FIGU~E 17 is a planar view, diagralmmatically
illustrating the interrelationship between the components
and operation of the system shown in Figure 15.
FIGURE 18 is a perspective view of a further
embodiment of the hydrogen generating system of the pres-
ent invention.
FIGURE 19 is a planar view, diagra~matically
illustrating the interrelationship between the components
and operation of the system shown in Figure 18 wherein
the steam is fed into the catalyst in each of the reactor
tubes.
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FIGURE 20 is a planar view also diagrammatically
illustrating the interrelationship between ~he components
and operation of the sys~em as shown in Figure 18 wherein
the steam is fed about th~ catalyst in each of the re-
actor tubes.
FIGURE 21 is a perspective view, partially
broken away, showning the energy system producing hydrogen
fuel for a boiler.
FIGU~E 22 is a perspective view, partially
broken away, showing the energy system of the invention
for producing hydrogen fuel for a turbine.
FIGURE 23 is a side view showing the system of
the invention producing hydrogen fuel ~or a four cycle
internal combustion engine.
FIGURE 24 is a side view showing the system
of the invention producing hydrogen fuel for the Wankel
engine.
FIGURE 25 is a front view, partially broken
away, of a Stirling cycle engine which includes the hydro-
gen generating system.
` FIGURE 26 is a planar view, diagrammatically
illustrating the reactor of the present invention for
~ the Stirlîng cycle engine shown in Figure 25.
`~ FIGURF. 27 is a side view, diagrammatically
illustrating the system of the invention for producing
hydrogen ~uel for a fuel cell which generates electricity.
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~ FIGURES 1-14
`; Referring first to Figures 1-2, there is shown
a preferred embodiment of the system 10 of the invention
for producing hydrogen from water upon demand, where
needed, as need~d. The sys~em 10 includes a cylindrical
~` reactor 12 about which is a cylindrical boiler or steam
generator 14 in which steam is generated for the reactor
` 35 12. The reactor 12 has a heat generating chamber lS
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disposed centrally of a plurality of longitudinally
extending, circumferentially spaced zones in the form
of eight bores or tubes 18a-h having a catalyst 20
in each tube. At each end of the tubes 18a h are ~rans-
verse passages 22a-d - 25a-d and radial passages 26a-h
and 2Ba-h for selectively connecting the ~ubes 18a h
with each other, with the surrounding atmosphere, and
with the steam generator 14. As shown, a network of
conduits, generally identified herein by reference num-
lU ber 30, conveys fluids to and from the reactor 12 andboiler 14.
STEAM GENERATOR
The steam generator or boiler 14 includes an
annular chamber 32 which extends the length thereof for
receiving water and generating steam for the reac~or 12.
Extending through the boiler 14 is a central opening 34
for slidably fitting the boiler 14 about ~he central
portion of the reactor 12 where it is secured ~hereto
by flanges 36.
A conduit 38 is connected into the lower por-
tion of the chamber 32 for conveying water from a source
(not shown) to the boiler 14 through a control valve 40.
On the opposite side of the boiler 14, a conduit 42 is
connected into the upper portion of the chamber 32 for
conveying steam ~o the reactor 12.
As shown the boiler 14 includes a pressure
relief valve 41, a pressure gauge 43, and a sight glass
. assembly 45 with an upper valve 47 to monitor the level
~ of the water in the boiler and with a valve 49 for drainage.
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REACTOR
In the embodiment of the invention shown in
Figures 1 and 2, the cylindrical reactor 12 is integral
being formed of a solid piece of metal with a large
longitudinal central bore therethrough which forms the
heat genera~ing chamber 16 and with eight smaller longi-
tudinal bores therethrough circumferentially positioned
about the cham~er 16 which form equidistant reaction
zones or tubes 18a-h.
In the illustrative embodiment, a burner 44
is positioned within the upstream portion of the chamber
16 to provide heat from combustion derived from the fuel
that issues from the burner 44. This heat is sufficient
to generate steam from water in the boiler 14 and to
facilitate and cause the reactions within the zones or
tubes 18a-h for the generation of hydrogen. The burner
44 is positioned ~ithin chamber 16 so that the flame
therefrom contacts the portion of ~he tubes 18a-h which
contain three eatalyst 2~. In other embodiments of the
invention, described hereafter, ~he heat source required
for the system of ~he invention can be provided by rejected
waste heat, or other suitable sources.
Extending from the chamber 16 is an exhaust
conduit 45 for conveying the exhaust :Erom ~he system.
As shown in Figures 3 and 4, the ends of ~he
tubes 18a-h (upsteam and downstream) are connected in
pairs by transverse bores 22a, b, c and d, and 24a7 b,
` c and d, respectively. Each trans~erse bore extends
`~ between two longitudinal tubes, e.g., ups~ream trans
verse bore 22a interconnects ~he upstream ends of longi-
tudinal bores 18a and b while downstream transverse bore
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24a interconnects the downstream ends of the same tubes
18a and b. For access, additional upstream and downstream
transverse bores 23a, b, c and d, and 25a, b, c and d ex-
tend from one of each of ~he interconnected pairs of the
longitudinal bores, i.e., 18a, c, e, g, at the upstream
.and downstream ends thereof through the outer reactor
wall. As shown, the transverse bores, e.g., upstream
bores 22a, 23a, etc., downstream bores 24a, 25a, etc.,
are coaxial with the outer access bores, e.g., 23a and
25a being of greater breadth.
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Also, -the reactor 12 includes the radial bores
26a-h and 28a-h which extend radially outward from each
tube 18a-h at the end thereof, upstream and downstream
respectively, through the outer wall of the reactor 12.
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tudinal tubes 18a-h are interconnected in pairs by trans-
~; verse bores 22a-d and 24a-d; are connected to surrounding
atmosphere by both the transverse access bores 23a-d and
25a-d and the radial bores 26a-h and 28a-h; and are adapted
to be connected as will be described hereinafter, to the
steam generator 14 via the radial bores 26a-h and 28a-h.
25Moreover, accessibility and interconnectability
are selective. As shown, each of these bores and passages
have threaded portions for the receipt of correspondingly
~` threadcd plugs 29 having slotted heads for such purposes.
i~ As desired, these plugs 29 may be removed for the passage
of steam between adjacent tube~, e.g., tubes 18a, 18b,
etc., for the passage of steam through one or more
radial bores, e.g., 26a or 28a, etc., for drainage of
the tubes 18a-h through the same radial bores, or for
access to the interconnecting ~ransverse bores, e.g.,
upstream transverse bore 22a via bore 23a, etc. In the
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illustrative embodiment, all the plugs 29 are in
place so that pairs of tubes are not interconnected,
e.g., 18a is not connected to 18b via upstream trans-
verse bore 22a, and the ~ubes are not open to atmosphere
such as by radial bores 26a-h.
How removal of sel~cted plugs 29 provides flex-
ibility for the reactor 12 is demonstrated hereinafter
in connection with several embodiments of the invention.
CATALYST SYSTEMS
As illustrated in Figures 1 and 2, within the
tubes 18a-h of the reactor 12~ are catalyst systems 20
of the invention for facilita~ing an~ causing ~he separa-
tion of water vapor into hydrogen and oxygen.
In Figures 5-10 there are illustrated various
embodiments of the catalyst systems 20.
In the embodiment of the catalyst system shown
in Figure 5, there is illustrated the catalyst 20 in the
form of a spirally wound sheet 46 positioned within the
tubes 18a-h between two hollow end caps 48 held together
by wire 50 to form a cartridge slidably mounted within
each tube 18. Each cap 48 has a hollow sleeve 54 having
holes 56 drilled therethrough for the wire 50 and from
which a hollow plug 58 extends inwardly for abutment
against the spirally wound catalyst 20.
