高等学校化学学报 ›› 2021, Vol. 42 ›› Issue (1): 21.doi: 10.7503/cjcu20200201
所属专题: 分子筛功能材料 2021年,42卷,第1期
收稿日期:
2020-04-14
出版日期:
2021-01-10
发布日期:
2021-01-12
通讯作者:
肖丰收
E-mail:fsxiao@zju.edu.cn
基金资助:
WU Qinming, WANG Yeqing, MENG Xiangju, XIAO Fengshou()
Received:
2020-04-14
Online:
2021-01-10
Published:
2021-01-12
Contact:
XIAO Fengshou
E-mail:fsxiao@zju.edu.cn
Supported by:
摘要:
目前针对沸石分子筛的晶化过程已经进行了大量研究, 但是近年来硅铝分子筛的合成显示其晶化过程超出了传统的沸石分子筛晶化理论, 特别表现在硅铝沸石分子筛的模板作用、 水的作用以及沸石晶体之间的转化等. 本文讨论了上述作用的本质, 并通过研究模板法作用提出了无有机模板法合成硅铝沸石的策略, 通过了解水的作用提出了无溶剂法合成沸石分子筛, 通过表征沸石之间的转化过程发现不仅低骨架密度可以向高骨架密度晶体转化, 而且高骨架密度也可以向低骨架密度晶体转化.
中图分类号:
TrendMD:
吴勤明, 王叶青, 孟祥举, 肖丰收. 硅铝沸石分子筛晶化过程再思考. 高等学校化学学报, 2021, 42(1): 21.
WU Qinming, WANG Yeqing, MENG Xiangju, XIAO Fengshou. Reconsideration of Crystallization Process for Aluminosilicate Zeolites. Chem. J. Chinese Universities, 2021, 42(1): 21.
Fig.1 X-Ray crystallization curves of pure silica MFI zeolite synthesized with(a) and without(b) TPA+(A) and scheme for the crystallization of zeolites synthesized with organic templates(B)[22]Copyright 2017, Elsevier.
Fig.2 TEM images of Beta-SDS samples crystallized for 1, 4, 8, and 18.5 h at 140 ℃ by addition of 10.3% Beta seeds(Si/Al molar ratio: 10.2) in the starting aluminosilicate gels[23]Copyright 2011, Royal Society of Chemistry.
Fig.3 Position of ethanol adsorbing in the channel of S-1 zeolite(A) and isodensity surface colored by potential energy for ethanol in silicalite-1 zeolite(B)[35]Blue represents low potential energy/(kcal·mol-1). Copyright 2019, Wiley.
Fig.4 Representation of the synthesis of S-Si-ZSM-5 zeolite from a combination of zeolite seeding and alcohol filling in the absence of any organic templates[35]Copyright 2019, Wiley.
Fig.7 Investigation on the crystallization process in solvent-free synthesis of ZSM-5(A) Photographs of the samples crystallized at 0(A1), 2(A2) and 24 h(A3); (B) XRD patterns; (C) UV-Raman spectra; (D) 29Si NMR spectra of the samples crystallized at 0(a), 2(b), 10(c), 12(d), 18(e) and 24 h(f)[16].Copyright 2012, American Chemical Society.
Zeolite | MFI | *BEA | FAU | AEI |
---|---|---|---|---|
Framework density(T/1000 ?3) | 17.9 | 15.1 | 12.7 | 14.8 |
Number of OSDA per unit cell | 4 | 4 | 4 | 4 |
Stability energy OSDA?zeolite | 4.71 | -8.39 | -2.02 | -9.97 |
Table 1 Framework density of zeolites and the calculated energies (kJ/mol Si) between OSDA and zeolite framework[43]
Zeolite | MFI | *BEA | FAU | AEI |
---|---|---|---|---|
Framework density(T/1000 ?3) | 17.9 | 15.1 | 12.7 | 14.8 |
Number of OSDA per unit cell | 4 | 4 | 4 | 4 |
Stability energy OSDA?zeolite | 4.71 | -8.39 | -2.02 | -9.97 |
Zeolite | Channel size | Topological | SBET/(m2·g-1) | Vmicro/(cm3·g-1) |
---|---|---|---|---|
SSZ?39(AEI) | 0.38 nm×0.38 nm | 3-Dimensional | 587 | 0.26 |
Table 2 Framework properties of as-synthesized SSZ-39 zeolite[43]
Zeolite | Channel size | Topological | SBET/(m2·g-1) | Vmicro/(cm3·g-1) |
---|---|---|---|---|
SSZ?39(AEI) | 0.38 nm×0.38 nm | 3-Dimensional | 587 | 0.26 |
Fig.8 XRD pattern(A), SEM image(B), N2 sorption isotherm(C) and TG?DTA curves(D) of the Z?SSZ?39 zeolite sample from the transformation of ZSM?5 zeolite[43]Copyright 2019, Royal Society of Chemistry.
