文献类型：期刊文献

英文题名：Direct Synthesis of Highly Siliceous Faujasite-type Zeolite Enabled by Low Charge Density Organic Structure-directing Agents

作者：Mi, Zhenrui[1];Li, Shaojie[1];Liu, Wei[2];Wang, Jia[3];Deng, Donghao[2];Liu, Pusheng[4];Tian, Peng[5];Liu, Chuang[2];Yan, Wenfu[1];Zhu, Kake[3];Wang, Zhendong[2];Liu, Zhongmin[5];Yu, Jihong[1,4]

机构：[1]Jilin Univ, Coll Chem, State Key Lab Inorgan Synth & Preparat Chem, Changchun 130012, Peoples R China;[2]Sinopec Shanghai Res Inst Petrochem Technol Co Ltd, State Key Lab Green Chem Engn & Ind Catalysis, Shanghai 201208, Peoples R China;[3]East China Univ Sci & Technol, Sch Chem Engn, State Key Lab Green Chem Engn & Ind Catalysis, Shanghai 200237, Peoples R China;[4]Jilin Univ, Int Ctr Future Sci, Changchun 130012, Peoples R China;[5]Chinese Acad Sci, Natl Engn Lab Methanol Olefins, Dalian Natl Lab Clean Energy, Dalian Inst Chem Phys, Dalian 116023, Peoples R China

年份：2025

卷号：147

期号：20

起止页码：16922

外文期刊名：JOURNAL OF THE AMERICAN CHEMICAL SOCIETY

收录：;EI(收录号：20252018408560);WOS:【SCI-EXPANDED(收录号:WOS:001484234700001)】；

基金：We acknowledge the financial support from the National Natural Science Foundation of China (22288101, 22472054), the National Key Research and Development Program of China (2021YFA1501202), and the "111 Center" (B17020) for supporting this work. We acknowledge Yaqi Fan and Yanhang Ma in School of Physical Science and Technology & Shanghai Key Laboratory of High-resolution Electron Microscopy, Shanghai Tech University for the help on TEM characterizations and Lei Wang in School of Chemistry and Molecular Engineering, Nanjing Tech University for the help on the Rietveld refinement of conventional NaY zeolite and as-synthesized/calcined Y21.28.

语种：英文

外文关键词：Fluid catalytic cracking - Gasoline - Liquefied petroleum gas - Petroleum coke - Quartz - Rietveld method - Silica fume - Silica gel - Synchrotron radiation

摘要：Ultrastable Y (USY) zeolites (Faujasite-type, FAU) with high SiO2/Al2O3 ratios (SARs) have been widely applied in fluidized catalytic cracking and hydrocracking processes. However, their preparation typically involves labor-intensive post-treatments that inevitably introduce defects, extra-framework species, and compositional gradients. Herein, we report the direct synthesis of FAU-type zeolite with a record-high SAR up to 21.28, which shows superior catalytic performance in the catalytic cracking of cumene and straight-run diesel. This was achieved by using a highly siliceous initial gel and seed, together with low charge-density organic structure-directing agents (OSDAs) of tetramethylammonium (TMA+) and tetrabutylammonium (TBA+) cations, while minimizing the use of high charge-density inorganic Na+ cations. Comprehensive NMR analyses, including two-dimensional (2D) heteronuclear correlation (HETCOR) experiments (1H-13C, 1H-27Al, 1H-29Si), and synchrotron radiation X-ray diffraction-based Rietveld refinements, revealed that (1) TMA+ and TBA+ preferentially interact with Si species over Al species in the initial gel, promoting Si incorporation into the FAU structure's long-range order; and (2) TMA+ cations were tightly confined within the sodalite (sod) cages, while TBA+ cations occupied the faujasite (fau) supercages, adopting folded butyl chain configurations. The encapsulation of low charge-density OSDA cations, coupled with the exclusion of high charge-density Na+ cations, resulted in a highly siliceous Y zeolite with a SAR of 21.28. The synthesized Y zeolite exhibited improved durability and enhanced activity in cumene cracking and comparable selectivity for the target products [liquefied petroleum gas (LPG) and gasoline] while reducing coke formation by 28% in straight-run diesel catalytic cracking compared to conventional USY zeolites.