Direct Synthesis of SSZ-13 Zeolite Using Tetraethylammonium Hydroxide as an Efficient Organic Template in the Presence of Conventional Aluminum and Silicon Sources†

doi:10.7503/cjcu20200197

Abstract

Abstract:

High silica CHA zeolite(SSZ-13) has been commercially applied in selective catalytic reduction of NO_x with ammonia currently, but the use of costly organic templates of N,N,N-trimethyl-adamantammonium hydroxide(TMAdaOH) in the synthesis strongly limits its industrial application. To solve this problem, it is developed a synthetic route using relatively low-cost organic templates such as tetraethylammonium hydroxide(TEAOH), but in this case it is necessary to use costly high silica Y zeolite as a starting source. In this report, we for the first time show that SSZ-13 zeolite could be synthesized directly from conventional silicon and aluminum sources using TEAOH as an efficient organic template by carefully adjusting the starting gels in the presence of SSZ-13 seeds. The obtained aluminosilicate SSZ-13 product has good crystallinity, uniform crystals, and excellent hydrothermal stability. Furthermore, copper-exchanged SSZ-13 zeolite has excellent catalytic performance in NH₃-SCR reaction before and after hydrothermal treatment. The combination of good catalytic performance with low-cost synthesis offers a good opportunity for wide applications of this zeolite in the future.

Key words: SSZ-13 zeolite, TEAOH, Conventional source, Design synthesis, NH₃-SCR

CLC Number:

O643

TrendMD:

LUAN Huimin, CHEN Wei, WU Qinming, XU Hao, HAN Shichao, MENG Xiangju, ZHENG Anmin, XIAO Fengshou. Direct Synthesis of SSZ-13 Zeolite Using Tetraethylammonium Hydroxide as an Efficient Organic Template in the Presence of Conventional Aluminum and Silicon Sources^†[J]. Chem. J. Chinese Universities, 2020, 41(7): 1470.

Figures/Tables 8

Entry^a	Molar ratio			Seed/SiO₂ (mass fraction, %)	Temp./℃	Product^b
Entry^a	Si/Al	Na₂O/SiO₂	H₂O/SiO₂	Seed/SiO₂ (mass fraction, %)	Temp./℃	Product^b
1	10	0.12	20	10	160	Amorphous
2	10	0.16	20	10	160	MOR+CHA+GME
3	10	0.21	20	10	160	MOR+GME
4	20	0.22	20	10	160	MOR+CHA
5	20	0.25	20	10	160	CHA
6	20	0.28	20	10	160	ANA+CHA
7	20	0.25	20	0	160	MOR+CHA
8	40	0.24	20	10	160	MOR+CHA
9	40	0.31	20	10	160	CHA
10	40	0.37	20	10	160	CHA+ANA
11	40	0.31	5	10	160	MFI+CHA
12	40	0.31	35	10	160	CHA+Amorphous
13	60	0.33	20	10	160	CHA
14	∞	0.34	20	10	160	Beta
15	40	0.31	20	10	140	CHA+GME
16	40	0.31	20	10	180	CHA
17	40	0.31	20	10	200	CHA+MOR

Organic template	TEAOH (tt.tt)	TEAOH (tg.tg)	TMAdaOH
Number	3	3	3
Stability energy/(kJ·mo $l Si - 1$ )	-1.33	-1.02	-1.55

Organic template	TEAOH (tt.tt)	TEAOH (tg.tg)	TMAdaOH
Number	3	3	3
Stability energy/(kJ·mo $l Si - 1$ )	-1.33	-1.02	-1.55