1 | Davis M. E., Nature, 2002, 417, 813—821 |
2 | Corma A., Chem. Rev., 1999, 95, 599—614 |
3 | Li Y., Li L., Yu J. H., Chem, 2017, 3, 928—949 |
4 | Meng X. J., Xiao F. S., Chem. Rev., 2014, 114, 1521—1543 |
5 | Cundy C. S., Cox P. A., Chem. Rev.2003, 103, 663—701 |
6 | Breck D. W., Zeolite Molecular Sieves, Krieger Publishing Company, Malabar, 1984 |
7 | van Bekkum H., Flanigen E. M., Jacobs P. A., Jansen J. C., Introduction to Zeolite Science and Practice, Elsevier, Amsterdam, 2001 |
8 | Barrer R. M., Hydrothermal Chemistry of Zeolites, Academic Press, London, 1982 |
9 | Xu R. R., Pang W. Q., Yu J. H., Huo Q. S., Chen J. S., Chemistry of Zeolite and Related Porous Materials, Wiley, Singapore, 2007 |
10 | Xie B., Song J. W., Ren L. M., Ji Y. Y., Li J. X., Xiao F. S., Chem. Mater., 2008, 20, 4533—4535 |
11 | Ng E. P., Chateigner D., Bein T., Valtchev V., Mintova S., Science, 2012, 335, 70—73 |
12 | Itabashi K., Kaminura Y., Iyoki K., Shimojiama A, Okubo T., J. Am. Chem. Soc., 2012, 134, 11542—11549 |
13 | Yokoi T., Yoshioka M., Ima H., Tatsumi T., Angew. Chem. Int. Ed., 2009, 48, 9884—9887 |
14 | Awala H., Gilson J. P., Retoux R., Boullay P., Goupil J. M., Valtchev V., Mintova S., Nature Mater., 2015, 14, 447—451 |
15 | Feng G. D., Cheng P., Yan W. F., Boronat M., Li X., Su J. H., Wang J. Y., Li Y., Corma A., Xu R. R., Yu J. H., Science, 2016, 351, 1188—1191 |
16 | Ren L. M., Wu Q. M., Yang C. G., Zhu L. F., Li C. J., Zhang P. L., Zhang H. Y., Meng X. J., Xiao F. S., J. Am. Chem. Soc., 2012, 134, 15173—15176 |
17 | Wu Q. M., Wang X., Qi G. D., Guo Q., Pan S. X, Meng X. J., Xu J., Deng F., Fan F. T., Feng Z. C., Li C., Maurer S., Muller U., Xiao F. S., J. Am. Chem. Soc., 2014, 136, 4019—4025 |
18 | Wu Q. M., Liu X. L., Zhu L. F., Ding L. H., Gao P., Wang X., Pan S. X., Bian C. Q., Meng X. J., Xu J., Deng F., Maurer S., Muller U., Xiao F. S., J. Am. Chem. Soc., 2015, 137, 1052—1055 |
19 | Wu Q. M., Meng X. J., Gao X. H., Xiao F. S., Acc. Chem. Res., 2018, 51, 1396—1403 |
20 | Zhang B., Douthwaite M., Liu Q., Zhang C., Wu Q. F., Shi R. H., Wu P. X., Liu K., Wang Z. Q., Lin W. W., Cheng H. Y., Cheng H. Y., Da D., Zhao F. Y., Hutchings G. J., Green Chem., 2020, 22, 1630—1638 |
21 | Xu H., Chen W., Wu Q. M., Lei C., Zhang J., Han S. C., Zhang L., Zhu Q. Y., Meng X. J., Dai D., Maurer S., Parvulescu A. N., Muller U., Zhang W. P., Yokoi T., Bao X. H., Marler B., De Vos D. E., Kolb U., Zheng A. M., Xiao F. S., J. Mater. Chem. A, 2019, 7, 4420—4425 |
22 | Wang Y. Q., Wu Q. M., Meng X. J., Xiao F. S., Engineering, 2017, 3, 567—574 |
23 | Xie B., Zhang H. Y., Yang C. G., Liu S., Ren L. M., Zhang L., Meng X. J., Yilmaz B., Muller U., Xiao F. S., Chem. Commun., 2011, 47, 3945—3947 |
24 | Zhang H. Y., Guo Q., Ren L., Yang C., Zhu L. F., Meng X. J., Li C. J., Xiao F. S., J. Mater. Chem., 2011, 21, 9494—9497 |
