E. J. PYRCIOCH and H. R. LINDEN Institute of Gas Technology, Chicago, 111.
Pipeline Gas By High-Pressure Fluid-Bed Hydrogasificafion of Char This hydrogenation process yields hig h-methane-content gas directly in a fluidized bed reactor with bituminous coal char feed
METHAW,
the desired major constituent of pipeline gas. can be produced by direct hydrogenation of coal or char. T h e feed will be completely utilized if less than half of the more reactive constituents are hydrogasified and the residue is used as a source of hydrogen (6). However, smooth operation of a continuous fluid-bed reactor requires the use of nonagglomerating feeds such as lignite and low-temperature char. I n this study, the feasibility of producing high-methane-content fuel gas by continuous fluid-bed hydrogenolysis of a low-temperature bituminous coal char was demonstrated. S o major difficulties were encountered in operation of the fluid-bed reactor a t a n inlet hydrogen superficial velocity of only 0.06 foot per second at 500 to 2000 p.s.i.g. and 1400" to 1500' F. However, the results obtained with a 5-foot bed show that a more reactive feed material, such as bituminous coal pretreated under conditions developed in a n earlier study (7), a deeper bed, or a number of countercurrent stages, will be necessary to achieve both high conversions and high product gas heating values.
Experimental T o ensure positive control over bed depth, the hydrogasification unit was designed for parallel upward flow of pulverized coal or char and hydrogen, with discharge through a standpipe. The main problem was selection of the bed depth, hydrogen superficial velocity, and coal feed rate. At nominal design operating conditions of 1400' F., 1000 p.s.i.g., and 60- to 325-mesh particle size range, it was necessary to have sufficient agitation for free movement of the bed, sufficient gas residence time for utilization of most of the hydrogen feed, and hydrogen to coal ratios sufficient for gasification of a substantial portion of the coal feed. Tests made in glass models with carbon dioxide a t atmospheric pressure and temperature to simulate the mass ve-
590
locity of hydrogen a t reaction conditions confirmed the fluidization requirements reported by Clark and others (2). In a 2-inch diameter reactor with a 1-inch standpipe, adequate fluidization of a 5-foot char bed was obtained a t a superficial gas velocity of about 0.06 foot per second. This corresponded to a gas residence time of 1.3 to 1.4 minutes and, a t a char feed rate of about 4 pounds per hour, to a char residence time of 30 minutes and an equivalent hydrogen to char ratio of 20 standard cubic feet (SCF, measured at 60" F., 30 inches of mercury, and dry) per pound. I t appeared from batch reactor tests that these conditions should give acceptable gasification results ( 7 , 6 ) ; however, the reactor was designed to accommodate an approximately 9-foot bed. Equipment. The semicontinuous pilot unit consisted of an interconnected reactor, feed hopper. screw feeder, and residue receiver (see diagram). The reactor had an effective inside length of 113 inches, an outside diameter of 5 inches and an inside diameter of 2 inches. It was designed for a working pressure of 3500 p.s.i.g. at 1500' F. and was fabricated of 19-9 DL alloy. A standpipe controlled the height of the char bed and served for the removal of the residual char and product gases from the top of the bed. Self-sealing closures a t the top and bottom of the reactor were of the modified Bridgman type with a stainless steel seal ring. The feed hopper was fabricated of Type 316 stainless steel and had a n inside length of 120 inches, a n inside diameter of 5 inches, and a n outside diameter of 6.75 inches. I t was fitted with confined gasket-type closures a t the top and the bottom. Capacity of the hopper was about 40 pounds of char. Originally, a hopper with a n inside length of 60 inches and half of the present char capacity was used. T h e residue receiver had the same dimensions as the original hopper and was also fabricated of Type 316 stain-
INDUSTRIAL AND ENGINEERING CHEMISTRY