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In the embodiment of the catalyst system 20
shown in Figure 6, the catalyst 20 is cut from the sheet
` 46 into a number of discs 60 juxtaposed between the porous
end caps 48 and held together by the wire 50 to form the
slidably mounted cartridge.
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As shown in the magnif}cation of the ca~alyst
20 (Figure 7) the catalyst preferably is formed from
a powderPd metal product defining a web-like, three
dimensional, cellular structure in which the metal pro-
vides a network of in~erconnected metal filaments withinterconnected, asymmetrical spaces or cells therebetween.
By reasons of the network-like, porous, cellular struc-
ture, the metal provides large surface areas which are
reactive si~es. The metals which can be used for the
catalyst include iron, iron-nickel, copper and molybdenum,
palladium, and platinum. Several of these catalysts have
been made available by Foammetal Inc. of Willoughby,
Ohio, under the designation foametal, and are described
in its 1974 brochure entitled "LOW DENSITY FOAMETAL,
A Study of Surface Area, Texture, Cell Size and Filament
Diameters".
In use, the porous catalyst systems 20 provide
countless sites, which, with elevated temperatures, cause
the steam to disassociate to form hydrogen gas.
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Where the catalyst reacts with the steam, e.g.,
a catalyst formed of iron, the countless sites are oxi-
dized to produce an oxidized metal surface and hydrogen
gas. The decomposition of the steam passing therethrough
will continue until the metal essentially becomes coated
with oxygen at which time the catalyst becomes deactivated.
To regenerate the countless sites, hydrogen can be fed
through the tubes 18a-h into contact with the catalyst
20 where the hydrogen reacts wqth the oxygen on the metal
surface to form water vapor and a free metal surface.
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As wqll be described hereafter in more detail,
decomposition of the water to provide freed hydrogen
occurs with the iron catalyst system 20 in one tube
18, e.g., 18a, while oxygen is removed from the iron
5 catalyst system 20 in the adjacent ~ube 18, e.g., 18b.
In doing so the heat o~ the exothermic reaction, whlch
occurs in the tube 18 where oxygen is removed from the
catalyst 20, is us~d to increase the oxidation of the
catalyst 20 in the adjacent tube 18 which produces hy-
drogen gas from steam.
Where the catalyst causes disassociation with-
out reacting with the steam, e.g., a platinum type
catalyst ! the water disassociates to form hydrogen and
oxygen gases. In these embodiments the catalyst will
not become deactivated under normal operating conditions
so that hydrogen gas can be produced in all the reactor
tubes, e.g., 18a-h.
In the illustrative embodiments of the catalyst
systems 20 of Figures 8, 9 and 10, the catalysts are
~` formed from the platinum type metals and alloys of Group
VIIIB elements, and particularly platinum and palladium
metals and alloys. These platinum type catalysts are
sufficiently porous so as to allow the permeation or
diffusion of hydrogen therethrough while prohibiting
the passage of water vapor and oxygen. These catalysts
form a web-like cellular structure defined by inter-
connected platinum type metal filaments which prohibit
the passage of the larger water vapor molecules and oxy-
gen, but which permit the smaller hydrogen atoms to pass
therethrough.
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Moreover, the platinum type metal catalysts
of the invention are essentially ~elf-sustaining under
normal operating conditions. They do not become readily
deactivated. They can remain active for extremely long
periods of time.
As shown in Figures 8-10 the catalyst systems
20 include a conduit 62 which extends through the cat-
alyst and which is slidably and removably secured and
positioned within a reactor tube 18. The conduit 62
has a central portion 64 about which the catalyst 20
is mounted and through which the diffused hydrogen can
pass.
: 15 About one end of the conduit 62 (upsteam),
which extends from the catalyst 20, there is a support-
ing and metering disk 66 (Figure 8) having a slip fit
with respect to the conduit 62 and havîng a sliding fit
with respect to the reactor tube 18. Abou~ the outer
portion o the disk 66 are a plurality of U-shaped grooves
68 for directing and metering the passage of steam down-
stream about the catalyst into ~he space between the walls
of the tube 18 and the o~ter periphery of the catalyst 20.
About the other end of the conduit 62 (downstream~,
which also extends from the catalyst 20, there is a plug 70
welded t~ the conduit that is threaded for reception by
a correspondingly threaded end of the reactor tube 18 for
, ~ positioning and securing the catalyst system 20 in a gas
` 30 tight relationship in the reactor 12.
In the illustra~ive embodiment shown in Figure 8
the hydrogen porous platinum type metal catalyst 20 is --
; in the form of a plurali~y superimposed ~ubes 72 where
the openings ~n each tube generally are non-aligned or
asymmetrical to facilitate the separation of the gen~rated
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hydrogen from the other fluids in the reactor tubes 18.
As shown, there are two such superimposed hexagonally-
shaped ~ubes 72 which are fused together and which have
ends 74 that are tapered inwardly to the conduit 62
to contain t~e diffused hydrogen.
In the embodiment of Figure 9, the already
described catalyst 20 is in the form of a multi-layered
spiral wound material bonded together to form a contin-
uous maze of increased surface area for diffusion of
hydrogen.
In the embodiment shown in Figure 1OJ the des-
cribed catalyst ls multi-layered with a central core 76
from which extend a plurality of radial webs or wings
78 along a length ~hereof to provide ~he increased sur-
face area. The catalyst 20 is X-shaped with four radially
extending webs 78.
With respect to ~he central portion 64 of the
conduit 62, it can be made of a hydrogen permeable metal,
such as the platinum type metals (see Figure 9). In this
embodiment the ends of the conduit 62 are formed from an
inert non-diffusable metal, such as stainless steel, welded
to the central porous portion 64.
As shown in Figure 8, the conduit 62 of the
catalyst system 20 also can have perforations 80 in the
central portion 64 thereof for the rec~ption and passage
of diffused hydrogen. In this instance the entire con-
duit 62 can be made from stainless steel or other inert,
non diffusable metals.
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In the embodiments (Figures 8 and 10) the dif-
fused or permeated hydrogen passes through the conduit
62 while the remaining fluids (water, vapor and oxygen)
flow through the space between the catalyst 20 and
reactor tube 18 through passages in the other end of the
reactor 12.
Further, in these illustrative embodiments
one end of each conduit 62 is closed (upstream) so that
the incoming steam cannot flow directly into the conduit
62. Instead it flows about the catalyst 20 as has been
described.
In an embodiment of the catalyst system 20,
such as shown in Figure 9, the steam can be fed into
conduit 62 and the hydrogen can diffuse through the
hydrogen permeable central portion 64 and catalyst 20
into the reactor tube 18, while the remaining fluids
pass downstream through the conduit 62.
CONDUIT SYSTEM
As an introduction to the conduit system 30,
and in addition to the conduits already described, the
system 30 conveys fluids to and from the reactor 12 by
upstream manifolds 96 and 98 and downstream conduits
100a-h, and controls the flow of fluids through the
reactor 12 by a control circuit 102 connected to the
upstream manifolds 96 and 98.
In general, there are a pair of manifolds (96
and 98) upstream of the reactor 12, for conveying fluids
thereto, wherein each manifold has a circular conduit and
four spoke or branch like conduits which extend therefrom
and which are connected to four tubes 18. Specifically:
the upstrPam manifold 96 has a circular
conduit 104 and four inwardly extending
L-shaped curved conduits 106, 108, 110
and 112 threadably and removably connected
S to longitudinal bores 18a, c, e and g in
a fluid tight relationship (See Figures 1,
2 and 11); and
the upstream manifold 98 has a circular
conduit 114 and four inwardly extending
L-shaped curved conduits 116, 11~, 120
and 122 threadably and removably connected
to longi~udinal bores 18b, d, f and h in
a fluid tight relationship (See Figures 1,
2 and 11).
