llllllllllllllllllllllllllllllllllllllllll||l|l|l|||lllllllllllllllllllllll US0054 72928A Uni.t ed States Patent [19] [11] Patent Number: 5,472,928 Scheuerman et al. [45] Date of Patent: Dec. 5, 1995 [54] CATALYST, METHOD AND APPARATUS 4,287,088 9/1981 Sirkar .................................... .. 252/414 FOR AN ONSTREAM PARTICLE 4,312,741 1/1982 lacquin . 208/11 LE 18128 21138 ---- "2323122 COUNTERCURRENT CONTACT OF A GAS 4,398,852 8/1983 Milligan 406/47 AND LIQUID FEED STREAM WITH A 4:4l1:768 10/1983 Unger at al. .. .. 208/59 PACKED BED 4,411,771 10/1983 Bambrick et al. .. 208/112 4,422,960 121983 Shiroto ct a1. 507/706 [76] Inventors: Georgieanna L. Scheuerman, 1155 4,444,653 4/1984 E1119“ et al. 208/152 Sanders DL’ Moraga, Calif_ 94556; 4,502,946 3/1985 Pronk ......... .. 208/152 David R. Johnson 7 Azalea Ct- 4,571,326 2/1986 Bischoi‘l' et al. .. .. 422/207 . ’ . ’ 4,576,710 3/ 1986 Nongbrl et al. .... .. 208/58 Pmluma’ Callf- 94954; Davld C- 4,590,045 5/1986 van derWal et a1. 422/216 Kramer, 54 Brookside Dr, San 4,639,354 1/1987 BlSCl'lOlf et a1. 422/140 Anselmo, Calif. 94960 4,684,456 8/1987 Van Driesen et al. 208/143 4,685,842 8/1987 Smith et al. .... .. 406/106 4,687,382 8/1987 Smith ...... .. 406/168 [21] APPl- NO-I 235,777 4,716,142 12/1987 Laine et al. 502/220 - 4,725,571 2/1988 Tusz ski 502/220 [22] Flled: AP‘- 29’ 1994 4,738,770 4/1988 nasnligs et al. 208/152 _ _ 4,744,887 5/1988 Van Driesen et al. 208/152 Related U-s-Appllcatwn Data 4,767,523 8/1988 Kukes et a1. .. 208/217 4,808,297 2/1989 Chen ....... .. 208/ 164 [63] Continuation-impart of Ser. No. 215,254, Mar. 21, 1994, 4,820,676 4/1989 Kukes et a1 ....... .. 502/220 Pat. No. 5,409,598, which is a continuation of Ser. No. 4,875,995 10/1989 Van Driesen et a1. 2081152 14,847, Apr. 1, 1993, Pat. No. 5,302,357, which is a con- 4,968,409 11/1990 Smith ................. .. 208/157 tinuation of Ser. No. 727,656, Jul. 9, 1991, abandoned, 5,008,003 4/1991 smegal et a1_ _____ ,_ 208/254 H which is a division of Ser. No. 381,948, Jul. 19, 1989, Pat. 5,021,147 6/1991 van Driesen et a1_ 203/152 NO- 5,076,908- 5,045,518 9/1991 Heinerman etal. 502/216 6 5,076,908 12/1991 Stan eland et al. . 208/148 [51] Int. Cl. .................................................... .. B01J 23/58 5,098,230 3,1992 Scheiflenmn ___________ __ 406/143 [52] U.S. Cl. ........................ .. 502/305; 502/337; 5021354; 5,209,340 5/1993 Shel-wood, Jr. et a]. 20g/21O 502/439; 502/527 5,232,673 8/1993 Notestein .............................. .. 422/216 [58] Field of Search ................................... .. 5021527, 354, 502,305, 337’ 439 FOREIGN PATENT DOCUMENTS 1217756 2/1987 Canada . [56] References Cited 1550285 8/1979 United Kingdom . U.S. PATENT DOCUMENTS Primary Examiner—.1anyce Bell 2,567,207 9/1951 Hoge ....................................... .. 196/52 ‘421392125?’ 121' J 061 1' DeYoung’ John W‘ Car' 2,631,968 3/1953 Peery . . . . . . . . . . . . . . . . . . . . .. 196/52 p ’ ' 2,688,401 9/1954 Schmitkons et a1. . 209/172 [57] ABSTRACT 2,987,465 6/1961 Johanson . . . . . . . . . . . . . . . .. 208/10 2,987,470 6/ 1961 Turken 208/253 This invention makes possible substantially continuous ?ow 3,336,217 8/1967 Me?llX 208/143 of uniformly distributed hydrogen and hydrocarbon liquid 3,398,035 8/1953 E9216 ------ -- 208/ 157 across a densely packed catalyst bed to ?ll substantially the 3,410,791 11/ 1953 Perry 6? a1- ----- -- 203/143 entire volume of a reactor vessel by introducing the ?uids as 3,410,792 11/1968 van Dnesen 6‘ al- 208/143 alternate annular rings of gas and liquid at a rate insu?icient 3,470,090 9/1969 Carson """"""" " 208/138 to levitate the catalyst bed. Catalyst are selected by density, lggjlgr'tkét'glm shape and size at a design feed rate of liquids and gas to 3’541’002 11/1970 Rapp ' 208/143 prevent ebullation of the packed bed at the design feed rates. 