less steel. It was joined to the bottom of the reactor by a short tube and selfsealing closures. This receiver separated the product gas and the ungasified char. The product gas was passed through a porous stainless steel filter, a water-cooled condenser, and a bank of gas filters for final cleanup. Pressure on the hydrogasification unit was maintained by a n externally loaded backpressure regulator. .4rotating spiral screw with an outside diameter of j/s inch, a root diameter of 0.25 inch, and a pitch of 0.40 inch was used to feed char through a horizontal housing, 24 inches in length, which connected the feed hopper and reactor near the bottom of the two vessels. Commercial electrolytic hydrogen, recompressed to 3000 p.s.i.g., was fed from a manifolded cylinder bank through a pressure regulator. Flow was controlled by a manually operated needle valve and was metered by a plate orifice with flange pressure taps. The char bed (reaction) volume was 0.07391 cubic foot when a nominal 5foot standpipe (4.714-foot true height) of 1-inch diameter was used. The reactor cross-sectional area, based on a 2 X 1 inch annulus and corrected for two 0.25-inch diameter thermowells that extended the length of the reactor, was 0.01568 square foot. A sintered steel disk, of 0.0025-inch mean pore size, which was fastened to the standpipe just below the point where char from the screw feeder entered the reactor, served as a base for the char bed and as a distributor for the feed hydrogen as it entered the reactor below the disk. The reactor was heated externally by an electric furnace having eight individually controlled heating zones. Char bed temperatures were sensed in 10 locations with Chromel-Alumel thermocouples. Feed hydrogen and gas stream temperatures were also sensed with Chromel-Alumel thermocouples. Reactor pressure, differential pressure across the reactor, and differential
H I G H B.T.U. GAS pressure across the hydrogen orifice, were recorded by circular chart instruments. Product gas volume was measured with a wet test meter, and product gas specific gravity was indicated and recorded by a continuous gravitometer. Procedure, For the reported tests, a low-temperature bituminous coal char (Montour No. 10 mine), supplied by the Research and Development Division of the Consolidation Coal Co., was used. This material was produced in a fluidized carbonization process a t much more severe conditions than those employed in the earlier pretreatment study; in batch hydrogasification tests it produced a free-flowing residue but had significantly less reactivity than chars produced a t optimum pretreatment condirions ( 7 ) . It was selected for a study of process variables because of its ready availability and uniform properties and the prospect of minimum handling difficulties. Unlike the feed material employed in the laboratory semiflow study reported by Hiteshue and others ( 5 ) , the char was not impregnated with a catalyst. Feed batches were prepared by crushing and screening the char to a 60- to 325-mesh size and drying in air a t 110' C. in a forced-convection oven. After the char had been charged to the hopper, the preheated unit was purged with nitrogen and pressurized with hydrogen. T h e hydrogen orifice meter was then calibrated against the wet test gas meter, the desired hydrogen feed rate established, and the char screw feeder started a t a preset rate. Hydrogen was preheated to 150' F. before entering the reactor. Char was fed at nominal rates of 2, 4.5, and 6 pounds per hour, corresponding to screw feeder settings ranging from about 25 to 85 r.p.m. Precise adjustment of char rate by control of screw feeder speed was not practical. Hydrogen feed rates normally corresponded to a superficial velocity of about 0.06 foot per second, the level required to maintain free flow of char through the reactor; this was equivalent to rates ranging from 34 to 35 SCF per hour a t 500 p.s.i.g. to 130 to 133 SCF per hour a t 2000 p.s.i.g. Consequently, with the exception of a few tests a t a hydrogen rate higher than the minimum, the hydrogen residence time based on the free reaction volume with the 5 foot standpipe was nearly constant a t 1.2 to 1.5 minutes. T h e steady-state operating period began when the product gas specific gravity reached a constant value. A composite gas sample was continuously bled into a 10-cubic foot water-sealed gas holder during the steady-state period; spot gas samples were also taken period-
