US1036609A - Method of conducting catalytic reactions. - Google Patents

Method of conducting catalytic reactions. Download PDF

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US1036609A
US1036609A US41172508A US1908411725A US1036609A US 1036609 A US1036609 A US 1036609A US 41172508 A US41172508 A US 41172508A US 1908411725 A US1908411725 A US 1908411725A US 1036609 A US1036609 A US 1036609A
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    • CCHEMISTRY; METALLURGY
    • C01INORGANIC CHEMISTRY
    • C01BNON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
    • C01B17/00Sulfur; Compounds thereof
    • C01B17/69Sulfur trioxide; Sulfuric acid
    • C01B17/74Preparation
    • C01B17/76Preparation by contact processes

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  • My invention relates to the production:
  • Figure 1 represents a plan view of one form of apparatus appropriate for the practice of my nventi0n, the top cover of the apparatus being removed.
  • F ,ig. 2 represents a' vertical sectional view thereof.
  • Figs. 3 and' i represent like views, respectively, of a modified.
  • FIG. 5 and 6 represent like views, respectively, of a further modification.
  • a indicates ⁇ the bottom plate of the apparatus and b the top plate thereof, said bottom andto'p plates being prov d w t a h k ay (if in -lating material a, so as to prevent loss of heat.
  • a indicates ⁇ the bottom plate of the apparatus and b the top plate thereof, said bottom andto'p plates being prov d w t a h k ay (if in -lating material a, so as to prevent loss of heat.
  • cold gases varying anywhere from 3% S0 about its center and made up by spiral walls 1 e, f, preferably of metal, said involuted. passage communicating at the two outerends thereof with an inlet 9 for the gases to be converted and an outlet h for the converted product, the involutions of the passage from its .central portion to either end being substantially parallel and adjacent throughout.
  • an involuted passage is provided leading spirally from the inlet 9 for the gases .to be converted, to the .center of the apparatus, and backagain by a similar spiral to the final exit of the converted gases, and the first spiral is, throughout its whole extent, flanlced on both sides by the inyolutions of the other spiral .Opens outinto the exit port Ii, as described.
  • the entire continuous passage may be filled with the contact material, which may be inserted therein in any suitable or convenient manner. A convenient method of supplying the contact material to the converter,
  • contact material of this type could be as readily removed from the apparatus by reversing its rotation upon the trunnions; or the apparatus may, if preferred, have doors in its top and bottom for the insertion and removal of the contact material.
  • the entire continuous channel formed by the two i i-going and out-going portions of the involute passage may be filled with contact material, when employing moderately weak gases, it is possible to economize the contact material by filling only the central zone of theapparatus therewith. In this case, however, I find it desirable to make the dividing walls between the zone containing the contact material and the outer zone of the contact chamber, of insulating material, as indicated at i in Fig.
  • this insulating material being to prevent the cooling of the contact mass by the outlying portion of the chamber containing the enteringgases, and preserving its heat, so that such heat may be utiliz'ed to the full extent practicable in maintaining the temperature of the inlet portions of the contact mass.
  • '-outer periphery of the apparatus may be protected against radiation by an additional jacketing of insulating material, a portion of which is indicated at s in Figs. 1 and 2. With richer gases, however, this precaution is not required, although it will in no way prevent the efficient conversion of said gases,
  • the length of the passage through the contact mass and the involution of the contact mass are sufiicient to allow the zone of maximum temperature to shift and broaden out in order to accommodate its action to the nature of the gases supplied.
  • This is illustrated by the upper and lower sets of arrows and the figures attached thereto.
  • the upper set of arrows indicates the conditions to be expected in converting a moderately weak gas, say from three to four per cent, by volume, of $0,.
  • the zone of active reaction is quite narrow and is confined well within the contact mass, occupying only four or five of the convolutions of the spirals, and the maximum temperature is reached at a point near the center of involution.
  • ]5 have indicated by heavy-line (black face) numbers the temperatures of the incoming gas, and by light-line numbers the temperatures of the out-going gas.
  • FIG. 3 and a another arrangement of the involuted contact chamber is shown, wherein, instead of being in the same plane and interwoven with each other, the two spirals into which the passageis involuted are superposed, so that the currents of gas traverse them in the same direction, the one over the other.
  • An advantage possessed by the arrangement shown in Figs. 3 and l and by that shown in Figs. 1 and 2 is that units of very large capacity can be built up in practically the same floor space upon identical foundations, and that the addition of each integer of the larger plant will improve the heat I inner portion only of thespiral, in which V event said inner portion or zone is provided with an insulating wall 2".
