Direct Synthesis of UOS Zeolite Using a Simple and Commercially Available Organic Structure-directing Agent

doi:10.1007/s40242-024-4196-0

Abstract

Abstract: The preparation of zeolite utilizing commercially available organic compounds instead of complex and expensive ones is of practical significance. Herein, we report the synthesis of germanosilicate zeolite with UOS framework by utilizing a simple and commercially available compound 3-diethylamino-1-propanol (DEAP) as organic structure-directing agent (OSDA) under fluoride condition. The synthesis has been optimized by rational modification of the variables, including the Si/Ge molar ratios, the amount of DEAP and F^- anions, the concentration of the synthesis gel and crystallization temperature. UOS zeolite materials were prepared with Si/Ge ratio in the range of 1—4. The physicochemical properties, including crystallinity, crystal morphology, chemical environment of framework elements, textural properties and acidity were characterized by multiple techniques. Ge atoms are proved to preferentially occupy the T sites in the double-four-ring (D4Rs) units. Compared to the isostructural IM-16 zeolite, the UOS zeolites prepared herein are of similar textural properties, such as specific surface area and micropore volume. The simple structure and commercial availability of DEAP endow this synthesis with a cost advantage over the conventional preparation of UOS zeolite, where an expensive imidazolium derivative is employed.

Key words: UOS zeolite, Organic structure-directing agent, Hydrothermal synthesis, Physicochemical property

HU Chao, FU Wenhua, YUAN Zhiqing, LIU Chuang, WANG Zhendong, YANG Weimin. Direct Synthesis of UOS Zeolite Using a Simple and Commercially Available Organic Structure-directing Agent[J]. Chemical Research in Chinese Universities, 2025, 41(1): 113-120.