ically TO confirm other observations relating to attainment of steady operating conditions. Upon termination of the test, which normally lasted from 4.5 to 5.5 hours, the unit was depressurized, purged, and allowed to cool. Char remaining in the feed hopper, solid residues. and condensed liquids were then removed and weighed. Samples of char feed and solid residues were subjected to proximate, ultimate, and sieve analyses, and their heating values were determined. Product gases were analyzed with a Consolidated Engineering Co. Model 21-103 mass spectrometer. Carbon monoxide content was determined by infrared analysis with a Perkin-Elmer Model 12-C infrared spectrometer. The properties of the composite gas samples and the char and residue weights corrected to a dry basis were used in the computation of hydrogasification test results. T h e char feed rate was computed from the difference between the charged and recovered weights and from the total feed time. Hydrogen and product gas volumes for the steady-state period are reported as standard cubic feet (SCF) on a dry basis. Gas heating values and specific gravities were computed from the gas analysis; heating values are reported a t 60" F., 30 inches of mercury pressure, and saturated with water vapor, whereas specific gravities are for dry gas referred to dry air. Hydrogen residence times and super-
ficial velocities were computed for average reactor temperatures based on measurements taken 1, 8, 18, 28, 42, and 54 inches above the bottom of the char bed. The low temperatures a t the bottom were partially responsible for the substantial difference between the average and maximum temperatures; the latter closely approached the nominal temperature levels of 1400' and 1500' F. Results and Discussion Typical properties of the feed char and the hydrogasification residues a r e given in Table I, and selected results for operation a t 500, 1000, 1500 and 2000 p.s.i.g., 1400" and 1500' F. nominal temperature. and char feed rates of 1.6 to 6.3 pounds per hour are given in Table 11. Key hvdrogasification results for all runs made with lowtemperature bituminous coal char a t 1400' F. are plotted against char feed rate expressrd as space velocity or reciprocal space velocity (see figure). Char residence times can be computed by assuming a typical bulk density of the expanded bed of 25 pounds per cubic foot. T h e plotted data exhibited the expected trends. T h e percentage of char hydrogasified (on a moisture- and ashfree basis) increased as pressure and hydrogen rate were increased in proportion and as char space velocity was decreased. T h e percentage of carbon gasified was about the same as the per-
Hydrogasification of char was studied in a semicontinuous fluid-bed pilot unit designed for operation at 3500 p.s.i.g. and 1500' F. VOL. 52, NO. 7
JULY 1960
59P
centage of moisture- and ash-free char hydrogasified (Table 11). The increase in char conversion was accompanied by a n equivalent increase in the quantity of feed hydrogen reacted-the difference between the amount of hydrogen fed and the amount of unreacted hydrogen contained in the product gas, both per pound of dry char. T h e net B.t.u. recovery-the difference between the heat of combustion of the product gas and the heat of combustion of the feed hydrogen, both per pound of dry charalso exhibited the same trends as the conversion of char to gas. The gaseous hydrocarbon (mostly methane) space-time yield increased with increases in pressure, as well as with increases in char space velocity a t constant pressure and nearly constant hydrogen feed rate. As there was no clearly defined tendency for a shift in the source of the hydrogen contained in the gaseous hydrocarbons, the effect of char feed rate must be primarily due to an increase in average reactivity of the char bed. The total feed hydrogen reacted per hour increased nearly in proportion to the gaseous hydrocarbon formation and corresponded to 80 to 100% of the hydrogen contained in the gaseous hydrocarbons over the whole range of operating conditions, except