  • the entering gases are admitted throu h the intake 9 and the converted product lssues through the out-take h.
  • the most marked advantage possessed by the form of apparatus shown in'Figs. 3 and 4 is that the hottest particles of gas rising to the upper surface of the lower portion of the involuted passage of each unit or integer are brought immediately opposite the colder portions on the lower surface of thenppc'r portion of the involuted passage of said unit or integer.
  • the entering gases passing through the inlet-s g pass spirally within the contact chamber and either enter the contact mass immediately, provided that it fills the entire converter, or finally enter the contact mass when such mass fills less than the entire chamber.
  • the gases Upon reaching the center of involution the gases pass downward and thence outward through the contact mas-5 (and through the unoccupied portion of the lower part of the passage, if any unoccupied portion exists) until they reach the outer turn'of the lower part of the passage,
  • the broad underlying or characteristic principle of the invention resides in the circumstance that before the entering gas has reached the temperature of active conversion, it is introduced directly into the initial portion of the contact mass, in which it is gradually raised to the temperature of complete conversion, partly by local reaction, and partly, by heat communicated to said initial portion of the mass from that portion of the mass beyond the zone, of maximum temperature. After traversing the zone of maximum temperature, which may even be a bright red heat (and which zone I do not attempt to restrict in extent,
  • said gases being at a lower temperature than that of reaction on entering the mass, and at a temperature lower than that of dissoci-ation on leaving it,-and likewise conducting the said gases before entering-the contact mass in a path adjacent to the converted product issuing from the contact mass; substantially as described.
  • the method of conducting the catalytic conversion of gases which consists in continuously introducing said gases, at an entrance temperature below reaction into the presence of a preliminary portion of heated contact material, and elevating their temperature on the way to the zone of maximum temperature required for their conversion and cooling them as they leave said maximum zone by transference of heat to the preliminary portion of the contact material from the-egress portion thereof while retact mass. substantially throughout the operation; substantially as described.
  • the method of conducting the catalytic conversion of gases which consists in introducing the gases below their reaction temperature into heated contact material, allowing the conversion thus initiated and the transfer of heat from other portions of the contact mass to raise the temperature to the maximum that may be generated by the reaction and of so involvmgthe path of the 1 gases through the contact material that their point of removal therefrom shall be adjacent to the point of entrance of said .gases and shall be cooler than the temperature of dissociation; substantially as described.

Description

3 SHEETS-SHEET 1.
Patented Aug. 27, 1912.
W. M. GROSVENOR.
METHOD OF GONDUGTING CATALYTIC REACTIONS.
APPLICATION FILED JAN.20. 1908.
tNVENTORZ ATTURKHJ WITNESSES W. M. GROSVENOR.
METHOD OF CONDUCTING CATALYTIC REACTIONS.
APPLICATION FILED JAN. 20. 1908.
1,036,609, Patented Aug. 27, 1912.
3 SHEETS-SHEET 2.
ATTORN EYS,
W. M.-GROSVENOR. METHOD OF GONDUGTING CATALYTIC REACTIONS.
APPLICATION FILED JAILZO, 1908.
1,036,609. Patented Au 27, 1912.
3 BHEET8SHEBT 3.
ITNESSE INVENTOR w W ATTORNEYS.
sire snares ears rein WILLIAM M. GROSVE'NOR, 035 NEW YORK, N. Y.
METHOD OF CONDUCTING CATALYTIC REACEIONS.
Specification of Letters Patent.
1 Patentednug. 27,1912.
Application filed January 20, 1908. Serial No. $11,725.
To a l wit-am it may concern:
Be it known that 1, WILLIAM M. Gnosvnnon, a citizen of the United States, residing at New York, in the county of New York and State of New York, have invented certain new and useful Improvements in Methods of Conducting Catalytic .Reactions; and I do hereby declare the follow-' ing to be a full, clear and exact description of the invention, such as will enable others skilled in the art .to which it appertainsj to make and use the same.
My invention relates to the production:
of catalytic reactions by means of contact materials as, for instance, in the conversion of a mixture containing S0 and into S0 by means of platinized substances, such as platinized asbestos, or other like catalytic material.