References

[1] Koike N., Iyoki K., Wang B., Yanaba Y., Elangovan S. P., Itabashi K., Chaikittisilp W., Okubo T., Dalton Trans., 2018, 47, 9546.
[2] Xia H., Hu Y., Bao Q., Zhang J., Sun P., Liang D., Wang B., Qiao X., Wang X., Microporous Mesoporous Mater., 2023, 350, 112442.
[3] Tang X., Wang Y., Wei M., Zhang X., Li Y., Li X., Li J., Yang J., Sep. Purif. Technol., 2023, 318, 124003.
[4] Abdi H., Maghsoudi H., Akhoundi V., Fluid Phase Equilib., 2021, 546, 113171.
[5] Lee H. I., Lee P. S., Microporous Mesoporous Mater., 2022, 334, 111768.
[6] Wang X., Ma Y., Wu Q., Wen Y., Xiao F.-S., Chem. Soc. Rev., 2022, 51, 2431.
[7] Zheng M., Chen Y., Liu Z., Lyu J., Ye B., Sun M.-H., Chen L.-H., Su B.-L., Chem. Res. Chinese Universities, 2024, 40, 704.
[8] Chen L., Jiao W., Wang C., Zhou H., Liu S., Su J., Wang Y., Yu J., Xue Z., Mao D., Catal. Commun., 2023, 177, 106653.
[9] Li X., Han H., Xu W., Hwang S.-J., Shi Z., Lu P., Bhan A., Tsapatsis M., J. Am. Chem. Soc., 2022, 144, 9324.
[10] Ge L., Qiu M., Zhu Y., Yang S., Li W., Li W., Jiang Z., Chen X., Appl. Catal., B, 2022, 319, 121958.
[11] Su H., Zhou Q., Jin K., Li Q., Wang Y., Fan W., Zhang J.-N., Yan W., Fuel, 2024, 376, 132651.
[12] Weisz P. B., Pure Appl. Chem., 1980, 52, 2091.
[13] Lee C., Lee S., Kim W., Ryoo R., Catal. Today, 2017, 303, 143.
[14] Li H., Yu J., Du K., Li W., Ding L., Chen W., Xie S., Zhang Y., Tang Y., Angew. Chem. Int. Ed., 2024, 63, e202405092.
[15] Yu L., Xu C., Zhang W., Zhou Q., Fu X., Liang Y., Guo Z., Wang W., J. Solid State Chem., 2023, 327, 121271.
[16] Zhang B., Douthwaite M., Liu Q., Zhang C., Wu Q., Shi R., Wu P., Liu K., Wang Z., Lin W., Cheng H., Ma D., Zhao F., Hutchings G. J., Green Chem., 2020, 22, 1630.
[17] Jonscher C., Seifert M., Kretzschmar N., Marschall M. S., Le Anh M., Doert T., Busse O., Weigand J. J., ChemCatChem, 2022, 14, e202101248.
[18] Dai W., Zhang L., Liu R., Huo Z., Dai W., Guan N., Mater. Today Sustainability, 2023, 22, 100364.
[19] Chen P., Xie M., Zhai Y., Wang Y., Huang Z., Yang T., Sun W., Wang Y., Sun J., Chemistry: A European Journal, 2022, 28, e202202170.
[20] Tsaplin D., Gorbunov D., Ostroumova V., Naranov E., Kulikov L., Egazaryants S., Maximov A., Mater. Chem. Phys., 2024, 326, 129825.
[21] Rosso F., Rizzetto A., Airi A., Khoma K., Signorile M., Crocellà V., Bordiga S., Galliano S., Barolo C., Alladio E., Bonino F., Inorg. Chem. Front., 2022, 9, 3372.
[22] Luan H., Xu C., Wu Q., Xiao F.-S., Front. Chem., 2022, 10, 1080554.
[23] Wang S., Zhou L., Gao B., Su Y., Yang X., Microporous Mesoporous Mater., 2022, 335, 111812.
[24] Xiong G., Yang H., Liu L., Liu J., RSC Adv., 2023, 13, 4835.
[25] Zhao Y., Wu S., Wang J., Peng M., Xu H., Jiang J., Ma Y., Wu P., Angew. Chem. Int. Ed., 2024, 63, e202318298.
[26] Peng M., Deng Q., Zhao Y., Xu H., Guan Y., Jiang J., Han L., Wu P., Angew. Chem. Int. Ed., 2023, 62, e202217004.
[27] Kemp K. C., Choi W., Jo D., Park S. H., Hong S. B., Chemical Science, 2022, 13, 10455.
[28] Cai X., Zhao Y., Zi W., Jiao F., Du H., Chemistry: A European Journal, 2022, 28, e202200934.
[29] Hou X., Yao Z., Li H., Wang M., Wei Y., Zhang L., Liang Y., Qiao J., Jia J., Zhang R., Microporous Mesoporous Mater., 2023, 348, 112340.
[30] Bnmner G. O., Meier W. M., Nature, 1989, 337, 146.
[31] Sastre G., Pulido A., Castañeda R., Corma A., J. Phys. Chem. B, 2004, 108, 8830.
[32] Sastre G., Pulido A., Corma A., Microporous Mesoporous Mater., 2005, 82, 159.
[33] Paillaud J.-L., Harbuzaru B., Patarin J. l., Bats N., Science, 2004, 304, 990.
[34] Corma A., Diaz-Cabanas M. J., Jorda J. L., Rey F., Sastre G., Strohmaier K. G., J. Am. Chem. Soc., 2008, 130, 16482.
[35] Tang L., Shi L., Bonneau C., Sun J., Yue H., Ojuva A., Lee B.-L., Kritikos M., Bell R. G., Bacsik Z., Mink J., Zou X., Nat. Mater., 2008, 7, 381.
[36] Luo Y., Fu W., Wang B., Yuan Z., Sun J., Zou X., Yang W., Inorg. Chem., 2022, 61, 4371.
[37] Dodin M., Paillaud J.-L., Lorgouilloux Y., Caullet P., Elkaïm E., Bats N., J. Am. Chem. Soc., 2010, 132, 10221.
[38] Lorgouilloux Y., Dodin M., Paillaud J.-L., Caullet P., Michelin L., Josien L., Ersen O., Bats N., J. Solid State Chem., 2009, 182, 622.
[39] Peng M., Jiang J., Liu X., Ma Y., Jiao M., Xu H., Wu H., He M., Wu P., Chem. Eur. J., 2018, 24, 13297.
[40] Li X., Curnow O. J., Choi J., Yip A. C. K., Mater. Today Chem., 2022, 26, 101133.
[41] Zhang Y., Li A., Sajad M., Fulajtárová K., Mazur M., Kubů M., Shamzhy M., Hronec M., Bulánek R., Čejka J., Chem. Eng. J., 2021, 412, 128599.
[42] Comin E., Aquino A. S., Favero C., Mignoni M. L., de Souza R. F., de Souza M. O., Pergher S. B. C., Campos C. X. D. S., Bernardo-Gusmão K., Mol. Catal., 2022, 530, 112624.
[43] Gao Z. R., Balestra S. R. G., Li J., Camblor M. A., Chemistry: A European Journal, 2021, 27, 18109.
[44] Peng R., Li S., Wan Z., Wang Z.-Q., Si X., Tuo J., Xu H., Guan Y., Jiang J., Ma Y., He X., Gong X.-Q., Wu P., ACS Applied Materials & Interfaces, 2023, 15, 28116.
[45] Emeis C. A., J. Catal., 1993, 141, 347.
[46] Corma A., Díaz-Cabañas M. J., Jordá J. L., Martínez C., Moliner M., Nature, 2006, 443, 842.
[47] Dorset D. L., Strohmaier K. G., Kliewer C. E., Corma A., Díaz-Cabañas M. J., Rey F., Gilmore C. J., Chem. Mater., 2008, 20, 5325.
[48] Yue Q., Kasneryk V., Mazur M., Abdi S., Zhou Y., Wheatley P. S., Morris R. E., Čejka J., Shamzhy M., Opanasenko M., J. Mater. Chem. A, 2024, 12, 802.
[49] Gramatikov S. P., Petkov P. S., Vayssilov G. N., Inorganic Chemistry Frontiers, 2022, 9, 3747.
[50] Shamzhy M., Opanasenko M., Tian Y., Konysheva K., Shvets O., Morris R. E., Čejka J., Chem. Mater., 2014, 26, 5789.
[51] Zhang J., Yue Q., Shamma E., Abdi S., Petrov O., Čejka J., Mintova S., Opanasenko M., Shamzhy M., J. Mater. Chem. A, 2024, 12, 31195.
[52] Gao Z. R., Li J., Lin C., Mayoral A., Sun J., Camblor M. A., Angew. Chem. Int. Ed., 2021, 60, 3438.
[53] Verheyen E., Joos L., Van Havenbergh K., Breynaert E., Kasian N., Gobechiya E., Houthoofd K., Martineau C., Hinterstein M., Taulelle F., Van Speybroeck V., Waroquier M., Bals S., van Tendeloo G., Kirschhock C. E. A., Martens J. A., Nat. Mater., 2012, 11, 1059.
[54] El-Roz M., Lakiss L., Vicente A., Bozhilov K. N., Thibault-Starzyk F., Valtchev V., Chem. Sci., 2013, 5, 68.