Liquefaction co-processing of coal shale oil at - Argonne National ...
Liquefaction co-processing of coal shale oil at - Argonne National ... Liquefaction co-processing of coal shale oil at - Argonne National ...
%I ,100 60 40 20 0 100 222 %I EO - 60 40 20 0 100 20 I .^^ I II I II 11111 11111111111l lllll 111, I I UOP PAH Fraction ITSL PAH Fraction NTSL PAH Fraction 0 100 200 300 400 5 0 amu Figure 2. LVMS Spectra. See Figure 1 for Sample Descriptions. See Text for Conditions. 239
PROCESS DEVELOPMENT STUDIES OF TWO-STAGE LIQUEFACTION AT WILSONVILLE C. W. Lamb, R. V. Nalitham Catalytic, Inc., Wilsonville, AL 35186 and T. W. Johnson Southern Company Services, Inc., Wilsonville, AL 35186 INTRODUCTION The Advanced Coal Liquefaction RAD Facility at Wilsonville. Alabama, has been in operation for over 12 years. It is the largest direct coal liquefaction pilot plant still in operation in the United States. Process investigations have evolved from the original study of the Solvent Refined Coal Process for making a clean solid fuel to the recent investigation of two-stage liquefaction processes for making clean distillate fuels. This paper presents results from the current study of various processing schemes designed to reduce the cost of fuels produced by two-stage liquefaction plants. Most important among these configurations is direct coupling of the thermal and catalytic reactors. Such close-coupled operation should lower the cost of two-stage fuels by increasing overall thermal efficiency and improving product quality. Results from W i l sonville runs are characterized by discussion of representative product yield and product quality data. Also, a comparison of performance and stability of Shell 324 and Amocat 1C catalysts is presented. Other pertinent tests in the close-coupled mode are discussed with particular emphasis on the effect of higher system space velocity and on the impact of solids recycle. PROCESS CONFIGURATION COMPARISON The integrated TSL (ITSL) mode and the close-coupled (CC-ITSL) mode are shown in Figures 1 and 2, respectively. In both modes, the reaction stages are integrated by the recycle of hydrotreated resid with the goal of producing "all-distillate'' yield slates. The CC-ITSL configuration differs from ITSL in that for the CC-ITSL mode, products from the thermal reactor are fed directly to the catalytic reactor without pressure letdown or significant cooling. Accordingly, vacuum-flashed product from CC-ITSL is deashed downstream of the catalytic reactor rather than upstream as in the ITSL mode. Close-coupled operation thus eliminates thermal inefficiency of the cool down/reheat cycle associated with deashing between reaction stages. PROCESS PERFORMANCE A wide range of thermal and catalytic stage operating conditions were investigated in the CC-ITSL mode to determine their effects on product yield structure and quaiity. For comparison purposes, Table 1 l ists five sets of CC-ITSL conditions and yields relative to one typical set of ITSL conditions and yields. Illinois No. 6 coal from Burning Star Mine was used in all the runs. An initial baseline run (250B) was conducted using aged Shell 324 catalyst to quantify the impact of coupling the reactors. No interstage-vapor separation was utilized in Run 250B, although a high pressure separator was installed and operated during the remainder of the run. The major effect of close-coupled operation was an increase in hydrogen consumption with a corresponding improvement in distillate product quality (Table 2). Hydrogen and sulfur values were significantly better for CC-ITSL (250B) when compared to ITSL (244). This improvement resulted from the fact that all the TSL product was derived from the 240
- Page 37 and 38: Temperature WHSV, G/hr/cc TABLE 6 C
