Abstract
The mordenite (MOR) nanoparticles (MNPs) with ultra-small crystallites (∼30 nm) were synthesized by using tetraethylammonium bromide (TEAB) as structure directing agent at low temperature (403 K). The formation of MNPs was considered to be due to high concentration of TEAB and occurrence of limiting Ostwald ripening at low temperature. The MNPs exhibited not only higher catalytic activity at low temperature for selective catalytic reduction of NOx but also higher catalytic activity and longer lifetime for disproportionation of toluene than conventional MOR (c-MOR) bulk crystals.
摘要
本文在一个较低的温度(403 K)下使用四乙基溴化铵(TEAB)为模板剂合成出超小的(30 nm)MOR型分子筛. 超小的产物粒径是由于高浓度的TEAB可以提供更多的晶核以及低温限制了奥氏熟化. 产物在低温区域的NOx选择性催化还原活性远远高于传统MOR型分子筛. 此外, 超小的纳米颗粒减小了物质的传输限制以及较大的比表面积使得其在甲苯歧化反应中具有比传统MOR更高的催化活性和耐失活性.
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References
Corma A. From microporous to mesoporous molecular sieve materials and their use in catalysis. Chem Rev, 1997, 97: 2373–2420
Davis ME. Ordered porous materials for emerging applications. Nature, 2002, 417: 813–821
Davis ME. Zeolites from a materials chemistry perspective. Chem Mater, 2014, 26: 239–245
Li Y, Yu J. New stories of zeolite structures: their descriptions, determinations, predictions, and evaluations. Chem Rev, 2014, 114: 7268–7316
Mintova S, Gilson JP, Valtchev V. Advances in nanosized zeolites. Nanoscale, 2013, 5: 6693–6703
Xue Z, Ma J, Zhang T, et al. Synthesis of nanosized ZSM-5 zeolite with intracrystalline mesopores. Mater Lett, 2012, 68: 1–3
Ng EP, Chateigner D, Bein T, et al. Capturing ultrasmall EMT zeolite from template-free systems. Science, 2012, 335: 70–73
Awala H, Gilson JP, Retoux R, et al. Template-free nanosized faujasite-type zeolites. Nat Mater, 2015, 14: 447–451
Meier W, Kristallogr Z. The crystal structure of mordenite (ptilolite). Zeitschrift für Kristallographie-Crystalline Mater, 1961, 115: 439–450
Lv A, Xu H, Wu H, et al. Hydrothermal synthesis of high-silica mordenite by dual-templating method. Microporous Mesoporous Mater, 2011, 145: 80–86
Ren L, Guo Q, Zhang H, et al. Organotemplate-free and one-pot fabrication of nano-rod assembled plate-like micro-sized mordenite crystals. J Mater Chem, 2012, 22: 6564–6567
Zhang H, Zhang H, Wang P, et al. Organic template-free synthesis of zeolite mordenite nanocrystals through exotic seed-assisted conversion. RSC Adv, 2016, 6: 47623–47631
Yang Y, Ding J, Xu C, et al. An insight into crystal morphologydependent catalytic properties of MOR-type titanosilicate in liquid- phase selective oxidation. J Catal, 2015, 325: 101–110
Jo C, Jung J, Shin HS, et al. Capping with multivalent surfactants for zeolite nanocrystal synthesis. Angew Chem, 2013, 125: 10198–10201
Kim GJ, Ahn WS. Direct synthesis and characterization of high- SiO2-content mordenites. Zeolites, 1991, 11: 745–750
Buerger MJ, Azaroff LV. The Powder Method in X-Ray Crystallography. New York: McGraw-Hill, 1958
Kim SD, Noh SH, Seong KH, et al. Compositional and kinetic study on the rapid crystallization of ZSM-5 in the absence of organic template under stirring. Microporous Mesoporous Mater, 2004, 72: 185–192
Li J, Li Z, Han D, et al. Facile synthesis of SAPO-34 with small crystal size for conversion of methanol to olefins. Powder Tech, 2014, 262: 177–182
Bohström Z, Arstad B, Lillerud KP. Preparation of high silica chabazite with controllable particle size. Microporous Mesoporous Mater, 2014, 195: 294–302
Schmidt JE, Fu D, Deem MW, et al. Template-framework interactions in tetraethylammonium-directed zeolite synthesis. Angew Chem Int Ed, 2016, 55: 16044–16048
Sultana A, Nanba T, Sasaki M, et al. Selective catalytic reduction of NOx with NH3 over different copper exchanged zeolites in the presence of decane. Catal Today, 2011, 164: 495–499
Acknowledgements
This work was supported by the National Natural Science Foundation of China (21533002 and 21571128), the National Excellent Doctoral Dissertation of China (201454), and the National Key R&D Program of China (2016YFC0205900).
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Yi Xu received his BSc degree in chemistry from Donghua University in 2015. He joined Prof. Che’s group as a master candidate in 2015. His research interests focus on the design and synthesis of hierarchical zeolitic materials.
Shunai Che is a professor in the Department of Chemistry, School of Chemistry and Chemical Engineering, Shanghai Jiao Tong University. She received her PhD degree from Yokohama National University. She was a guest researcher at Saitama University and worked as a postdoctoral fellow at Yokohama National University. Her research interests encompass the development of chiral inorganic materials and porous materials with novel structures and functions in view of applications in optical devices and heterogeneous catalysis.
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Xu, Y., Shen, X., Peng, C. et al. Synthesis of ultra-small mordenite zeolite nanoparticles. Sci. China Mater. 61, 1185–1190 (2018). https://doi.org/10.1007/s40843-018-9257-3
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DOI: https://doi.org/10.1007/s40843-018-9257-3