CHEM ICAL JOU RNAL O F CH IN ESE UN IV ERS IT IES 10 15

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1 V ol. 22 N o CHEM ICAL JOU RNAL O F CH IN ESE UN IV ERS IT IES NaY (g ) (, ) (, ) N ay ( ), SiO 2gA l2o 3., N ay., n ( ) n ( ) 2 1,, N ay,. ; N ay; ; ; O A (2001) Y. Y nm [1 3 ]., Y,,, Y [4 14 ]., (< 100 nm ) Y., [15 19 ]., [15 ]. Bodart [16 ], Y 0. 8 Λm 0. 5 Λm. L inder [17 ],,,,,,. M aher [18 ],,, N, N 2, Λm. Am bs [19 ], Λm.,, SiO 2gA l2o 3, D utta [20 ],,. [20 ], (P recursors) [21 ],. N ay 0. 1 Λm, N ay, ED TA,. N ay,. : : ( : X598010). : (1967 ),,,,.

2 N o. 1 : N ay (g ) (26% SiO 2, 0. 8% N a2o, 73. 2% H 2O, ) [ (A l2 (SO 4) 3 18H 2O,, ]. (, ).. (, ) NaY 16N a2o A l2o 3 16SiO 2 210H 2O, 275 K rgm in. ( 293 K) 48 h, :, 3. 2N a2o A l2o 3 10SiO 2 160H 2O,, A l2o 3 10%.,,.,, 373 K,. N ay, ( ),. A l2o R igaku D gm A X2g A X, R IPP N orm R IPP N orm [22 ],. JEM 2000 FX2g gq X22000, ; B ruker DRX24000M H z, TM S A l2 (SO 4) 3, 29 Si 27 A lm A S2NM R, [23 ]. 2 A SA P22400,. 1 N ay 1. 5, 363 K N ay. 1. T EM 2. XRD, Y ,,, N ay,. 29 Si 27 A lm A S2NM R, N ay,. 3 1 N ay 29 SiM A S2NM R. 3,, N ay F ig. 1 Crysta ll iza tion curve of zeol ite NaY syn thesized a t Si(A ln) (n= 0 3), 363 K w ith differen t complex ing agen ts[ n (com -, plex ing agen t) n (A l2o 3) = ]. NM R XRD N ay. 2 N ay 1. 5, 373 K N ay K, K N ay

3 12 V ol. 22 Table 1 Effect of complex ing agen t on max imum crysta ll in ity, time to max imum crysta ll in ity, and SiO 2gA l2o 3 ra tio and average crysta l size a t max imum crysta ll in ity of zeol ite NaY syn thesized a t 363 K and n (complex ing agen t) n (A l2o 3) = A dditive Crystallization tim eg n (SiO 2) gn (A l2o 3) BET A reag Crystal sizeg Crystallinity (% ) h XRD NM R (m 2 g - 1 ) nm None Editate Citrate A cetate F ig. 2 TEM p ictures of zeol ite NaY syn thesized a t 363 K in the absence of com lex ing agen t(a), in the presence of complex ing agen t of edita te (B), c itra te (C) and aceta te (D ) respectively n (comp lexing agent) n (A l2o 3) = ,., [24 ].,, [25 ]. [17, 26, 27 ], SOD FAU,,., F ig SiM AS-NM R spectra of zeol ite NaY syn thesized, [28 ]. Kuh i [29 ] a t 363 K (a ) in the absence of complex ing agen t, ED TA in the presence of complex ing agen t of edita te (b),, OH -,, N ay. c itra te (c) and aceta te (d), respectively n (comp lexing agent) n (A l2o 3) = L inder [17 ],,, OH -,.,,.,,.,, OH -,.

4 N o. 1 : N ay (g ) 13 Table 2 Effect of complex ing agen t on max imum crysta ll in ity, time to max imum crysta ll in ity, and SiO 2gA l2o 3 ra tio and average crysta l size a t max imum crysta ll in ity of zeol ite NaY syn thesized a t 373 K and n (complex ing agen t) n (A l2o 3) = Crystallization tim eg n (SiO 2) gn (A l2o 3) BET A reag Crystal sizeg A dditive Crystallinity (% ) h XRD NM R (m 2 g - 1 ) nm None Editate Citrate A cetate N ay, OH -,,,, N ay,., 1 2, ( ),, N ay, ; F ig. 4 Crysta ll iza tion curve of zeol ite NaY syn thesized a t, N ay, 373 K ;, n (citrate) n (A l2o 3) : a. ED TA. e. 4. 0; f. 6. 0; g ; b. 1. 0; c. 1. 5; d. 2. 0;, : > >.,, A l N ay,,., N ay 373 K. Table 3 Effect of c itra te addition w ith differen t n (c itra te) n (A l2o 3) ra tios on max imum crysta ll in ity, time to max imum crysta ll in ity and n (SiO 2 ) gn (A l2o 3 ) ra tio and crysta l size a t max imum crysta ll in ity of NaY syn thesized a t 373 K Crystallization n (SiO 2) gn (A l2o 3) BET A reag Crystal sizeg n (citrate) n (A l2o 3) Crystallinity (% ) tim egh XRD NM R (m 2 g - 1 ) nm ,, N ay. [n ( ) n ( ) 2 1 ], N ay.,,, N ay ; [n ( ) n ( ) > 2 1 ],,,,,,, n ( ) n ( ) = 8 1, N ay, N ay.,,,