for some tests a t 500 p.s.i.g. Conversely, the relatively small change in residual char properties with increases in char feed rate and pressure (Table I) is consistent with the assumption that the increase in the amount of hydrogen supplied by the char was also roughly proportional to the increase in gaseous hydrocarbon formation. At 500 p.s.i.g., a n increase in hydrogen rate to double the level required to maintain a minimum superficial velocity resulted in a measurable increase in char conversion, gaseous hydrocarbon space-time yield, and quantity of feed hydrogen reacted (Table 11). Similar results were obtained a t higher pressures when the hydrogen feed rate was increased. An increase in temperature from 1400' to 1500' F. a t 1000 p.s.i.g. also resulted in a small but significant improvement in hydrogasification results. The char feed and residue analysis data of Table I show that, in the course of hydrogasification, the volatile matter and oxygen-plus-nitrogen contents of the char were reduced to a small fraction of the original values, hydrogen content was reduced to about one half of the original value, and sulfur content remained about the same. The increase in moisture content was caused by water formation through evolution of bound water or reactions of oxygen-containing coal constituents and gasification products with hydrogen; most of this water condensed in the residue receiver and moistened the char residue. Systematic variations of residual char properties
592
with hydrogasification conditions appeared to exist, such as more severe reduction in hydrogen and volatile matter contents at the higher reaction temperature. The screen analyses of the feed and residual chars indicate some size reduction; however, analyses of the residues remaining in the reactor after shutdown showed this was not due to accumulation of larger particles in the reactor. Of considerable practical significance are the unexpectedly high gaseous hydrocarbon space-time yields obtained with the bituminous char a t 1400' F. A series of studies (3, 4, 7, 8 ) of the kinetics of Disco char gasification with hydrogen-steam mixtures and pure hydrogen in a fluid-bed batch reactor, a t pressures u p to 30 atmospheres (426 p.s.i.g.) and temperatures of 1500' to 1700' F., is of interest in this connection. Direct comparison is not possible, as results are reported as differential gasification rates-Le., rates corresponding to zero bed weight, which is equiva-
[
lent to conditions where no equilibrium hindrance or other inhibiting effects of reaction products exist. The integral gasification rates obtained in this study would, therefore, be expected to be lower than equivalent differential rates, although this difference should be relatively small a t low conversions. I t appears that, because of the lower reactivity of Disco char, differential rates of methane formation extrapolated to the conditions of the present study are substantially lower than the integral rates reported in Table 11. For example, in terms of the units employed by other workers (3, 4, 7, a), integral rates of methane formation in the 5-foot fluid bed a t 1500' F. and 1000 p.s.i.g. ranged from about 70 to 100 X 10-4 poundmoles of methane per pound-atom of carbon per minute over a range of about 50 to 20% carbon gasification; this is approximately equivalent to extrapolated differential rates for Disco char and pure hydrogen a t 1600' F. At the relatively low pressures and
[
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REACTOR TEMP = 1400°F: BED HEIGHT=4.7 F T . BED VOL. :0.074 CU. FT. PRESS., P S . I . G . = 500 0 ;70 1000 1500 2000 H p RATE, SCF/HR.= 0 34-35 0 64-67 A 61-67 0 93-102 V 130-133 Hz RES. TIME, M1N.z 1.3-1.4 1.3-1.5 1.3- 1.5 1.3- 1.4 60
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RECIPR. CHAR SPACE VEL., [ CU. FT. -HR./LB.) x 100
CHAR SPACE V E L O C I T Y LB./CU. FT. HR.
-
Hydrogasification yields from low-temperature char increase with pressure and hydrogen rate
INDUSTRIAL AND ENGINEERING CHEMISTRY
H I G H 9.T.U. high temperatures employed in the Disco char gasification study, steam was found to accelerate methane formation greatly, in addition to increasing char
Table I.