The control circuit 102 controls ~he flow of
fluids to and through ~he reactor 12 by selectively pro-
viding steam to produce hydrogen, and, as necessary,
hydrogen to reactivate the catalyst in the tubes 18a-h.
In the illustrative embodiment, the tubes 18
operate in two sets of four tubes each. When on s-tream,
hydrogen will be genera~ed in four tubes, e.g., l~a,
c, e and g, while the catalyst 20 will be regenerated
in the tubes 18b, d, f and h,between or adjacent to the
first set of tubes 18a, c, e and g. This process will
be reversed when the catalyst 20 in tubes 18a, c, e and
g becomes deactivated while the catalyst 20 in tubes 18b,
d, f and h has become regenerated. During each cycle,
moreover, the reacti~n in ~he tubes where catalyst re-
generation is occurring will provide heat which increases
j the amount of hydrogen being generated from steam in
`- adjacent tubes.
` 3S
, ~ , .
.
.
22-
O
In the illustrative embodimen~ of the inven~
tion shown in Figures 1 and 2, ~he circuit 102 includes
a rectangularl.y shaped loop about the boller 14 which
has four legs: two transverse legs 126 and 128, and two
longitudinal legs 130 and 132.
.,
Centrally connected into the transverse leg
126 is the steam conduit 42 with valves 134 and 136 on
either side thereof. Correspondingly, centrally connected
into the transversP leg 128 is a conduit 138 which conveys
a regeneration agent, such as hydrogen, from a source (not
shown) for the regeneration of catalyst 20. Here too
valves 140 and 142 are connected into the transverse leg
128 on either side of conduit 138.
' 15
! Centrally connec~ed into the longitudinal leg
130 is a pressure gauge 144 for measuring and controlling
steam pressure, and a conduit 146 for selectively con-
veying steam or regenerating agent to manifold 96. Simi-
larly centrally connected into the longitudinal leg 132
. is a pressure gauge 148 also for measuring and controlling
steam pressure, and a conduit 150 for selectively convey-
ing steam or regenerating agent to manifold 98. Typically,
the steam supplied to the reaction tubes 18a-h can be at
a controlled pre~sure of about 3 p.s.i.g.
Downstream of the reactor are the conduits lOOa-h
; connected ln fluid tight relationship to the downstream
end of the tubes 18a-h for conveying fluids, generated
30 hydrogen, oxygen and water vapor therefrom. From these
conduits lOOa-h the fluids are conveyed into a temperature
reducing means 152 where the fluids are collected and cooled.
From the temperature reducing means 152, a pair o condu~ts
. 154 and 156 convey the fluids through gas detectors 158
`35 and 160, which measure the yield of hydrogen, and into
~`
, ~
separators 162 and 164, where the fluids are separated
with the hydrogen being conveyed to the collectors 166
and 168 and the other fluids being conveyed to collectors
or separators 170 and 172.
; 5
The temperature reducing means 152 lowers the
temperatures of the fluids to increase the yield of hy-
drogen. Cooling prevents the gases formed from the steam,
hydrogen and oxygen, from reforming in~o water vapor or
water. The reduction in temperatwre also makes the fluids
easier to handle downstream.
In the illustrative embodiment shown in Figures 1,
2, 12 and 13, the temperature reducing means 152 is a water
cooled heat exchanger or quencher having a shell which
includes a chamber 176 formed by a cylindrical housing
178 and upstream and downstream end plates 180 and 182
welded to the inner periphery at the upstream and down-
stream ends of the housing 178. The cylindrical housing
includes a series of fins 184 to inerease the surface area
for coaling purposes, and the upstream and downstream end
plates 180 and 182 include central openings 186 and 188
therethrough.
; 25 Positioned within the chamber 176 spaced from
the housing 178 and end plates 1~0 and 182 for the circu-
lation of a cooling medium, such as wa~er, the quencher
152 includes manifold 190 having a central opening 192
therethrough and two outer annular chambers 194 and 196
formed by spaced annular partitions 198 and an outer two
segmented cover 200 welded thereto. Extending through the
central openings 186, 188 and 192 of the end plates 180
and 182 and the manifold 190 is an inner tube ~02 which
is welded to ~he inner periphery of the end plates 180
and 182. The manifold 190 also includes a plurality of
..
. .
`
- 2~
the longitudinal grooves 204 therethrough which, with
the space 205 between the inner tube 202 and the mani-
fold 192 deEine passages to facilitate the flow and
effectiveness of the cooling medium.
Extending from the upstream end of the mani-
fold 190 there are eight passageways 206a-h therewithin:
four passageways 206a, c, e and g extend into one annular
chamber 194 and four passageways 206b, d, f and h extend.
into the other annular chamber 196. In the illustrative
embodiment the downstream conduits lOOa, c 7 e and g
extend through bores 208a, c, e and h in ~he upsteam
end plate 180 and are connected in a fluid type relation-
ship into one set of pas~ageways 206a, c, e and g while
the other downstream conduits lOOb, d, f and h extend
through bores 208b, d, f and h in plate 180 and are
connected in a 1uid type relationship into the other
set of passageways 206b, d, f and h.
In use, fluids from the reactor 12 are conveyed
through the conduits lOOa-h and into the chambers 194
and 196 via the appropriate set of passageways 206a, c,
. e and g or 206b, d, f and h. For cooling these 1uids,
a conduit 210 is connected into the downstream end
plate 182 which conveys a cooling medium such as water,
from a source (not shown) into the quencher chamber 176.
For conveying the cooling medium from the chamber 176,
a conduit 212 is connected to the upstream end plate 180
and a reservoir (no~ shown). Within the chamber 176, the
cooling medium fl OW5 about the manifold 190 and through
the grooves 204 and space 205 about the inner tube 202
to reduce the temperature of the reactor fluids collected
: in the annular chambers 194 and l96.
- 25-
' For conveying the cooled reactor fluids down-
,'' stream of the quencher 152 ~he conduits 154 and 156
"' extend from the annular chambers 194 and 196, respec-
tively, and through bores 154a and 156a in the end
-, 5 plates 180 and 182.
. , .
The downstream gas detectors 158 and 160 pro-
vide a control over the productivity of the r~actor 12
and the reactivation o~ catalyst 20 in the tu~es 18a-h.
The gas detectors 158 and 160 indicate whether hydrogen
is being generated within each set of four tubes 18a,
c, e and g, and 18b, d, f and h, When a gas detec~or
158 or 160 shows little, or no hydrogen is being con-
veyed through the appropriate conduit 154 or 156, this
normally indicates that the catalyst 20 in the operatively
connected tubes 18 has been deactivated. The sequencing
of valves 134, 136, 140,and 142 in the upstream control
circuit 102 then is set to provide hydrogen and not
steam to the appropriate set of tubes to reactivate or
regenerate ~he catalyst 20 therein. Wh~n the gas detec-
tor 158 or 160 again provides high hydrogen readings this
indicate~ that regeneration of catalyst has occurred and
the steam cycle can commence again. At such time the
sequencing of the valves 134, 136, 140 and 142 is reset
to shut off the supply of hydrogen to such catalyst and
to convey a fresh supply of steam thereto.
In the illustrative embodiment, the gas indica
tors 158 and 160 are read by an operator and the valves
134, 136, 140 and 142 are set and reset manually. It is
within the scope of this invention to provide or automa-
tic means to open and close the valves 134, 136, l~'0 and
142 responsive to the detection of hydrogen or other fluids
in the conduits 154 and 156. Such automatic means can be
electrical, hydraulic, pneumatic or mechanical, or a com-
bination of such means.