3:716:478 2/1973 K 208,152 Catalysts are selected by measuring bed expansion with 3,725,247 4/1973 Johnson et al. ..... .. 208/111 hydrocarbon’ hyiirogen’ alld ‘iatalyst at the deslg“ Pressures 3,730,880 5,1973 Van der Toom et al_ 208,213 and ?ow veloclties. The l1qu1d and gas components of the 3,841,981 10/1974 Layng ______________ __ 208,48 Q feed ?ow mto the bed in alternate annular rings across the 3,870,623 3,1975 Johnson et a1_ 208,103 full area of the bed. At the desired ?ow rate, such catalyst 3,880,569 4/1975 Bannister et al. ...... .. . 431/4 continually ?OWSiII aplug-like mannerdownw?rdly through 3,330,598 4/1975 van der Tom-n et a1, 23/239 the reactor vessel by introducing fresh catalyst at the top of 3,893,911 7/1975 Rovesti et a1. ...... .. 208/251 H the catalyst bed by laminarly ?owing such catalyst in a 3,915,894 10/1975 Clements et a1. . 252/439 liquid stream on a periodic or scmicontinuous basis. Catalyst 3,932,269 1/1976 Lehman 208/ 157 is removed by laminarly ?owing catalyst particles in a liquid 3,972,803 8/1976 Wolk et al. 208/97 stream out of the bottom of the catalyst bed. Intake for such 4,016,106 4/ 1977 Sawyer 6t a1~ 252/455 R ?ow is out of direct contact with the stream of gas ?owing 4,051,019 9/ 1977 Johnson ------ '- 203/146 through the bed and the ?ow path is substantially constant in 4,059,502 11/1977 JamFS ----- --_- 208/152 cross-sectional area and greater in diameter by several times 4,119,530 10/1978 cFalkPwskl etal- - 208/213 than the diameter of the catalyst particles. The catalyst 4,167,474 9/1979 sikonla ........... .. 208/140 produces a plug_?owing Substantially packed bed of hydro_ 4’172’024 10/1979 Sim?“ at 208,10 processing catalyst which occupies at least about 75% by 4,188,283 2/1980 czajkowski et a1. . 208/143 volume of the reactor volume 4,213,850 7/1980 Riddick, Jr. et a1. . 208/216 R ' 4,217,206 8/1980 Nongbli ............................ .. 208/251 H 4,259,294 3/1981 Van Zijil Langhout et al. .... .. 422/190 69 Claims, 10 Drawing Sheets US. Patent Dec. s, 1995 Sheet 1 of 10 5,472,928 FIGURE 1 US. Patent Dec. 5, 1995 Sheet 2 of 10 5,472,928 FIGURE 2 M21 M25 - M25 26 M 3 Z3 272 28 3 M12 + 211 + - 25 r 28 ' 27 ‘g? *8’ 2 271 72 23 27 27 214 274 275 12 2116 276 27 212 5 US. Patent Dec. s, 1995 Sheet 3 of 10 5,472,928 /7///////////////////////////A FIGURE 3 F nlu U R E 4 U.S. Patent Dec. 5, 1995 Sheet 4 0f 10 5,472,928 45 FIGUREB 4 9 FIGURES FIGURET US. Patent 5,472,928 Dec. 5, 1995 Sheet 5 of 10 FIGURE 8 18 42 14 19 /180 /é//////////////////////l//////9n/z////////////////9/////// ////// o9r lm //IrI// J/V91?/////11/7/1/0/I1/////1_///7/l////A1//1//V ! 121| k‘/n_4__/F_ _ 1 amw 0 2 1I L_w\ o3on 0 2 o3 |oo 0 oOO 3 o38o 63 V0 2o /oo m e 5 16 US. Patent Dec. 5, 1995 Sheet 6 of 10 5,472,928 FIGURE 9 19 I.‘ .. ////W///. // HGH Mr GFE11FE ‘11| I _.___..________._____./ 10 //////P//1 2 D1C4CE33BD7 _2..1 US. Patent Dec. 5, 1995 Sheet 7 of 10 5,472,928 N2ED.GE US. Patent Dec. s, 1995 Sheet 9 of 10 5,472,928 00Puu::Mmm WNmDFUE 01-1.. ..a : -u0?w0 M0.0 682.1. . ~2, 5 (00|:: amn. 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