gasification by reactions leading to the formation of carbon monoxide, carbon dioxide, and hydrogen. However, the effect of steam on methane formation
GAS
decreased rapidly with increases in pressure. This was confirmed in exploratory fluid-bed tests with low-temperature bituminous coal char; steam
Analyses of Char Feeds and Residues Show No Agglomeration and a Large Decrease in Reactive Constituents Run
Operating conditions Reactor pressure, p.s.i.g. Max. reactor temp., ' F. Char feed rate, Ib./hrs4 Sample Proximate analysis, wt. % Moisture Volatile matter Fixed C Ash Total Ultimate analysis, wt. % (dry basis) C H S
Ash N 0 (by difference) Total Heating value, B.t.u./lb. (dry basis) Screen analysis, wt. %* 40 mesh 60 mesh 80 mesh 100 mesh 140 mesh +ZOO mesh +325 mesh -325 mesh Total
+
+ + + + +
19
17
45
13
52 1 1415 2.07
516 1405 5.95
1007 1405 1.92
1031 1410 0.26
Feed
Residue
0.1 17.2 74.7 8.0 100.0
Feed
Residue
-
7.1 3.2 79.9 9.8 100.0
-
0.4 17.1 74.4 8.1 100.0
77.6 3.15 0.93 8.0 10.32 100.0
83.6 1.55 0.95 10.6 3.30 100.0
77.4 3.32 0.93 8.1 10.25 100.0
12,877
13,035
0.0 0.0 5.2 22.0 10.0 33.0 20.6 9.2 100.0
0.0 0.4 1.2 17.8 11.2 33.0 26.0 10.4 100.0
-
-
0.0 17.4 75.1 7.5 100.0
-
6.2 3.8 78.7 11.3 100.0
84.7 1.82 0.89 9.8 2.79 100.0
78.7 3.19 0.93 7.5 9.68 100.0
83.9 1.57 0.76 12.0 1.77 100.0
4.3 3.6 82.7 9.4 100.0
-
13,214
12,765
0.0 0.0 7.2 21.6 8.4 34.6 19.2 9.0 100.0
12,839
12,889 0.1 0.4 10.1 10.6 18.4 23.8 27.2 9.4 100.0
-
7.0 4.2 79.9 8.9 100.0
0.1 17.6 74.2 8.1 100.0
-
-
77.6 3.38 1.05 8.1 9.87 100.0
84.4 1.82 0.97 9.6 3.21 100.0
13,256
12,133
0.0 0.0 1.2 10.2 8.6 32.0 35.0 13.0 100.0
0.0 0.2 2.8 14.2 9.2 31.6 24.4 17.6 100.0
0.4 0.2 2.2 7.6 15.4 20.0 29.6 24.6 __ 100.0
-
Residue
Feed
-
-
0.0 0.2 2.4 18.6 8.2 28.8 27.6 14.2 100.0
-
Residue
Feed
-
-
Run
Operating conditions Reactor pressure, p.s.i.g. Max. reactor temp., F. Char feed rate, lb./hr." Sample Proximate analysis, wt. % Moisture Volatile matter Fixed C Ash Total Ultimate analysis, wt. yo (dry basis) C
H S Ash
+
43
44
40
32
1015 1510 1.57
1001 1505 6.08
2012 1425 2.03
2004 1415 5.75
Feed
Residue
0.0 17.1 75.3 7.6 100.0
6.4 2.2 79.1 12.3 100.0
78.1 3.18 0.93 7.6 10.19 100.0
83.1 1.28 0.67 13.2 1.85 100.0
~
Feed 0.0 17.9 74.1 8.0 100.0
5.5 2.0 82.3 10.2 __ 100.0
78.4 3.19 0.85 8.0 9.56 100.0
85.5 1.25 0.67 10.8 1.78 100.0
-
0 (by difference) -Total Heating value, B.t.u./lb. (dry basis) 12,743 12,584 12,760 Screen analysis, wt. % b 40 mesh 0.2 0.2 0.0 0.2 f 60 mesh 0.4 0.4 80 mesh 9.4 9.2 1.0 100 mesh 12.6 11.4 5.6 140 mesh 18.6 14.6 19.2 +ZOO mesh 22.2 20.0 22.0 +325 mesh 25.7 31.8 26.8 -325 mesh 11.1 26.4 11.0 __ Total 100.0 100.0 100.0 a Based on weight of dry char. U. S standard sieve series. N