'``' .
.
26 -
;' ~
Downstream of the quencher 152 and gas detec-
tors 158 and 160, the cooled fluids are separated with
the hydrogen and oxygen ready for use or collection.
In the illustrative embodi.ment ~he separators 162 and
164 are those disclosed in my earlier United States
Patent No. 3,967,589. Each separator 162 or 164 in-
cludes a tubular housing 214 in which there is dis-
posed an active microporous asymmetric membrane 216.
The membrane 216 is a thin, selectively permeable film
having a porous supporting substrate which has been
rolled to form a tubular asymmetric microporous membrane.
These membranes are sold by the Roga Division of Unlver-
sal Oil Products Company, 2980 Harbor Drive, San Diego,
California 92101 and are described in its brochure, Mem-
brane Production of Nitrogen Enriched Air For Fuel TankBlanketing Applica~ions, dated September 1974.
Extending through each membrane 216 and from
the downstream end of the housing 214 is a conduit 218
having perforations 219 (Figure 14) along the length
which lies wi~hin the membrane 216. Also, extending
from the downstream side of each housi.ng 214 is a con-
duit 220 which opens into space between the membrane
216 and housing 214.
As the fluids are conveyed from the conduits
154 and 156 into each housing 214, the pressure of the
fluids and the porosity of each membrane 216 is such so
as to allow only hydrogen to be diffused therethrough.
The separated hydrogen then passes through the perfora-
tions 219 in each conduit 218 and is conveyed downstream
ready for use.
At the same time the oxygen and water collected
in each housing 214 about each membrane 216 is conveyed
downstream by the conduit 220 where the oxygen can be
33; 167
-27 ~
separated from the water and used as desired.
.
As shown in ~he illustrative embodiment, the
separated hydrogen in each conduit 218 and the oxygen
and water vapor in each condllit 220 can be fed into t~e
appropriate collectors and separators 166, 168, 170 and
172.
OPERATION
, 10
Referring first to Figure 1, at start up, the
valves 134, 136, 140 and 142 are closed. Water, as
needed, is supplied to the boiler 14 through conduit
~` 38 and fuel is supplied to the burner 44 and ignited,
to thereby provide heat for the generation of steam and
heat for the tubes 18a-h and catalysts 20 therein. When
steam has been generated, valve 136 is opened and the
steam a~ a controlled pressure and flow rate is suppli~d
to a set of four tubes, e.g., tubes 18a, c, e and g,
via the upstream conduit 146 and manifold 96, wherein
the steam is elevated to temperatures at w~ich it re-
acts with the catalyst 20 in these tubes 18 to form
hydrogen and minor amounts of water vapor and oxygen.
These fluids are conveyed from tubes 18a, c, e and 8
through the downstream conduits 100a, c, e, and g ~nd
into quencher chamber 194 where the temperature of the
fluid is reduced by water circulating through the cham~
ber 176 and grooves 204 to inhibit reformation of the
hydrogen and oxygen gases. From the quencher 152 the
cooled fluids are conveyed into and through the separa-
tor 162 where only the hydrogen diffuses through the
membrane 216 into the conduit 218 and is conveyed to
the collector 166 ready for use. At the same time the
non-diffused fluids (oxygen and water vapor~ pass through
the housing 214 and into the conduit 220 and collector
170 or further processing, as desired.
..
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- 28-
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~;, This start up operation will continue until
,~ the downstream gas detec~or 158 indicates that meaningul
!~'' quantities of hydrogen are not being generated in the
~i ~ tubes 18a, c, e and g. This reading shows that the
`~ 5 catalyst 20 therein has been oxidized and become de-
, activated.
,. .
. At such timP, and now referring to Figure 14,
. valve 136 is closed and valve 140 is opened to provide
]0 hydrogen to the tubes 18a, c, e and g via upstream con
duit 146 and manifold 96 to regenerate the catalyst 20
therein. Concurrently valve 134 is opened to provide
,. steam to the other set of tubes 18bl d, f and h, via
the upstream conduit 150 and manifold 98, wherein the
steam reacts with catalyst 20 therein to produce hydro-
~, gen gas and minor amounts of water vapor and oxygen.
. .
With these ongoing concurrent operations, the
` heat from the exothermic reaction occurring in tubes
18b, d, f and g is used to generate hydrogen occurring
in ~he adjacent ~ubes 18a, c, e and g. Also, the amount
of fuel being supplied to the burner 44 can be reduced
because of the heat from the exothermic reaction is being
used to generate hydrogen.
From the reactor 12 the generated hydrogen and
minor amounts of oxygen and water vapor are cDnveyed
from tubes 18b, d, f and h through the conduits lOOb, d,
f and h into the quencher chamber 196. Simultaneously,
fluids, water vapor and gases, are conveyed from the
react~r tubes 18a, c, e and g, wherein the catalyst is
being reactivated, through the downstream conduits lOOa,
c, e and g into the quencher chamber 194. The fluids
in the quencher 152 are cooled by the water flowing there-
through to reduce the temperature thereof ~o inhibit r -
formation of the gases. A~ shown in Figure 14, from the
., .
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O
quencher 152 the fluids in chambers 194 and 196 are
fed into the separators 162 and 164 via-conduits 154
and 156 for recovering the hydrogen-generated in tubes
18b, d, f and h, as well as any residual amounts of
hydrogen not consumed in the reaction in regenerating
the catalyst 20 in tubes 18a, c, e, and g. In each
separator 162 or 164 hydrogen diffuses through each
membrane 216 and perforations 219 in the centrally
positioned condui~ 218 and is conveyed into collectors
166 and 168 ready for use. Simultaneously the fluids
which cannot permeate the membrane 216, e.g., wa~er
vapor and oxygen, pass about the membranes 216 and
through the conduits 220 into the separators 170 and
172.
These concurrent operations, which represent
the full cycle of operation, will continue until the
gas detector 160 for the tubes 18b, d, f and h indicakes
that hydrogen is no longer being produced in such tubes
in meaningful quantities because of deactivation of the
catalyst 20 therein. At this juncture the other gas
detector 158 operatively connected to the other tubes
18a, c, e and g will show meaningful quantities of hydro-
gen being passed through the conduit 154 which indicates
that the catalyst 20 in such tubes has been reactivated,
ready once again to produce hydrogen. The opening and
closing of the valves is reversed so that steam is sup-
plied through valve 136 to the tubes 18a, c, e and g
as hydrogen is -supplied through valve 142 to the tubes
18b, d, f and h, thereby reversing the reactions in each
set of four tubes.
Thus, by the pr~ctice of the present invention,
hydrogen i9 continuously produced ready for use upon
demand, where needed, as needed.
- 30
'.,;
.
s As an illustrative example of the hydrogen
generating system 10 shown in Fi$ures 1-2 and 9-14,
the reactor 12 i5 about 15 inches in length and 6.15
inches in diameter, while the centrally positioned
boiler 14 is about 10 inches in diameter. Typically,
the reactor tubes 18a-h, which also are about 15 inches
~, in length, are about 0.875 in diameter.
.:
As shown, the wat~r quencher 152 is about
5.0 inches in length and about 10 inches in diameter,
and the inner tube 202 has a diameter of about 3.125
inches. Within the quencher 152 ~he manifold 190 has
; a length of about 4.0 inches, and an outer diameter of
~` 15 about 6.5 inches.
'
Further in the illustrative embodiment of
~, Figure 14, a metering device 221 a~ the upstream ends
of each of the tubes 18a-h is provided which controls
the flow of steam and hydrogen thereinto.