- Page 39 and 40: z FIGURE 3 COAL REACTIVITY SCREENIN
- Page 41 and 42: COPROCESSING USING HzS AS A PROMOTE
- Page 43 and 44: - 3 - that product yields depend on
- Page 45 and 46: - 5 - occurs in the yields of aspha
- Page 47 and 48: Table 1 Analysis of Feedstocks Fore
- Page 49 and 50: THO-STAGE COPROCESSING OF SUBBITUMI
- Page 51 and 52: esult in retrogressive reactions ta
- Page 53 and 54: 8. 6. Ignasiak, L. Lewkowicz, G. Ko
- Page 55 and 56: Table 4 OVERALL MASS BALANCE FOR TH
- Page 57 and 58: BACKGROUND COAL LIQUEFACTION/RESID
- Page 59 and 60: system, which could be operated wit
- Page 61 and 62: TABLE 1 EFFECT OF LC-FINING~"' TEMP
- Page 63 and 64: Figure 1. SCHEMATIC OF LCI CO-PROCE
- Page 65 and 66: SIMULATION OF A COAL/PETROLEuII RES
- Page 67 and 68: 20 pseudocomponents was developed t
- Page 69 and 70: ottoms is less sensitive to the num
- Page 71 and 72: Low Pressure Separator A temperatur
- Page 73 and 74: 7. Gallier, P.W., Boston, J.F., Wu,
- Page 75 and 76: I I I I I I I I I 100- --- Experime
- Page 77 and 78: Coprocessing Schemes The coprocessi
- Page 79 and 80: processing 25,000 and 150,000 bbl/d
- Page 81 and 82: FIGURE 1 I DISTRIBUTION OF REFINERI
- Page 83 and 84: Table 1. Samples Analyzed PNLNumber
- Page 85 and 86: the coal itself. The chemical compo
- Page 87: - - ITSL PAH Fraction PAH Fraction
- Page 91 and 92: SUMMARY e The major effect of close
- Page 93 and 94: omw '??h 4NO WNID ?N? 000 wmm c9'1'
- Page 95 and 96: tl f 246
- Page 97 and 98: 248
- Page 99 and 100: qkCqQ r! o! 0 0 0 0 0 0 0 I-UH ')I
- Page 101 and 102: Materials The catalyst was shell 32
- Page 103 and 104: CONCLUSIONS Separation of a light h
- Page 105 and 106: Table 3. Results of activity testin
- Page 107 and 108: feed coal and plant configuration a
- Page 109 and 110: P1 #2 #3 114 115 #6 ITSL subbitumin
- Page 111 and 112: temperature, time and solvent power
- Page 113 and 114: TABLE 1 EXPERIMENTAL CONDITIONS AND
- Page 115 and 116: la Figure 1. lH-NMR spectra of samp
- Page 117 and 118: PERFORMANCE OF THE LOW TEMPERATURE
- Page 119 and 120: BENCH UNIT DESCRIPTION Process deve
- Page 121 and 122: Recycle Residuum Hydrogenati On Res
- Page 123 and 124: FIRST STAGE HRI'S CATALYTIC TWO STA
- Page 125 and 126: FIRST-STAQ COAL CONVERSION (W I IIA
- Page 127 and 128: REACTOR SOLIOS HTOROGEN/CARBON ATOl
- Page 129 and 130: TRANSPORTATION FUELS FROM TWO-STAGE
- Page 131 and 132: Process Identification LV% Of AS- R
- Page 133 and 134: Table I11 HYDROTREATING TESTS WITH
- Page 135 and 136: Table IV HYDROTREATING TO 0.2 PPM N
- Page 137 and 138: Table VI EFFECT OF BOILING RANGE ON
PROCESS DEVELOPMENT STUDIES OF<br />
TWO-STAGE LIQUEFACTION AT WILSONVILLE<br />
C. W. Lamb, R. V. Nalitham<br />
C<strong>at</strong>alytic, Inc., Wilsonville, AL 35186<br />
and T. W. Johnson<br />
Southern Company Services, Inc., Wilsonville, AL 35186<br />
INTRODUCTION<br />
The Advanced Coal <strong>Liquefaction</strong> RAD Facility <strong>at</strong> Wilsonville. Alabama, has been in oper<strong>at</strong>ion<br />
for over 12 years. It is the largest direct <strong>co</strong>al liquefaction pilot plant still in<br />
oper<strong>at</strong>ion in the United St<strong>at</strong>es. Process investig<strong>at</strong>ions have evolved from the original<br />
study <strong>of</strong> the Solvent Refined Coal Process for making a clean solid fuel to the recent<br />
investig<strong>at</strong>ion <strong>of</strong> two-stage liquefaction processes for making clean distill<strong>at</strong>e fuels. This<br />
paper presents results from the current study <strong>of</strong> various <strong>processing</strong> schemes designed to<br />
reduce the <strong>co</strong>st <strong>of</strong> fuels produced by two-stage liquefaction plants.<br />