+ + +
+
-
Residue
12.966 0.2 0.2 2.8 10.4 20.8 23.4 27.8 14.4 ___ 100.0
Feed 0.0 19.7 73.1 7.2 100.0
Residue 10.0 4.4 74.2 11.4 100.0
-
-
78.5 3.22 0.93 7.2 10.15
82.7 1.73 0.78 12.7 2.09 100.0
1EGX13,011 0.0 1.4 9.0 12.8 11.6 25.2 32.4 7.6 100.0
-
12,432
0.1 19.7 73.0 7.2 100.0
78.5 3.22 0.93 7.2 10.15 100.0
0.2 1.8 13.2 12.7 20.0 21.7 19.7 10.7 100.0
-
NO. 7
5.6 4.1 79.1 11.2 100.0
83.4 2.20 0.93 11.9 1.57 100.0 13,142
13,011
0.2 0.2 3.0 5.8 13.8 18.4 27.8 30.8 __ 100.0
VOL. 52,
Residue
Feed
0.2 1.0 6.3 12.0 19.1 20.9 21.0 19.5 100.0
-
JULY 1960
593
fable II. High-Methane-Content Gas Is Produced b y Pressure Hydrogasification of Low-Temperature Char in a 5-Foot Fluid Bed Feed char: Low-temperature bituminous tool chor, Consolidation Coal Co. Montour No. 10 mine" Particle size: 60-325 mesh, U. S. standard sieve series. Char bed height: 4.714 ft. Char bed volume: 0.07391 cu. ft. Run 19
17
18
23
45
Operating conditions Reactor pressure, p.s.i.g. 52 1 515 516 502 1007 Reactor temp., F. Max. 1415 1405 1405 1405 1395 Av. 1340 1375 1315 1350 1380 Char rate, lb./hr. 2.07 5.95 2.47 1.92 5.89 HZrate, SCF/hr. 34.5 34.9 63.7 65.2 66.5 Hdchar ratio, SCF/ 25.8 lb. 16.68 5.86 34.7 11.08 Char space velocity, lb./cu. ft.hr. 28.0 80.8 33.5 79.8 26.0 Hydrogen residence time, m h b 1.35 1.34 0.71 1.33 0.67 Operating results Product gas rate, 30.4 55.6 52.8 SCF/hr. 35.8 59.9 Product gas yield, SCF/lb. 22.5 27.5 14.70 6.02 10.18 Product gas net B.t.u. recovery, 4.53 M B.t.u./lb. 2.99 1.58 2.57 1.82 Gaseous hydrocarbon spacetime yield, SCF/ cu. ft.-hr. 148 172 250 252 188 Net moisture-, ashfree char hydro42.7 gasified, wt. %" 26.4 15.2 25.7 17.6 14.4 C gasified, wt. % 42.7 23.7 11.5 23.7 Feed HZ reacted, 17.62 2.80 9.12 4.70 SCF/lb. 7.96 Char residue, lb./ lb. 0.591 0.765 0.483 0.687 0.706 Condensed liquid 0.019 0.055 0.027 0.017 0.003 products, lb./lb.d Residue moisture, 0.021 0.034 0.027 0.036 0.028 lb./lb. Material balance, 87.8 89.5 98.6 97.0 98.6 % 94.8 94.9 97.9 88.2 H balance, %* 100.2 Product gas properties Gas composition, mole % Nz 2.7 4.0 2.0 3.4 1.5
co coz
Hz CHI CZH6 Benzene Total
1.9 0.2 59.2 35.4 0.4 0.2
3.9 2.5 50.8 38.4 0.2 0.2 100.0
0.8 0.2 74.1 22.0 0.7 0.2
2.4 0.7 62.6 30.4 0.3
0.2 - 100.0 100.0 100.0
1.3 0.1 61.9 34.5 0.4 0.3
100.0
13
43
44
28
31
40
32
031
1015
1001
1518
1512
2012
2004
410 385 6.26 66.4
1510 1445 1.57 65.5
1505 1465 6.08 69.8
1405 1265 1.76 93.2
1435 1320 5.27 102.3
1425 1340 2.03 131.4
1415 1325 5.75 132.9
10.60
41.9
11.49
52.9
19.43
64.7
23.1
84.7
21.2
82.2
23.8
71.3
27.5
77.8
1.34 54.8 8.75 2.11
335 21.1 17.7 6.28