'~In the embodiment where the catalyst becomes
`deactivated and is regenerated as just described, more-
over, a foametal catalyst of iron is used. Where the
``25 foametal catalyst of iron is wound in a spiral sheet 46
as shown in Figure 5, its length can be about 2.0 inches
and its diameter can be from about 0.5 to 0.625 inches.
Where the foametal catalyst of iron is the form of a
series of juxtaposed discs as shown in Figure 6, each
disc can be about 0.125 in thickness and the combined
length of the juxtaposed discs also can be about 2.0
~ inches in length.
,. :
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_ 31-
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-~ Whether the catalyst 20 is in the :Eorm of a
sheet or discs, the temperature of the steam in the
reactor is raised to about 1000F.-1800F., at which
temperature, and with such catalysts, the steam dis-
associates and hydrogen is generated.
.. ~
In the practice of the invention the required
quantities of fuel for the burner 44 and the regenerating
~` agent for the deactivated catalysts are substantially
; 10 less than the hydrogen generated, resulting in an effic-
ient system.
As will be described in the next several embodi-
ments, platinum type catalysts, which normally do not
need regeneration, can be used to achieve even greater
efficiencies.
~,,
FIGURES 15-18
Referring generally to this and other embodi-
ments of the invention hereinafter described, lik~
reference numbers refer to like parts of the system which
: have been already described.
In the embodiment shown in Figures 15-18, steam
; is fed from the steam generator 14 into the downstream
end of the reactor 12 wherein the steam flow~ in a ser
pentine path through interconnected tubes 18a-h contain-
: ing platinum type catalyst sytems 20.
As shown in Figure 15, steam is conveyed to
the downstream radial bore 2Bh of the reactor 12 by the
steam conduit 42 which includes a valve 222 and pressure
guage 224 that monitors and controls the pressure and
flow of steam therethrough.
. , .
~;~7
~ _ 32_
O
To provide the serpentine path for the flow
of steam within the reactor 12, a second set of trans-
~erse bores 24e-h in the downstream portion of the
reactor 12 connect alternate pairs of longitudinal
reactor tubes, i.e., 18b-c, 18d-e, 18f g and 18h-a
(See Figure 16).
Taken together the most downstream transverse
bore 24a-d, shown in detail in Figure 4, connect the
longi~udinal tubes 18a-h in pairs: 18a-b, 18c-d, 18e-f
and 18g-h while the next downstream -~ransverse bores
24e-h, shown in detall in Figure 16, connect the longi-
tudinal bores 18a-h in pairs: 18b-c, 18d-e, 18f-g and
18h-a.
As with their counterparts, transverse bores
24e-h also are threaded and are connected to threaded,
transverse access bores 25e-h. In each of these bores,
moreover, removable plugs 29 are provided.
In this embodiment platinum type catalyst sys-
tems 20, such as illustrated in Figures 8-10, can be used.
As has been previously explained with a platinum
type catalyst, deactivation normally does not occur and
regeneration is,therefore, not required. Accordingly,
feeding steam and a regenerating agent to a particular
tube 18 or set of tubes 18, on an alterna~ing basis, is
not needed. Also, downstream of the reactor 12, the
quencher manifold 190 need only have one cooling chamber
194 and there need be only one separator lS2 downstream
thereof. In addition, a downstream gas detector~ such
as detectors 158 and 160, shown in Figure 1, becomes
optional because hydrogen will be generated on a continu-
ous basis within the platinum type, catalyst containing
reactor tubes 18a-h.
~2~
~ - 33-
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As shown in Figure 17 radial. bore 26h has been
opened by removing the plug 29 therein and is connected
to the steam conduit 42 in a fluid tigh~ relationship.
At the same time the transverse bores 24e-g and bores
22a-d are opened by removing the plugs 29 while the
., remaining bores (transverse bores 24a-d and 24h and
radial bores 26a-h and 28a-g) are closed.
i,
In operation the burner 44, or other source of
heat, effects the generation of steam within the boiler
14 and the steam is fed from the boiler 14 to the reactor
tubes 18a-h through the conduit 42 under a control led
rate of flow and pressure, e.g., 3 p.s.i.g. The flow
rate and pressure is sufficient for passage of steam
through the interconnected tubes 18a-h and for disassocia-
tion of steam to hydrogen.
.~
From the conduit 42 the steam initially flows
through the radial bore 26h and into the adjacent end
of the reactor tube 18h. The steam within the tube 18h
`` is raised to disassociation temperatures of about 1000F.
;~ to 1800F. by the burner 44 and with the pla~inum type
catalyst system 20 effects disassociation. As previously
explained, only hydrogen is allowed to diffuse through
the platinum type catalyst 20 and into the catalyst con-
~`~ duit 62 for flow from the reactor 12 through conduit lOOh
into the water quencher 152. At the same time the steam,
~ which has not disassociated and the oxygen from the dis-
;` associated steam, flows about the catalyst 20 to the other
end of the reactor 12 and through the transverse bore 22d
and into the reactor tube 18gwhere the process is again
` repeated. As shown by the arrows indicating the flow of
'` steam, any remaining steam and disassociated oxygen moves
in a serpentine path through the remaining steam and dis-
associated oxygen moves in a serpentine path through the
:' .
~ 34-
O
remaining tubes 18f-18a and transverse bores 22c-a and
24g-e for further disassociation. The diffused hydrogen
in the conduits 62 and in the tubes 18a-h flows as
indicated from the reactor 12 through the conduits
lOOa-h into the quencher chamber 194. At the same time
residual steam and disassociated oxygen in ~he last
tube 18a are conveyed from the downstream end of the
reactor 12 through reactor bore 226 into a conduit 228
connected thereinto in a fluid type relationship. A
valve 230 in the condui~ 228 regulates the flow there-
through by throttling, to control, by back pressure,
the pressure of the fluids wq~hin the reactor tubes
18a-h and optimize the generation of hydrogen therein.
As illustrated, each of the conduits 62 of the
catalyst systems 20 also can be connected at their other
ends, in a fluid type relationship, with a manifold 231
which includes a control valve 232. In use, this control
valve 232 can be opened and closed to provide a positive
or negative pressure, as desired, for urging hydrogen
gas in the catalyst conduits 62 into the quencher 152 or
for exhausting gases from the catalyst conduits 62 through
the manifold ~31.
In addition, downstream of the quencher 152 the
cooled hydrogen gas can be fed into and through the pre-
viously described separator 162 to further ensure the
separation of hydrogen from any residual fluids which
may have diffused through the platinum type catalyst
along with the hydrogen.
FIGURES 18-20
In Figure 18 there is shown an embodi~ent of
the invention with 2 single upstream manifold 240 that
provides steam to the tubes 18a-h for generation of hydrogen
.
, ~
~ - 35 -
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: O
with either of the platinum type catalyst systems 20
shown in Figures 19 and 20.
Referring to Figure 18, the system includes
, 5 the previously described hydrogen generating reactor
" 12, steam generator 14, downstream conduits lOOa-h and
, quencher 152. The steam i9 conveyed from the generator
14 by the conduit 42 to the top of the single upstream
manifold 240 which includes a circular conduit 242 and
10 eight inwardly extending conduits 244a-h threadably
and removably connected to the reactor tubes 18a-h,
as has been described and illustrated for the dual mani-
folds 96-98 (see Figure 11). From the bottom of the
` circular conduit 242, a conduit 246 and valve 248 are
15 provided for drainage or for conveying gases or liquids
, from a source (not shown) to the reactor 12.
As shown in Figure 19 the steam from the con-
duîts 244a-h flows into the upstream portion of the tubes
18a-h and about the platinum type catalyst sys~ems 20.
