Zr K-Edge XAS and 29Si MAS NMR Studies on Hexagonal Mesoporous Zirconium Silicate
Source abstract
Abstract
Hexagonal mesoporous silicate (HMS) molecular sieve containing zirconium species (Zr-HMS) has been synthesized using a neutral template of hexadecylamine with ethanol and water. A disordered channel structure with a uniform diameter of 44.1 A was confirmed by powder X-ray diffraction after calcination. From N2 adsorption/desorption measurement, it is found that Zr-HMS has a very high surface area of about 910 m2/g (BET) and a mesopore with a size of 21 A (BJH). According to the X-ray absorption spectroscopy at the Zr K-edge, it is confirmed that Zr atoms are coordinated by six oxygen neighbors with a distance of 2.13 A, which is shorter than the (Zr—O) bond distance found in ZrO2 or ZrOCl2·8H2O. The 29Si MAS-NMR spectrum for Zr-HMS shows two additional peaks around −94.6 and −107.2 ppm due to the Q3Zr and Q4Zr components, respectively, besides three peaks at −91.1, −101.5, and −111.3 ppm due to the silicate network. The relation between the pore and crystal structures and the local environment around Zr is discussed in detail.
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Research context
OpenAlex topics: Mesoporous Materials and Catalysis · Zeolite Catalysis and Synthesis · Chemical Synthesis and Characterization
SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.
References (33)
Show source-provided references
1. C.T. Kresge, M.E. Leonowicz, W.J. Roth, J.C. Vartuli, and J.S. Beck, Nature 359, 710 (1992).10.1038/359710a0 ↗
2. J.S. Beck, J.C. Vartuli, W.J. Roth, M.E. Leonowicz, C.T. Kresge, K.D. Schmitt, C.T.-W. Chu, D.H. Olson, E.W. SHEPPARD, S.B. McCullen, J.B. Higgins, and J.L. Schlenker, J. Am. Chem. Soc. 114, 10834 (1992).10.1021/ja00053a020 ↗
3. Q. Huo, D.I. Margolese, U. Ciesla, P. Feng, T.E. Gier, P. Sieger, R. Leon, P.M. Petroff, F. Sch¨uth, and G.D. Stucky, Nature 368, 317 (1994).10.1038/368317a0 ↗
4. M.J. Hudson and J.A. Knowles, J. Mater. Chem. 6, 89 (1996).10.1039/jm9960600089 ↗
5. T. Sun and J.Y. Ying, Nature 389, 704 (1997).10.1038/39549 ↗
6. C. Saúl, E.H. Jamel, B.P. Aurelio, B.P. Daniel, M.M. Dolores, and A. Pedro, Solid State Science 2, 513 (2000).10.1016/S1293-2558(00)00057-1 ↗
7. U. Ciesla, D. Demuth, R. Leon, P. Petroff, G. Stucky, K. Unger, and F. Schuth, J. Chem. Soc. Commun. 20, 2083 (1995).
8. F.L. Chen and M.L. Liu, Chem. Commun. 18, 1829 (1999).10.1039/a904142g ↗
9. R. Mokaya and W. Jones, J. Chem. Soc., Chem. Commun. 981 (1996).10.1039/cc9960000981 ↗
10. Z. Zhang, Y. Han, F.S. Xiao, S. Qiu, L. Zhu, R. Wang, Y. Yu, Z. Zhang, B. Zou, Y. Wang, H. Sun, D. Zhao, and Y. Wei, J. Am. Chem. Soc. 123, 5014 (2001).10.1021/ja004138t ↗
11. P.T. Tanev, M. Chibwe, and T.J. Pinnavaia, Nature 368, 321 (1994).10.1038/368321a0 ↗
12. D.J. Jones, J.J. Jimenez, A.J. Lopez, P.M. Torres, and P.O. Pastor, Chem. Commun. 431 (1997).10.1039/a608145b ↗
13. M.L. Occelli, S. Biz, and A. Auroux, Appl. Catal. A 183, 231 (1999).10.1016/S0926-860X(99)00059-9 ↗
14. J.H. Choy, D.K. Kim, J.C. Park, S.N. Choi, and Y.J. Kim, Inorg. Chem. 36, 189 (1997).10.1021/ic960631n ↗
15. A. Mosset and J. Galy, in Synchrotron Radiation in Chemistry and Biology (Springer-Verlag, Berlin, 1988).
16. J.H. Choy, J.H. Park, and J.B. Yoon, J. Phys. Chem. 102, 5991 (1998).10.1021/jp9815863 ↗
17. P.T. Tanev and T.J. Pinnavaia, Science 267, 865 (1995).10.1126/science.267.5199.865 ↗
18. J.A. Bearden and A.F. Burr, Rev. Modern Physics. 39, 125 (1967).10.1103/RevModPhys.39.125 ↗
19. M. Nomura and A. Koyama, KEK Internal 93(1) (1993).
20. B.K. Teo, Basic Principle of EXAFS (Springer-Verlag, Berlin, 1986).10.1007/978-3-642-50031-2 ↗
21. E.A. Stern, M. Newville, B. Ravel, Y. Yacoby, and D. Haskel, Physica B 208/209, 117 (1995).10.1016/0921-4526(94)00826-H ↗
22. J.J. Rehr, J. Mustre de leon, S.I. Zabinsky, and R.C. Albers, J. Am. Chem. Soc. 113, 5135 (1991).10.1021/ja00014a001 ↗
23. P.A. O'day, J.J. Rehr, S.I. Zabinsky, and G.E. Brown Jr., J. Am. Chem. Soc. 116, 2938 (1994).10.1021/ja00086a026 ↗
24. S.A. Bagshaw, E. Prouzet, and T.J. Pinnavaia, Science 269, 1242 (1995).10.1126/science.269.5228.1242 ↗
25. A. Tuel and S. Gontier, Chem. Mater. 8, 114 (1996).10.1021/cm950276j ↗
26. E.P. Barrett, L.G. Joyner, and P.P. Halenda, J. Am. Chem. Soc. 73, 373 (1951).10.1021/ja01145a126 ↗
27. J.B. Yoon, Ph. D. Thesis, Seoul National Univ., Seoul, Aug. 1998.
28. C.J. Howard, R.J. Hill, and B.E. Reichert, Acta Crystallogr. B44, 116 (1988).10.1107/S0108768187010279 ↗
29. A. Clearfield and P. A. Vaugham, Acta Crystallogr. 9, 555 (1956).10.1107/S0365110X56001558 ↗
30. R.D. Shannon, Acta Crystallogr. A32, 751 (1976).10.1107/S0567739476001551 ↗
31. W. Zhang, M. Froba, J. Wang, P.T. Tanev, J. Wong, and T.J. Pinnavaia, J. Am. Chem. Soc. 118, 9164 (1996).10.1021/ja960594z ↗
32. M. Lipsicas, R.H. Raythatha, T.J. Pinnavaia, I.D. Johnson, R.F. Giese Jr., P.M. Costanzo, and J.L. Robert, Nature 309, 604 (1984).10.1038/309604a0 ↗
33. Z.Y. Yuan, S.Q. Liu, T.H. Chen, J.Z. Wang, and H.X. Li, J. Chem. Soc. Commun. 9, 973 (1995).10.1039/c39950000973 ↗