1.29 49.5 31.6 5.19
267 52.9 53.5 23.9
1.18 51.6 8.49 2.20
1.49 81.3
77.6
46.1
14.73
5.46
261
380 21.3 20.9 8.16
1.31
3.37
505
1.34 100.4 49.4 5.62
407
1.33 92.4 16.08 3.58
669
48.2 47.2
30.3 30.5
58.0 63.9
35.5 36.2
18.57
12.34
30.7
16.26
0.727
0.414
0.700
0.455
0.612
0.260
0.605
0.017
0.068
0.040
0.055
0.038
0.068
0.044
0.050
0.026
0.036
0.030
0.038
0.028
0.033
98.8 96.8
100.0 97.8
97.5 90.9
99.6 101.7
97.5 98.4
93.7 95.9
101.1 98.3
2.5 2.5 0.4 49.4 44.7 0.3 0.2
1.6 1.5 0.2 56.8 39.9
0.7 5.2 0.5 39.2 54.2 0.1 0.1 100.0
1.2 0.6 0.1 74.4 23.1 0.5 0.1 100.0
1.7 2.0 0.1 48.1 47.7 0.2 0.2 100.0
0.7 0.4 0.1 68.8 29.2 0.6 0.2 100.0
2.5 1.2 0.2 42.6 53.1 0.3
-
100.0
... ... - 100.0
-
0.1 100.0
Heating value, B.t.u./SCF (sat.) 562 568 478 523 564 624 584 687 482 646 530 678 Sp. gr. (air = 1) 0.295 0.370 0.216 0.288 0.275 0.374 0.294 0.396 0.207 0.343 0.234 0.369 Char bed volume/cu. f t . per min. Hz at reactor pressure and temp. Operating conditions and results based on weight of dry char. Wt. of product gas - wt. of H? in Based on H content of inlet and outlet streams, including moisture content Mostly water. 0 100 Wt. of moisture-, ash-free char of char feeds and residues, and assuming condensed liquid products to be water.
[
1.
addition u p to 1 mole per mole of hydrogen gave only small increases in gaseous hydrocarbon space-time yield a t 1500" F. and hydrogen partial pressures of 500 to 1000 p.s.i.g. Acknowledgment
T h e guidance and counsel of the Project Supervising Committee of the American Gas Association under the chairmanship of B. J. Clarke, and of M. A. Elliott, director of the Institute of Gas Technology, were very helpful.
594
Literature Cited
(1) Channabasappa, K. C., Linden, H. R., IND.ENC.CHEM.50, 637-44 (1958). (2) Clark, E. L., Pelipetz, M. G., Storch, H. H., Weller, S., Screiber, S., Zbid., 42, 861-5 (1950). (3) Goring, G. E., Curran, G. P., Tarbox, R. P., Gorin, E., Ibid., 44, 1051-65 (1952). (4) Goring, G. E., Curran, G. P., Zielke, C. W., Gorin, E., Ibid., 45, 2586-91 ( 1953). (5) Hiteshue, R. W., Anderson, R. B., Schlesinger, M. D., Ibid., 49, 2008-10 (1957).
INDUSTRIAL AND ENGINEERING CHEMISTRY
(6) Shultz, E. B., Jr., Channabasappa, K. C., Linden, H. R., Ibid., 48, 894-905 (1956). (7) Zielke, C. W., Gorin, E., Ibid., 47, 820-5 (1955). (8) Zbid.,49, 396-403 (1957). RECEIVED for review July 17, 1959 ACCEPTED January 14, 1960 Division of Gas and Fuel Chemistry, 136th Meeting, ACS, Atlantic City, N. J., September 1959. Study supported by the Gas Operations Research Committee of the American Gas Association with funds provided by the Promotion-AdvertisingResearch Plan of the Association.