References 36

[1]	Park J. W., Lee J. Y., Kim K. S., Hong S. B., Seo G., Appl. A, 2008, 339(1), 36—44
[2]	Zhu Q. J., Kondo J. N., Inagaki S., Tatsumi T., Top. Catal., 2009, 52(9), 1272—1280 doi: 10.1007/s11244-009-9272-7 URL
[3]	Hudson M. R., Queen W. L., Mason J. A., Fickel D. W., Lobo R. F., Brown C. M., J. Am. Chem. Soc., 2012, 134(4), 1970—1973 URL pmid: 22235866
[4]	Schmidt J. E., Xie D., Davis M. K., Chem. Sci., 2015, 6(10), 5955—5963 doi: 10.1039/c5sc02325d URL pmid: 29861917
[5]	Liu N., Wang J. Q., Chen B. H., Li Y. X., Zhang R. D., Chem. J. Chinese Universities, 2016, 37(10), 1817—1825
	( 刘宁, 王继琼, 陈标华, 李英霞, 张润铎. 高等学校化学学报, 2016, 37(10), 1817—1825)
[6]	Pappas D. K., Borfecchia E., Dyballa M., Pankin I. A., Lomachenko K. A., Martini A., Signorile M., Teketel S., Arstad B., Berlier G., Lamberti C., Bordiga S., Olsbye U., Lillerud K. P., Svelle S., Beato P., J. Am. Chem. Soc., 2017, 139(42), 14961—14975 doi: 10.1021/jacs.7b06472 URL pmid: 28945372
[7]	Kwak J. H., Tonkyn R. G., Kim D. H., Szanyi J., Pebden C. H. F., J. Catal., 2010, 287, 203—209 doi: 10.1016/j.jcat.2011.12.025 URL
[8]	Deka U., Juhin A., Eilertsen E. A., Emerich H., Green M. A., Korhonen S. T., Weckhuysen B. M., Beale A. M., J. Phys. Chem. C, 2012, 116(7), 4809—4818 doi: 10.1021/jp212450d URL
[9]	Schmieg S. J., OhS. H., Kim C. H., Brown D. B., Lee J. H., Peden C. H. F., Kim D. H., Catal. Today, 2012, 184(1), 252—261
[10]	Ma L., Cheng Y. S., Cavataio G., McCabe R. W., Fu L. X., Li J. H., Chem. Eng. J., 2013, 225, 323—330
[11]	Wang D., Jangjou Y., Liu Y., Sharma M. K., Luo J. Y., Kamasamudram K., Epling W. S., Appl. Catal. B, 2015, 165, 438—445 doi: 10.1016/j.apcatb.2014.10.020 URL
[12]	Borfecchia E., Lomachenko K. A., Giordanino F., Falsig H., Beato P., Soldatov A. V., Bordiga S., Lamberti C., Chem. Sci., 2015, 6(1), 548—563 doi: 10.1039/c4sc02907k URL pmid: 28936309
[13]	Wang J. H., Zhao H. W., Haller G., Li Y. D., Appl. Catal. B, 2017, 202, 346—354
[14]	Paolucci C., Khuranan I., Parekh A. A., Li S. C., Shih A. J., Li H., Di lorio J. R., Albarracin-Caballero J. D., Yezerets A., Miller J. T., Delgass W. N., Ribeiro F. H., Schneider W. F., Gounder R., Science, 2017, 357(6354), 898—903 doi: 10.1126/science.aan5630 URL pmid: 28818971
[15]	Zhang L., Duan H. C., Tan Z. G., Wu Q. M., Meng X. J., Xiao F. S., Chem. J. Chinese Universities., 2020, 41(1), 19—27
	( 章凌, 段宏昌, 谭争国, 吴勤明, 孟祥举, 肖丰收. 高等学校化学学报, 2020, 41(1), 19—27)
[16]	Gao F., Mei D. H., Wang Y. L., Szanyi J., Penden C. H. F., J. Am. Chem. Soc., 2017, 139(13), 4935—4942 URL pmid: 28288511
[17]	Eilertsen E. A., Haouas M., Pinar A. B., Hould N. D., Lobo R. F., Lillerud K. P., Taulelle F., Chem. Mater., 2012, 24(3), 571—578
[18]	Takata T., Tsunoji N., Takamitsu Y., Sadakane M., Sano T., Micropor. Mesopor. Mater., 2016, 225, 524—533
[19]	Guo Y., Sun T. J., Liu X. W., Ke Q. L., Wei X. L., Gu Y. M., Wang S. D., Chem. Eng. J., 2019, 358, 331—339
[20]	Itakura M., Inoue T., Takahashi A., Fujitani T., Oumi Y., Sano T., Chem. Letters, 2008, 37(9), 908—909
[21]	Ren L. M., Zhu L. F., Yang C. G., Chen Y. M., Sun Q., Zhang H. Y., Li C. J., Nawaz F., Meng X. J., Xiao F. S., Chem. Commun., 2011, 47(35), 9789—9791 doi: 10.1039/c1cc12469b URL
[22]	Xu R. N., Zhang R. D., Liu N., Chen B. H., Qiao S. Z., ChemCatChem, 2015, 7(23), 3842—3847
[23]	Martin N., Moliner M., Corma A., Chem. Commun., Chem. Commun., 2015, 51(49), 9965—9968
[24]	Ding L. H., Zheng Y., Zhang Z. S., Ring Z. N., Chen J. W., Micropor. Mesopor. Mater., 2006, 94(1—3), 1—8 doi: 10.1016/j.micromeso.2006.03.010 URL
[25]	Zhang Y., Jin C., J. Solid State Chem., 2011, 184(1), 1—6 doi: 10.1016/j.jssc.2010.10.012 URL
[26]	Yang G. J., Wei Y. X., Xu S. T., Chen J. R., Li J. Z., Li Z. M., Yu J. H., Xu R. R., J. Phys. Chem. C, 2013, 117(16), 8214—8222
[27]	Yuan Y. Y., Wang L. Y., Liu H. C., Tian P., Yang M., Xu S. T., Liu Z. M., Chin. J. Catal., 2015, 36(11), 1910—1919
	( 袁扬扬, 王林英, 刘红超, 田鹏, 杨淼, 徐舒涛, 刘中民. 催化学报, 2015, 36(11), 1910—1919)
[28]	Naudin C., Bonhomme F., Bruneel J. L., Ducasse L., Grondin J., LassHgues J. C., Servant L., J. Raman Spectrosc., 2000, 31(11), 979—985
[29]	Schmidt J. E., Fu D. L., Deem M. W., Weckhuysen B. M., Angew. Chem. Int. Ed., 2016, 55(52), 16044—16048
[30]	Pophale R., Daevaert F., Deem M., J. Mater. Chem. A, 2013, 1(23), 6750—6760
[31]	Mayo S. L., Olafson B. D., Goddard W. A., J. Phys. Chem., 1990, 94(26), 8897—8909
[32]	Gale J. D., Rohl A. L., Mol. Simul., 2003, 29(5), 291—341
[33]	Eilertsen E. A., Arstad B., Svelle S., Lillerud K. P., Micropor. Mesopor. Mater., 2012, 153, 94—99
[34]	Jangjou Y., Do Q., Gu Y. T., Li L. G., Sun H., Wang D., Kumar A., Li J. H., Grabow L. C., Epling W. S., ACS Catal., 2018, 8(2), 1325—1337
[35]	Shan Y. L., Shi X. Y., Du J. P., Yan Z. D., Yu Y. B., He H., Ind. Eng. Chem. Res., 2019, 58(14), 5397—5403
[36]	Lee H., Song I., Jeon S. J., Kim D. H., React. Chem. Eng., 2019, 4(6), 1059—1066 doi: 10.1039/C8RE00281A URL