25 | Zhang H. Y., Yang C. G., Zhu L. F., Meng X. J., Yilmaz B., Müller U., Feyen M., Xiao F. S., Micropor. Mesopor. Mater., 2012, 155, 1—7 |
26 | Majano G., Delmotte L., Valtchev V., Mintova S., Chem. Mater., 2009, 21, 4184—4191 |
27 | Kamimura Y., Chaikittisilp W., Itabashi K., Shimojima A., Okubo T., Chem. Asian J., 2010, 5, 2182— 2191 |
28 | Iyoki K., Kamimura Y., Itabashi K., Shimojima A., Okubo T., Chem. Lett., 2010, 39, 730—731 |
29 | Kamimura Y., Itabashi K., Okubo T., Micropor. Mesopor. Mater., 2012, 147, 149—156 |
30 | Wu Q., Wang X., Meng X., Yang C., Liu Y., Jin Y., Yang Q., Xiao F. S., Micropor. Mesopor. Mater., 2014, 186, 106—112 |
31 | Yang C. G., Ren L. M., Zhang H. Y., Zhu L. F., Wang L., Meng X. J., Xiao F. S., J. Mater. Chem., 2012, 22, 12238—12245 |
32 | Zhang H. Y., Wang L., Zhang D. L., Meng X. J., Xiao F. S., Micropor. Mesopor. Mater., 2016, 233, 133—139 |
33 | Iyoki K., Takase M., Itabashi K., Muraoka K., Chaikittisilp W., Okubo T., Micropor. Mesopor. Mater., 2015, 215, 191—198 |
34 | Wu Q. M., Ma Y., Wang S., Meng X. J., Xiao F. S., Ind. Eng. Chem. Res., 2019, 58, 11653—11658 |
35 | Wu Q. M., Zhu L. F., Chu Y. Y., Liu X. L., Zhang C. S., Zhang J., Xu H., Xu J., Deng F., Feng Z. C., Meng X. J., Xiao F. S., Angew. Chem. Int. Ed., 2019, 58, 12138—12142 |
36 | Wu D., Xu X., Chen X. Q., Yu G., Zhang K., Qiu M. H., Xue W. J., Yang C. G., Liu Z. Y., Sun Y. H., ChemSusChem, 2019, 12, 3871—3877 |
37 | Soekiman C. N., Miyake K., Hirota Y., Uchida Y., Tanaka S., Miyamoto M., Nishiyama N., Micropor. Mesopor. Mater., 2019, 273, 273—275 |
38 | Zhang C. S., Wu Q. M., Lei C., Pan S. X., Bian C. Q., Wang L., Meng, X. J., Xiao F. S., Ind. Eng. Chem. Res., 2017, 56, 1450—1460 |
39 | Xiao Y. C., Sheng N., Chu Y. Y., Wang Y. Q., Wu Q. M., Liu X. L., Deng F., Meng X. J., Feng Z. C., Micropor. Mesopor. Mater., 2017, 237, 201—209 |
40 | Goel S., Zones S. I., Iglesia E., Chem. Mater., 2015, 27, 2056—2066 |
41 | Jon H., Ikawa N., Oumi Y., Sano T., Chem. Mater., 2008, 20, 4135—4131 |
42 | Li C., Moliner M., Corma A., Angew. Chem. Int. Ed., 2018, 57, 15330—15353 |
43 | Xu H., Chen W., Wu Q. M., Lei C., Zhang J., Han S. C., Zhang L., Zhu Q. Y., Meng X. J., Maurer S., Parvulescu A. N., Muller U., Zhang W. P., Yokoi T., Bao X., Marler B., De Vos D. E., Kolb U., Zheng A., Xiao F. S., J. Mater. Chem. A, 2019, 7, 4420—4425 |
44 | Zhang J., Chu Y. Y., Liu X. L., Xu H., Meng X. J., Feng Z. C., Xiao F. S., Chinese J. Catal., 2019, 40, 1854—1859 |
45 | Bian C. Q., Zhang C. S., Pan S. X., Chen F., Zhang W. P., Meng X. J., Maurer S., Dai D., Parvulescu A. N., Muller U., Xiao F. S., J. Mater. Chem. A, 2017, 5, 2613—2618 |
46 | Tian P., Wei Y. X., Ye M., Liu Z. M., ACS Catal., 2015, 5, 1922—1938 |
47 | Beale A. M., Gao F., Lezcano-Gonzalez I., Peden C. H. F., Szanyi J., Chem. Soc. Rev., 2015, 44, 7371—7405 |
48 | Lin Y. C., Chang F. T., J. Hazard. Mater., 2009, 164, 517—526 |
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