In carrying out my invention, I first raise the body of catalytic material employed in theconverting apparatus ,to a'teinperature ap propriate'to the conversion required, and I thereafter maintain the necessary temperature of reaction within the apparatus by the heat developed by the reaction of fresh quantities of the gases to be converted, supplied in arelatively cool condition to the contact mass, the temperature of the inflowng eases bein perature thereof. This initial heating of far below the reacting ternthe catalytic material may be accomplished; 1n any 'convenlent manner, as, f r xamp e.
by means of a hot blast of air (or any other gas that will not poison the catalytic ma well-known way, followed by the action of \terial) blown through the apparatus in any} the cool gases'to be converted, which re-' move the heat from the outlying portions ofthe contact mass concentrating it toward thecsnter. At the same time, .the temperature within the contact mass itself is ,rnaintained at the desired elevation, by means of heat, transmitted from the outgoing converted gases to the initial portion of the contact mass through which the gases to be converted are entering, and the entire contact mass is so jacketed or insulated against radiation of heat that, commercially speak- "ing, practically all of the heat of reaction developed in the contact mass is available forntilization within the contact mass itself.
'By the practice of my invention, it is made possible, in the manufacture of sulfuric acid by the contact process, to supply gtiQIi of the contact mass to another.
In the accompanying drawings, Figure 1 represents a plan view of one form of apparatus appropriate for the practice of my nventi0n, the top cover of the apparatus being removed. F ,ig. 2 represents a' vertical sectional view thereof. Figs. 3 and' i represent like views, respectively, of a modified.
:form of the apparatus. Figs. 5 and 6 represent like views, respectively, of a further modification.
Similar letters of reference indicate Sll'Ill'. ;la r parts throughout'the several views.
Referring to the drawings, and particularly to Figs. '1 and 2 thereof, a indicates {the bottom plate of the apparatus and b the top plate thereof, said bottom andto'p plates being prov d w t a h k ay (if in -lating material a, so as to prevent loss of heat. Between the top and bottom plates {lS located a continuous passage involuted.
cold gases varying anywhere from 3% S0 about its center and made up by spiral walls 1 e, f, preferably of metal, said involuted. passage communicating at the two outerends thereof with an inlet 9 for the gases to be converted and an outlet h for the converted product, the involutions of the passage from its .central portion to either end being substantially parallel and adjacent throughout. {By thisexpedient, an involuted passage is provided leading spirally from the inlet 9 for the gases .to be converted, to the .center of the apparatus, and backagain by a similar spiral to the final exit of the converted gases, and the first spiral is, throughout its whole extent, flanlced on both sides by the inyolutions of the other spiral .Opens outinto the exit port Ii, as described. The entire continuous passage may be filled with the contact material, which may be inserted therein in any suitable or convenient manner. A convenient method of supplying the contact material to the converter,
would be. for instance, to mount the appawhich finally ratus temporarily or permanently upon trunnions, and to feed the contactmaterial into the involuted passage in the shape of small balls having a surface coating of the active mass; so, also, contact material of this type could be as readily removed from the apparatus by reversing its rotation upon the trunnions; or the apparatus may, if preferred, have doors in its top and bottom for the insertion and removal of the contact material.
Although, as I have just said, the entire continuous channel formed by the two i i-going and out-going portions of the involute passage may be filled with contact material, when employing moderately weak gases, it is possible to economize the contact material by filling only the central zone of theapparatus therewith. In this case, however, I find it desirable to make the dividing walls between the zone containing the contact material and the outer zone of the contact chamber, of insulating material, as indicated at i in Fig. 1, the purpose of this insulating material being to prevent the cooling of the contact mass by the outlying portion of the chamber containing the enteringgases, and preserving its heat, so that such heat may be utiliz'ed to the full extent practicable in maintaining the temperature of the inlet portions of the contact mass.
It 'will be apparent from what has been hereinbefore set forth, that the cold gases, introduced through the inlet 9 pass through the intake portion of the involuted passage to the axial center'of the apparatus, side by side throughout withthe gases passing away from the center and that they are everywhere flanked by said outgoing gases and insulated above and below by the insulating jackets 0, and that the gases passing away from the center of the involution finally, as shown, envelop the entire periphery of the apparatus, thereby inclosing all portions of the spiral passages and maintaining, as far as possible, the temperature of the contact mass within. As an additional means for preventing radiation, the
'-outer periphery of the apparatus may be protected against radiation by an additional jacketing of insulating material, a portion of which is indicated at s in Figs. 1 and 2. With richer gases, however, this precaution is not required, although it will in no way prevent the efficient conversion of said gases,
' inasmuch as the incoming gases always find themselves inclosed, within the, cont-act chamber between layers of gases passing away from the center of involution and having a higher temperature than the en tering ases.
