(12)  United States Patent  Xu et al.  (54)  IN-SITU ZSM-5 SYNTHESIS  (75)  Inventors:  Mingting Xu,  Edison, NJ (US);  John  Macaoay,  Linden, NJ (US)  (73)  Assignee:  Engelhard Corporation,  Iselin, NJ  (US)  ( *)  Notice:  Subject to any disclaimer, the term of this  patent is extended or adjusted under 35  U.S.C. 154(b) by 213 days.  (21)  Appl. No.:  10/452,257  (22)  Filed:  Jun. 2, 2003  (65)  Prior Publication Data  US 2004/0238407 Al Dec. 2, 2004  (51)  Int.  c1.7  .  ... ... .. ... ... ... ... .. ... ... ... ... ... .. ... ... ..  corn  39/38  (52)  U.S. Cl.  .......................  423/709;  423/712; 423/716;  423/DIG. 22; 208/120.01  (58)  Field of Search  ......................... 423/709, DIG. 22,  423/712, 716; 208/120.01  (56)  References Cited  U.S. PATENT DOCUMENTS  4,091,007 A  4,493,902 A  4,522,705 A  5/1978 Dwyer et al.  1/1985 Brown et al.  6/1985 Chu et al.  (10)  Patent No.:  US 6,908,603 B2  (45)  Date of Patent:  Jun.21,2005  4,631,262 A  12/1986 Altomare  4,650,655 A  3/1987 Chu et al.  5,145,659 A  9/1992 McWilliams  5,232,675 A  8/1993 Shu et al.  5,558,851 A  9/1996 Miller  5,951,963 A  9/1999 He et al.  6,004,527 A  12/1999 Murrell et al.  6,261,534  Bl  7/2001 Miller  6,667,023 B2  *  12/2003 Ludvig ....................... 423/709  2004/0091420 Al  *  5/2004 Rao ........................... 423/709  2004/0092396 Al  *  5/2004 Glazer et al. ............... 502/439  FOREIGN PATENT DOCUMENTS  CN  EP  EP  1057067 C  0068817  0156595  10/2000  6/1982  3/1985  *  cited by examiner  Primary Examiner-David  Sample  (74)  Attorney, Agent, or Firm-Raymond  F.  Keller  (57)  ABSTRACT  A  novel method of forming  ZSM-5  comprises reacting  calcined kaolin microspheres with silicate and a seed solu› tion used for forming zeolite  Y  under conditions of  pH,  temperature, and time to yield  ZSM-5  crystals formed  in-situ on said calcined kaolin microspheres. The reaction  medium does not contain any organic templates or ZSM-5  seeding crystals.  24 Claims, 1 Drawing Sheet  US006908603B2 