At the elevated temperatures and pressures previously
described, and in the presence of the platinum type
catalyst systems 20, the steam disassociates into hydro-
gen and oxygen gases with the hydrogen diffusing through
the catalyst into the conduit 62. Simultaneously, oxygen
and residual steam flows into the downstream portion of
the tubes 18a-h where they are removed via a manifold 250
having conduits connected into the downstream radial bores
28a-h in a fluid tight relationship. A valve 254 in the
manifold 250 is provided to control flow and pressure in
the manifold 25~,~nd tubes.l8a-h By controlling the
~ opening in the manifold 250 the pressure of the fluids
`, in the tubes 18a-h can be increased or decreased for
optimizing disassociation and diffusion of hydrogen through
` 35 the platinum type catalyst systems 20.
. ~ .
~%~3~i7 ~
,;,
0 - 36~
,~ O
Concurrent with removing oxygen and residual
steam from the tubes 18a-h, the hydrogen gas is conveyed
from the reac~or 12, through conduits 100a-h and into
, quencher chamber 194. The cooled hydrogen gas is fed
into conduit 154 and, if desired, into and through the
`' separa~or 162.
,
In the embodiment of the invention schematically
shown in Figure 20, the steam from conduit 42 is fed into
the conduits 62 of the catalyst system 20, wherein the
hydrogen diffuses outwardly into the tubes 18a-h while
the disassociated oxygen and residual steam flows through
closed ended conduits 62 into the downstream manifold
250 through intercormecting radial passageways 28a-h.
In thls instance, the diffused hydrogen flows about the
~ catalyst systems 20 downstream and in~o the conduits
'` 100a-h for quenching and separation, if desired, ready
~ for use upon demand.
,,
In the following embodiments of the invention,
we describe illustrative overall systems which incorporate
the hydrogen generating systems. These overall syst ms
include boilers, gas turbines, internal combustion engines,
wankel engines, stirling engines and hydrogen cells.
THE ENERGY SYSTEM IN A BOILER
, ~
` Referring first to Figure 21, there is shown
a boiler 300 within which the energy system 10 of the
invention is positioned.
.
The boiler 300 includes an upright cylindrical
`~ tank 302 on supporting legs 304. Water is supplied ~o
` the bottom of the tank 302 by an inlet conduit 306, and
`~ ` 35 steam for heating and working purposes in conveyed from
the tank 302 from the outlet conduit 308 extending from
the top thereof.
,
:'
-37
O
Centrally positioned within the tank 302 is the
reactor 12, in an upright position, with vertical tubes
18a-h and catalyst systems 20 about a vertical heat
generating chamber 16. Extending into the chamber 16
is the burner 44 providing an air-fuel mixture to the
lower portion therof. As shown, ~he catalyst systems
20 are in the lower portions of ~he tubes 18a-h and the
burning air-fuel mixture from the burner 44 impinger,
on said portion. To minimize heat loss a baffle 310
is centrally positioned within the chamber 16 above the
burning air-fuel mixture. In the illustrative embodiment
the baffle 310 is a spiral wound coil with its outer
periphery secured to the outer wall 312 of the chamber
16. Any residual heat that does escape is exhausted
from the chamber 16 through the exhaust pipe 45.
Compressed air for the burner nozzle 44 is pro-
vided in this embodiment by a motor driven centrifugal
blower 314 having a duct 316 extending from the blower
20 outlet 318 into the chamber 16. Fuel for the burner
nozzle 44 is supplied by the generated hydrogen as here-
after described and by fuel lines 319 havîng a supply
and return conduits 320 and 322 connected to a fuel pump
324, and a conduit 326 connected to a common fuel-hydrogen
conduit 328. The common conduit 328 extends through the
duct 316 to the burner 44 centrally positioned at the
outlet of the duct 316 in the lower portion of the cham
ber 16.
Steam for the reactor 12 is conveyed through
a conduit 330 connected to the top of the tank and to
the ups~ream side of the tubes 18a h via a manifold 331
which, in this embodiment, is in the lower portion of
the reactor 12. Hydrogen generated by the reactor 12
is conveyed from the top and downstream end of the reactor
. . .
s~-:
'`7
~, '
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38 -
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.,,
tubes 18a-h to and through a manifold and a conduit 333
which, in turn, is connected ~o the common conduit 328.
Control means, check valves 334 and 336, are
connected into the fuel and hydrogen conduit 326 and 333
j to control the flow of fuels to the burner 44.
-j During start up, the hydrogen check valve 336
is closed and the fuel check valve 334 is open. The
fuel a~ the burner 44 is ignited, and with the compressed
air supplied by the blower 314 throughout t~e operation,
burns to provide heat for the generation of steam in the
, tank 302.
, ~
~ 15 When the temperature of the water in the tank
, 302 has been raised and steam is being generated, it is
simultaneously conveyed from the tank 302 by conduit 308
for heating and working purposes, and by conduit 330 for
generating hydrogen. The steam in conduit 330 is fed
into the lower (upstream) por~ion of selected reactor
tubes 18, as previously described, wherein the steam
at the super heated temperatures reacts with the catalyst
20 to produce hydrogen.
~"
~S The generated hydrogen is then conveyed through
the upper (downstream) end of the reac~or 12. At this
juncture the hydrogen check valve 336 is opened and the
uel check valve 334 can be partially or entirely closed
so that hydrogen, with or without fuel, is ~onveyed ~o
the burner 44 via the common conduit 328.
.:,
When on stream, therefore, the generated hydrogen
~,` is the fuel source for the heat that produces steam in the
~"' tank 302 and hydrogen in the reactor 12.
.~ 35
~ `
,
'
:;
~ 39
O
THE ENERGY SYSTEM IN A GAS TURBINE
In Figure 22, there is shown the energy system
; 10 of the invention producing hydrogen fuel for operating
a gas turbine 400.
The gas turbine 400 includes an air compressor
;. 402, a combustion chamber 404, and a turbine wheel 406
within the chamber 404, wherein the compressed air and
fuel form a combustible mixture which drives the turbine
wheel 406.
The compressor 402 and turbine 406 are mounted
on a common shaft 408 which extends from the gas turbine
400 and which when rotated by the turbine wheel 406,
generates mechanical power useful in generating electricity.
Extending downstream from and connected to the
combustion chamber 404 is the reactor 12 wi~h its central
heating chamber 16 for receiving ~he hot exhaust gases of
combustion before they are exhausted downstream through
: exhaust pipe 45. About the reactor 12 is the boiler 14
with its conduit 3~ for supplying water and with its con-
duit 42 for supplying steam to the reactor 12 ~hrough an
upstream manifold 240.
:`
Prior to the generation of hydrogen within the
reactor 12, fuel is supplied to the combustion chamber
404 from a fuel line 412 having fuel supply and return
conduits 414 and 416 connected to a fuel pump 418. Down-
stream o~ the pump 418 the fuel line 412 is connected to
a hydrogen ~uel mixer 420 from which a conduit 422 extends
to the burner 44 in the chamber 404.
3iE~
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Initially a conventional starter motor 424
rotates the shaft 408 so that air is sucked in and
compressed by the rotating compressor 402 and conveyed
into the combus~ion chamber 404. At the same time fuel
is supplied by the line 412 to the burner 44 and ignited.
The compressed air and ignited fuel mixture burns and
rotates the turbine wheel 406 to drive the shaft 408,
independent of the starter motor 424, for providing the
desired mechanical power.