It will be noted that colder portions of the contact mass, which colder portions are first encountered by the entering gases, are
- located within the succeeding or hotter portions of said mass, and it will be further noted that the length of the passage through the contact mass and the involution of the contact mass are sufiicient to allow the zone of maximum temperature to shift and broaden out in order to accommodate its action to the nature of the gases supplied. This is illustrated by the upper and lower sets of arrows and the figures attached thereto. The upper set of arrows indicates the conditions to be expected in converting a moderately weak gas, say from three to four per cent, by volume, of $0,. In such case, the zone of active reaction is quite narrow and is confined well within the contact mass, occupying only four or five of the convolutions of the spirals, and the maximum temperature is reached at a point near the center of involution. The lower set of arrows, and the figures attachedthereto indivcate the conditions to be expected when a large stream ofrich gas is supplied to the apparatus. In such case the reaction zone broadens very greatly and a practically neutral area appears in its center wherein reaction ceases substantially, the equilibrium of the reaction having been reached, as determined by the temperature of said maximum zone.
For convenience of illustration, ]5 have indicated by heavy-line (black face) numbers the temperatures of the incoming gas, and by light-line numbers the temperatures of the out-going gas.
In the form of apparatus shown in Figs. 3 and a, another arrangement of the involuted contact chamber is shown, wherein, instead of being in the same plane and interwoven with each other, the two spirals into which the passageis involuted are superposed, so that the currents of gas traverse them in the same direction, the one over the other. An advantage possessed by the arrangement shown in Figs. 3 and l and by that shown in Figs. 1 and 2 is that units of very large capacity can be built up in practically the same floor space upon identical foundations, and that the addition of each integer of the larger plant will improve the heat I inner portion only of thespiral, in which V event said inner portion or zone is provided with an insulating wall 2". The entering gases are admitted throu h the intake 9 and the converted product lssues through the out-take h.
The most marked advantage possessed by the form of apparatus shown in'Figs. 3 and 4 is that the hottest particles of gas rising to the upper surface of the lower portion of the involuted passage of each unit or integer are brought immediately opposite the colder portions on the lower surface of thenppc'r portion of the involuted passage of said unit or integer. The entering gases passing through the inlet-s g pass spirally within the contact chamber and either enter the contact mass immediately, provided that it fills the entire converter, or finally enter the contact mass when such mass fills less than the entire chamber. Upon reaching the center of involution the gases pass downward and thence outward through the contact mas-5 (and through the unoccupied portion of the lower part of the passage, if any unoccupied portion exists) until they reach the outer turn'of the lower part of the passage,
which is made sufiiciently high to entirely surround the converter considered as ,a whole, including the upper;portion,as shown in Fig. 4. I
The broad underlying or characteristic principle of the invention resides in the circumstance that before the entering gas has reached the temperature of active conversion, it is introduced directly into the initial portion of the contact mass, in which it is gradually raised to the temperature of complete conversion, partly by local reaction, and partly, by heat communicated to said initial portion of the mass from that portion of the mass beyond the zone, of maximum temperature. After traversing the zone of maximum temperature, which may even be a bright red heat (and which zone I do not attempt to restrict in extent,
position or temperature), it passes on into fart-her portions of. the mass, until it has again fallen below the temperature at which dissociation is possible; for the duration of the passage of the gas through the contact mass must allow extra contact material at both ends to permit of the shifting and expansion of the maximum zone.
It will be understood that whereas the arrangement of the involute passage is not re- (stricted to the substantially circular cong for the gases to be converted) alternate both vertically and horizontally with its out-going convolutions m which lattercornmunicate with the outlet port h for the (55nverted product. In Fig. 6, the course of the in-going gas is indicated by the n passages numbered from 1 to 42 and the course of the outgoing gases is indicated by the m passages numbered from 43 to 85 in said figure. It is, of course, obvious that in. order to insulate the apparatus shown in Figs. 5 and 6 against radiation of heat, it may conveniently be provided with an external jacket of asbestos, or the like, which jacket may completely envelop the involuted passage at top and bottom and at the center and circumference, leaving passage, how ever, for the inlet and outlet ends of the passage. A portion of said insulating cover is indicated at s in Figs. 5 and 6.
What I claim is I. The method of conducting catalytic conversion of gases, which consists in bringing an intermediate portionof the mass of contact material to a temperature suitable for the desired conversion, admitting the incoming gases into the presence of an initial portion of the mass at an entrance tempera ture belowthat of their reaction,-,and raising them to the temperature of completed conversion, partly by heat communicated to the initial portion of the mass fromthat portion of the mass beyond the zone of maximum temperature, and partly by the heat generated by local reaction; substantially as described, I
2.. The method of conducting catalytic, conversion of gases, which consists in bringing an intermediate portion of the mass of contact material to a temperature suitable for the desired conversion, admitting theincoming gases into the presence of an initial portion of the mass at an entrance temperature below that of their reaction, passing them on through an intermediate or central zone of maximum temperature of the mass, and finally through a succeeding egress zone of decreasing temperature of the mass until they have fallen below the temperature of dissociation,- and, during-the travel of the gases through the mass, eft'ecting a transfer of heat from the egress zone of the mass to the initial portion thereof; substantially as described. j
3. The method of conducting the catalytic conversion of gases, which consists in arranging the contact mass in an involute path, the return convolutions of which are adjacent to the incoming convolutions, bringing an intermediate portion thereof to a temperature suitable for the desired conversion, admitting the incominggases at an initial portion of the involute and at an entrance temperature below that of their reaction, passing them through the central the center of the contact mass initially heat;
ed to the temperature of reaction and thence returning them through the mass by a circuituous route adjacent to their ingoing.