Most important among these <strong>co</strong>nfigur<strong>at</strong>ions is direct <strong>co</strong>upling <strong>of</strong> the thermal and c<strong>at</strong>alytic<br />
reactors. Such close-<strong>co</strong>upled oper<strong>at</strong>ion should lower the <strong>co</strong>st <strong>of</strong> two-stage fuels by<br />
increasing overall thermal efficiency and improving product quality. Results from<br />
W i l sonville runs are characterized by discussion <strong>of</strong> represent<strong>at</strong>ive product yield and<br />
product quality d<strong>at</strong>a. Also, a <strong>co</strong>mparison <strong>of</strong> performance and stability <strong>of</strong> Shell 324 and<br />
Amoc<strong>at</strong> 1C c<strong>at</strong>alysts is presented.<br />
Other pertinent tests in the close-<strong>co</strong>upled mode are discussed with particular emphasis on<br />
the effect <strong>of</strong> higher system space velocity and on the impact <strong>of</strong> solids recycle.<br />
PROCESS CONFIGURATION COMPARISON<br />
The integr<strong>at</strong>ed TSL (ITSL) mode and the close-<strong>co</strong>upled (CC-ITSL) mode are shown in Figures 1<br />
and 2, respectively. In both modes, the reaction stages are integr<strong>at</strong>ed by the recycle <strong>of</strong><br />
hydrotre<strong>at</strong>ed resid with the goal <strong>of</strong> producing "all-distill<strong>at</strong>e'' yield sl<strong>at</strong>es. The CC-ITSL<br />
<strong>co</strong>nfigur<strong>at</strong>ion differs from ITSL in th<strong>at</strong> for the CC-ITSL mode, products from the thermal<br />
reactor are fed directly to the c<strong>at</strong>alytic reactor without pressure letdown or significant<br />
<strong>co</strong>oling. Ac<strong>co</strong>rdingly, vacuum-flashed product from CC-ITSL is deashed downstream <strong>of</strong> the<br />
c<strong>at</strong>alytic reactor r<strong>at</strong>her than upstream as in the ITSL mode. Close-<strong>co</strong>upled oper<strong>at</strong>ion thus<br />
elimin<strong>at</strong>es thermal inefficiency <strong>of</strong> the <strong>co</strong>ol down/rehe<strong>at</strong> cycle associ<strong>at</strong>ed with deashing<br />
between reaction stages.<br />
PROCESS PERFORMANCE<br />
A wide range <strong>of</strong> thermal and c<strong>at</strong>alytic stage oper<strong>at</strong>ing <strong>co</strong>nditions were investig<strong>at</strong>ed in the<br />
CC-ITSL mode to determine their effects on product yield structure and quaiity. For<br />
<strong>co</strong>mparison purposes, Table 1 l ists five sets <strong>of</strong> CC-ITSL <strong>co</strong>nditions and yields rel<strong>at</strong>ive to<br />
one typical set <strong>of</strong> ITSL <strong>co</strong>nditions and yields. Illinois No. 6 <strong>co</strong>al from Burning Star Mine<br />
was used in all the runs.<br />
An initial baseline run (250B) was <strong>co</strong>nducted using aged Shell 324 c<strong>at</strong>alyst to quantify the<br />
impact <strong>of</strong> <strong>co</strong>upling the reactors. No interstage-vapor separ<strong>at</strong>ion was utilized in Run 250B,<br />
although a high pressure separ<strong>at</strong>or was installed and oper<strong>at</strong>ed during the remainder <strong>of</strong> the<br />
run. The major effect <strong>of</strong> close-<strong>co</strong>upled oper<strong>at</strong>ion was an increase in hydrogen <strong>co</strong>nsumption<br />
with a <strong>co</strong>rresponding improvement in distill<strong>at</strong>e product quality (Table 2). Hydrogen and<br />
sulfur values were significantly better for CC-ITSL (250B) when <strong>co</strong>mpared to ITSL (244).<br />
This improvement resulted from the fact th<strong>at</strong> all the TSL product was derived from the<br />
240