Once the turbine 400 is on stream, the gases
of combustion reach temperatures within the reactor 12
to generate steam in the boiler 14 and hydrogen fuel
from steam in the reactor tubes 18a-h, as previously
described. Within the tubes 18a-h the steam is elevated
' to disassociation temperatures in the presence of a pre
viously described catalyst system to produce hydrogen
fuel which is conveyed from a downstream manifold 410
and conduit 154 to the hydrogen-fuel mixer 420. With
the supply of hydrogen from the reactor 12, the amount
of fuel needed from the fuel line 412 is reduced or cut
off by the mixer 420 and is conveyed back to the return
fuel conduit 416. Accordingly, the generated hydrogen,
with or without fuel from line 412, is delivered to the
~' 25 burner 44 from the mixer 420 by conduit 422 -to provide
the combustible mixture for the combustion chamber 404.
THE ENERGY SYSTEM FOR A FOUR CYCLE
~ INTERNAL COMBUSTION ENGINE
`, 30 In Figure 23, there is shown the energy system
10 being used to produce hydrogen fuel for the four cycle
piston driven internal combustion engine 500 for land and
marine vehicles, such as automobiles, trucks, farm equip-
ment and boats.
; 35
; . ~1_
~:; o
The engine 500 is of the conventional type
~: and includes an engine block 502 having cylinders and
pistons, not shown, and a fan 504 for an air cooled
~ radiator 506 having conduits 508 and 510 for convey-
2~ 5 ing water to and from the engine block 502, and a con-
~ duit 512 for providing water to the radiator 556 as
i needed. As in conventional internal combus~ion engines,
there also is a carburetor 514 within which the air-fuel
mixture is formed for driving the pistons, and a mani-
` 10 fold 516 for exhausting the hot gases of combustion.
. .,
Initially fossil fuel, e.g., gasoline, is
provided to start and drive the engine 500 until it is
at normal operating temperatures which raises the water
to temperatures of about 180F. to 200F. The fuel is
supplied to the carburetor 514 by a fuel line 518 and
a fuel pump 520.
Once operating temperatures have been reached,
hydrogen is generated by the system 10 and is used as
a fuel for driving the engine 500. For this purpose the
` system 10 includes the reactor 12 through which the ex-
haust manifold 516 extends to provide heat for the pro-
duction of hydrogen and from which conduit 522 extends
to provide generated hydrogen to the carburetor 514.
: `
To provide steam for generating hydrogen, an
interconnecting conduit 524 extends from the hot water
" conduit 508 to a flasher 526 connected to the manifold
`: ~
516. In operation, the heat from the exhaust manlfold
516 generates steam in the flasher 526, and the steam
is conveyed from the flasher 526 to the reactor 12 by
~` conduit 528.
~; 35
.~
~`
,,
o
Within the reac~or 12 hydrogen is generated
from the steam provided by conduit 528. The generated
hydrogen is then conveyed ~o the carburetor 514 via
conduit 522. To insure ~hat only hydrogen reaches the
5 carburetor 514 there is provided a separator 162 in
the conduit 522 which, as previously described, allows
only hydrogen to pass therethrough.
When hydrogen is being delivered to the car-
10 buretor 514, a valve 536 in the fuel line 518 can cut
off or decrease the supply of fossil fuPl, as desired.
Thus, in this embodiment, fossil fuels initially
drive the engine until the engine reaches operating tem-
peratures when hydrogen from the reactor 12 can be used
to drive the engine 500.
THE ENERGY SYSTEM FOR A R0TARY
INTERNAL COMBUSTION ENGINE
In Figure 24 there is shown an energy system 10
of the invention which produces hydrogen fuel for driving
a Felix Wankel rotary internal combustion engine for
vehicles, boats, etc.
The engine 600 is of a conventional type, and
includes a block 602 for the rotor and combustion chamber,
not shown, a fan 604 for an air cooled radiator 606 hav-
ing conduits 608 and 610 for conveying water to and
from the block 602, a water pump 612 in the conduit 608
for circulating the water, a carburetor 614 within which
the air-fuel mixture is formed for driving ~he ro~or,
a fuel line 616 with a fuel pump 618 therein for provid-
ing fossil fuel to the carburetor S14, and a manifold 620
; for exhausting the hot gases of combustion.
~7
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:: About the maniold 620 is the hydrogen gener-
ating system 10 w~ich includes the reactor 12, the steam
. genera~or 14, the conduit 38 and valve 40 or providing
.: water to the steam generator 14, the conduit 42 for con-
5 veying steam from the generator to the reactor 12, the
water quencher 152 for cooling the hydrogen generated
within the reactor 12 and conveyed thereto by the con-
duits lOOa-h, and the conduit 154 for conveying the
cooled hydrogen to the carburetor 614 for driving the
rotor of the engine 600.
In this embodiment the water for the system
10 is delivered from a reservoir 622 by pump 623 connect
ed to the conduit 38.
''' 15
In operation, fossil fuel initially is provided
to the carburetor 612 via the fuel line 616 and fuel pump
618 for driving the rotor of the engine 600. When the
engine reaehes operating temperatures the valve 40 is
opened, and the exhaust gases flowing through the mani-
fold 620 and through the system 10 are sufficient to
generate steam within generator 14 from the water sup-
~, plied therein and to generate hydrogen within the reactor
i~ 12 în the presence of previously described catalyst sys-
, ~5 tem. From the reactor 12 the generated hydrogen is
conveyed via conduits lOOa-h into the water quencher
1.52 where the hydrogen is collected and cooled and de-
livered to the conduit 154. At this time the generated
~` hydrogen can be used to drive the rotary engine 600 with
or without fossil fuel. To effect ~he transition, the
control valves 624 and 626 in lines 154 and 616, respec-
tively, are regulated to provide the desired quantities
of hydrogen and fossil fuels.
.~ .
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Here again, fossil fuels initially are used
to ~rive the engine 600 until hydrogen is generated within
the reactor 12.
" .
, 5 THE ENERGY SYSTEM FOR A STIRLING ENGINE
. .
In general, 5tirling engines utilize a working
gas, such as hydrogen or helium, in a closed system to
drive pistons connected to the drive shaft of the engine.
The working gas moves continuously back and forth between
the hot space above the piston in one cylinder and the
cold space beneath the piston in the next cylinder.
Between these two spaces the gas passes through a heater
which heats the gas, a regenerator which stores and gives
off heat from the gas, and a cooler which cools the gas.
. .
As shown in Figure 25J the Stirling engine 700
includes heaters 702 which are positioned in the upper
chamber 704 and which are connected between the regenera-
tor 706 and upper side of the cylinders 708. Below theregenerators 706 are coolers 710 which are connected to
the opposite side of the cylinders 708 via passageways
712 (only partially shown).
The heat for the heater 702 is provided by the
combustion of an air-fuel mixture in the upper portion of
~ ~he chamber 70~. Fuel is supplied by a fuel injector 714
! connected to a fuel line 716, and air is supplied through
a turbulator 718 which provides flow patterns suitable
for combustion. The hot exhaust gases from the combus~ion
of the air-fuel mixture pass about the heater 702 so that
~ heat is transferred to the interior working gas. This
j illustrative Stirling engine is described in greater de-
tail in a brochure published by United Stirling (Sweden)
AB&CO.
~0~
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The system 10 for the engin~ 700 is positioned
within the upper chamber 704 of the engine 700, and
includes the steam generator 14 in the form of a coil
and the reactor 12 positioned within the generator 14.
Water is supplied to the steam generating coil 14 fro~
a water reservoir 720 by a pump 722 through the conduit
38 connected therebetween.