' taming the gases ln'the presence of the conpath; substantially 'as describe'd.
' 5. The method of conducting the catalytic conversion of gases, which consists in conducting the gases by a circuitous route into the center of the contact mass and thence returning them through the mass by a circuitous route adjacent to their ingoing path, said gases being at a lower temperature than that of reaction on entering the mass, and at a-temperature lower than that of dissociartion on leaving it; substantially as described. 7 I V 6. The method of conducting the catalytic conversion ofgases, which consists in conv ducting thegases by a circuitous route into the center of ,the contact mass and thence -returning themthrough the mass by a circuitous route adjacent to their ingoing path,
said gases being at a lower temperature than that of reaction on entering the mass, and at a temperature lower than that of dissoci-ation on leaving it,-and likewise conducting the said gases before entering-the contact mass in a path adjacent to the converted product issuing from the contact mass; substantially as described.
7. The method of conducting the catalytic conversion of gases, which consists in continuously introducing said gases, at an entrance temperature below reaction into the presence of a preliminary portion of heated contact material, and elevating their temperature on the way to the zone of maximum temperature required for their conversion and cooling them as they leave said maximum zone by transference of heat to the preliminary portion of the contact material from the-egress portion thereof while retact mass. substantially throughout the operation; substantially as described.
8. The method of conducting the catalytic conversion of gases, which consists in introducing the gases below their reaction temperature into heated contact material, allowing the conversion thus initiated and the transfer of heat from other portions of the contact mass to raise the temperature to the maximum that may be generated by the reaction and of so involvmgthe path of the 1 gases through the contact material that their point of removal therefrom shall be adjacent to the point of entrance of said .gases and shall be cooler than the temperature of dissociation; substantially as described.
In testimony whereof I aflix my signature,
in presence of two-witnesses. WILLIAM -M. GROSVENOR.
Witnesses: t
JOHN C. PENNIE, LAURA B. PENrmLn.
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Cited By (9)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US2735839A (en) * 1950-12-27 1956-02-21 schrenk
US2735840A (en) * 1956-02-21 Vacuum pump
US2832674A (en) * 1954-08-23 1958-04-29 E F Drew & Company Inc Reaction tank
US2989383A (en) * 1958-02-14 1961-06-20 Fluor Corp Solid adsorber
US3432353A (en) * 1965-03-03 1969-03-11 Asea Ab Fuel cell electrode
US3467553A (en) * 1966-06-29 1969-09-16 Leesona Corp Fuel cell construction with involute reactant flow directing means
US3653844A (en) * 1970-02-02 1972-04-04 Phillips Petroleum Co Gas purification apparatus
US3849076A (en) * 1972-06-21 1974-11-19 V Gryaznov Catalytic reactor for carrying out conjugate chemical reactions
US9556025B2 (en) 2011-12-06 2017-01-31 Hydrip, Llc Catalyst-containing reactor system with helically wound tubular assemblies

Cited By (9)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US2735840A (en) * 1956-02-21 Vacuum pump
US2735839A (en) * 1950-12-27 1956-02-21 schrenk
US2832674A (en) * 1954-08-23 1958-04-29 E F Drew & Company Inc Reaction tank
US2989383A (en) * 1958-02-14 1961-06-20 Fluor Corp Solid adsorber
US3432353A (en) * 1965-03-03 1969-03-11 Asea Ab Fuel cell electrode
US3467553A (en) * 1966-06-29 1969-09-16 Leesona Corp Fuel cell construction with involute reactant flow directing means
US3653844A (en) * 1970-02-02 1972-04-04 Phillips Petroleum Co Gas purification apparatus
US3849076A (en) * 1972-06-21 1974-11-19 V Gryaznov Catalytic reactor for carrying out conjugate chemical reactions
US9556025B2 (en) 2011-12-06 2017-01-31 Hydrip, Llc Catalyst-containing reactor system with helically wound tubular assemblies

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