5 14 V ol. 22.,, A l2o , 1. 5,,,, L inder [17 ]. N ay L inder [17 ],.,.,., ;,,., L inder [17 ], N ax 5. 4 Λm 3. 5 Λm, 35%, N ay., N ay, L inder. ( 275 K) [4 ] A l 3+,. 4 N ay,,,. ( A l2o 3 2 ),,,, N ay, ;,,. ED TA,,,.,,. 1 Ciric J.. J. Coll. Inṫ Sci. [J ], 1968, 28: Tom H., Hennie S., A rend H. et al.. EP, A 1[P ], F reund E. F.. J. Crysṫ Grow th [J ], 1976, 34: CHAO Zi2Sheng. Post Ph. D. D issertation[d ], Research Institute of Petroleum P rocessing, S INO PEC, 1998: Pu S. B., Inui T.. Zeolites[J ], 1996, 17: Herrm ann C., Haas J., Fetting F.. App l. Catal. [J ], 1987, 35: V an der PolA. J. H. P., V erduyn A. J., V an der Hooff J. H. C. ; Edṡ, Ballmoos R. Von, H iggins J. B., T reacy M. M. J.. P roceedings of the 9th International Zeolite Conference[M ], M obtreal: Butterworth2Heinem ann, 1992: A guiar E. F. S., V alle M. L. M., Silva M. P. et al.. Zeolites[J ], 1995, 15: Thom as C. L., Barm by D. S.. J. Catal. [J ], 1968, 12: M aselli J. M., W. Peters A.. Caṫ Rev. Sci. Eng. [J ], 1984, 26: Rajagopalan K., Peters A. W., Edw ards G. C.. App l. Catal. [J ], 1986, 23: Cam blorm M. A., Corm a A., M artinez A. et al.. App l. Catal. [J ], 1989, 55: Pachovsky R. A., W ojchiechow skib. W.. A IChe J. [J ], 1973, 19: Shiralkar V. P., Joshi P. N., Eapen M. J. et al.. Zelolites[J ], 1991, 11: M yatt G. L., Budd P. M., P rice C.. Zeolite[J ], 1994, 14: Bodart P., N agy J. B., Gabelica Z. et al.. J. Chim. Phyṡ [J ], 1986, 83: L indner T., L echert H.. Zeolites[J ], 1996, 16: M aher P. K., Scherzer J.. U S Patent [P ], Am bsw. A., Sw arthmore Pa.. U S Patent [P ], Dutta P. K., PuriM., Bow ers C. ; Edṡ, O ccellim. L., Robson H. E.. Zeolites Synthesis, ACS Sym. Seṙ, ACS[M ], 1989, 398: Dutta P. K., Bow ers C.. Zeolits[J ], 1991, 11: YAN G Cui2D ing ( ), GU Kan2Ying ( ), WU W en2hui( ). A nalysis M ethod in Petrochem ical Industry2R IPP Norm ( 2R IPP ) [M ], Bejing: Science P ress, 1990:

6 N o. 1 : N ay (g ) klinow aki J., Ram das S., Thom as J. et al.. J. Chem. Soc., Faraday T ranṡ g [J ], 1982, 78: Sano T., O kabe K., Kohtoku Y. et al.. Zeolites[J ], 1985, 5: Gonthier S., Thomp son R. W. ; Edṡ, Jansen J. C., StockerM., Garge H. G. et al.. A dvanced Zeolite Science and App lications, Study in Surḟ Sci. & Catal. [M ], Am sterdam: E lsevier, 1994, 85: Schoem an B. J., Sterte J., O tterstedt J. E.. Zeolite[J ], 1994, 14: L echert H., Kacirek H.. Zeolite[J ], 1991, 11: Cundy C. S., Low e B. M., Sinclair D. M.. Faraday D iscusṡ [J ], 1993, 95: Kuhi G. H.. A dv. Chem. Seṙ [J ], 1971, 101: Syn thesis of Ultraf ine Zeol ite NaY (g ) Effect of Com plex ing Agen t CHAO Zi2Sheng 3, L IN H ai2q iang, CH EN Guo2Zhou, WU T ing2h ua, WAN H ui2l in (Chem istry D ep artm ent and S tate K ey L aboratory f or P hy sical Chem istry of S olid S urf ace, X iam en U niversity, X iam en , Ch ina) M IN En2Ze (R esearch Institute of P etroleum P rocessing, S IN O P EC, B eij ing , Ch ina) Abstract U ltrafine zeolite N ay w as hydrotherm ally synthesized w ith silica sol and A l2 (SO 4) 3 as silica and alum ina sources, respectively, by adding com p lex ing agen t such as citrate, acetate o r editate to syn thesis batch. T he effect of the amount of citrate on the crystallization rate, SiO 2gA l2o 3 ratio and crystal size of as2synthesized zeolite N ay w as investigated. W hen the relatively low er amount of citrate [ n (citrate) n (A l2o 3) 2 1 ] w as added, both the crystallization rate and the SiO 2gA l2o 3 ratio increased w h ile the crystal size reduced obviously com paring w ith that in the absence of citrate. T h is indicates that the nucleation and crystallization of zeo lite N ay w as p rom o ted by com p lex ing agen ṫ W hen the relatively h igher amount of citrate [ n ( citrate ) n (A l2o 3 ) > 2 1 ] w as added, the above p romotion effect dim in ished. T he crystallization rate w as found to reduce com paring w ith that in the absence of citrate, although the crystal size w as still sm aller than that in the later case. T he op tim um amount of citrate added to batch appears to be at the citrate A l2o 3 molar ratio of T he sim ilar p romotion effect w as also observed both for the addition of editate and acetate w ith the molar ratio of editate A l2o 3 and acetate A l2o 3 equal to 1. 5, respectively. T he p rom o tion effect of com p lex ing agen ts to the nucleation and crystallization of zeolite N ay w as related w ith their comp lexing ability to alum inum. Keywords U ltrafine zeolite; N ay; Synthesis; C rystal size; Comp lexing agent (Ed. : F, G)

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