As schematically shown in Figure 26, the
reactor 12 is in the upright position and includes v~r-
tical reactor tubes l~a-h. In this embodimen~ there are
seven transverse bores at opposite ends of the tubes
18a-h (transverse bores 22a-g and 24a-g) for interconnect-
ing the tubes 18a-h. As illustrated upper transverse bores
22a, c, e and g and lower transverse bores 24b, d and f
are closed while the other transversP bores (upper trans-
verse bores 22b, d and f and lower transverse bores 24a,
c, e and g) are opened. With this configuration, steam
provided through interconnecting conduit 42 and radial
bore 26a flows through the reactor tubes 18a-h, and in
the presence of ~he catalyst systems 20, in a serpentine
path. The generated hydrogen and other fluids from the
reactor 12 are conveyed therefrom through radial bore 26h
and conduit 154 to the separator 162, which, as previously
described, separates the generated hydrogen from the other
fluids. As llOW will be explained, this hydrogen can be
used as the fuel for combustion in the chamber 704.
Initially the valve 726 in the fuel line 716 is
opened and the valve 728 in th~ conduit 154 is closed.
Accordingly, fuel, such as fossil fuel or other stored
fuel, is provided from a source, not shown, to the fuel
injector 714. The heat from the products of combustion
within the upper chamber 704 concurrently heats the working
gas in the heaters 7G2 as well as the water in the steam
:`
3~i7
-46 -
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generator 14 and the steam in the reactor 12 by passing
, therearound and therethrough the generator 14 and reactor
:~ 12. The hydrogen and other fluids generated in the
- reactor 12 flow through the conduit 154 to the separa-
: 5 tor 162 where only hydrogen is allowed to flow down-
stream. When the hydrogen fuel has reached appropri-
` ate levels, the valve 728 in the conduit 154 is opened
and the valve 726 ln the fuel line 716 can be closed or
throttled. In the event that the valve 726 is closed,
then only generated hydrogen will be supplied to the
fuel injector 714 as the fuel for the combustible mix-
ture. In the event that the valve 726 in ~he fuel line
716 is only throttled, then the hydrogen and the other
fuel will be mixed and supplied to the fuel injector
714 as the fuel for the combustible mixture.
Consequently, in this embodiment the heat for
the working gas for the engine 700 is used to generate
hydrogen which can be used as fuel for the combustible
mixture once the engine is at operating temperatures.
THE HYDROGEN GENERATING SYSTEM FOR FUEL CELLS
In a fuel cell electricity is generated by a
chemical reaction in which the reactants are continuously
fed to the cell as the reaction proceeds. One reactant
is a fuel, such as hydrogen, and the other reactant is an
oxidant, such as air or oxygen. So long as the reactants,
~ hydrogen and oxidant, are fed into the cell and the re-
; 30 ac~ion product, water, is removed from the cell, the
fuel cell generates power in the form of direct current
electricity.
In Figure 27 there is illustrated the hydrogen
generating system 10 which pxoduces hydrogen for a Francis
Bacon hydrogen-oxygen type fuel cell ~00.
~7
- 47
.
The fuel cell 800 includes a housing 802 and
a pair of spaced electrodes 804 and 806, such as porous
nickel electrodes. The electrodes 804 and 806 divide
the housing 802, into three chambers, 808, 810 and 812.
The intermediate chamber 810 contains an electrolyte
814, such as potassium hydroxide, which is conveyed to
and from the chamber 810 and a reservoir 816 through
conduit 818.
.
For the electrical generating chemical re-
action, air or oxygen is fed to and unreacted air or
oxygen is fed from ~he outer chamber 812 through a con-
duit 820. Simultaneously hydrogen gas is fed to the
; outer and opposite chamber 808 through an upper inlet
:15 conduit 822, and the unreacted hydrogen gas is convPyed
from the chamber 808 by a lower conduit 824. To remove
any condensate a collector 825 is provided in the con-
.duit 824. The direct current electricity generated
within the cell 800 is conducted between the electrodes
806 and 804 and the illustrative circuit 826.
In this fuel cell system, the hydrogen gas
is provided by hydrogen generating system 10 which in-
cludes the reactor 12 and the steam generator 14.
Water for the steam generator 14 is provided
from a reservoir 828. Make up line 830 is connected to
a source of water not shown. Pump return line is 832.
Water for the generator 14 is conveyed from the reservoir
828 by a pump 836 through the conduit 38 and control
valve 40 into the generator chamber 32.
Heat from burner 44 (or heat from another source)
raises the temperature in the reactor 12 to about 1000F.
to 2000F., whereupon steam is generated in the generator 14
:
~ -48 -
', ~
and conveyed ~o the reactor 12 through the conduit 42,
radial bore 28h and into tube 18h. The configuration.
of the bores within the reactor 12 is similar to that
` ~ shown in Figure 17 so that the steam passes about the
catalysts 20 in the reactor tubes 18h-a in a serpentine
path as previously described.
Within the tubes 18a-h the steam disassociates
into hydrogen and oxygen, and hydrogen passes through the
catalysts 20 into the conduits 62, interconnecting con-
duits lOOa-h and into the quencher 152. Pump 837 pro-
vides cooling wa~er from the reservoir 834 through thP
conduit 210 to a cooling chamber 176, and water is re-
` turned to the reservoir 834 through conduit 212.
15
At the same time disassociated oxygen, and any
~ residual steam, is conveyed from tube 18a through bore
:~ 226 and conduit ~38 to the reservoir 828. As shown the
disassociated oxygen can be removed from the reservoir
20 by conduit 838 which includes control valve 840 for such
purposes.
From the quencher 152 the cooled hydrogen gas
is conveyed to the separator 162 by the conduit 154 where
only hydrogen is allowed to diffuse through the membrane
216 and into conduit 218. Any residual oxygen and water
passes about the membrane 216 into ~he conduit 220 which
is connected at its other end into the reservoir 828.
Downstream, the conduit 218 is connected to
conduit 842. In the conduit 842 there is a pump 846 for
conveying the hydrogen to both condui~s 822 and 844.
One way valves 845 in conduits 218, 824, 844 and 822
insure the flow of hydrogen in the direction indicated
by the arrows.
~2~
:
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.
The hydrogen conveyed tv conduit 822 enters
the fuel cell chamber 808 ~o generate electricity while
the hydrogen in the conduit 844 is used with the pump
846 to increase the yield of hydrogen in the reactor
12 as will presently be described.
. "
From the conduît 844 ~he hydrogen is fed into
a manifold 848 connected to the conduits 62 of the cat-
alyst systems 20 in a fluid tight relationship as
1~ schematically shown in Figure 27. The pump 846 influences
the quan~ities of hydrogen gas diffused through the cat-
alysts 20 in the reactor tubes 18a-h by creating a nega-
tive pressure in the conduits 62 relative to the positive
steam pressure flowing about the catalyst 20 in these
same tubes 18a-h. In effect, the pump 846 continually
sweeps the diffused generated gases out o the reactor
~ 12. In doing so, the equilibrium on the steam side of
! the catalysts 20, within the tubes 18a-h, becomes upset
and causes further disassociation of the steam into hydro-
gen and oxygen in trying to maintain equilibrium.
~,
In this embodiment, therefore, the generated
hydrogen is used simultaneously to generate electricity
in a fuel cell and to increase the yield of the generated
hydrogen itself.
~` In addition to using hydrogen as a fuel, as
shown in the illustrative embodiments of Figures 21-27,
the hydrogen generated by the system 10 of the invention
can be used as a chemical in forming products and in
chemical processes. For example, the generated h~drogen
can be used in the manufacture of ammonia, nitrates,
amines and alcohols (e.g., methanol), as well as in the
hydrogenation of organic compounds. The generated hy-
`~ 35 drogen also can be used in steel making and other metal
, _
, ~
.
.
~2~
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industriesl the gasification and liquification of coal,
the recovery of shale oil, the production of protein
foods, and in total water management programs.
Thus, the invention in its broader aspects
is not limited to the specific described embodiments
and departures may be made therefrom within the scope
of the accompanying claims without departing from the
principles of the invention and withou~ sacrificing its
chief advantages.
