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Few‐Unit‐Cell MFI Zeolite Synthesized Using a Simple Di Angewandte Research Articles Chemie How to cite: Zeolites Very Important Paper International Edition: doi.org/10.1002/anie.202104574 German Edition: doi.org/10.1002/ange.202104574 Few-Unit-Cell MFI Zeolite Synthesized using a Simple Di-quaternary Ammonium Structure-Directing Agent Peng Lu, Supriya Ghosh, Matheus Dorneles de Mello, Huda Sharbini Kamaluddin, Xinyu Li, Gaurav Kumar, Xuekui Duan, Milinda Abeykoon, J. Anibal Boscoboinik, Liang Qi, Heng Dai, Tianyi Luo, Shaeel Al-Thabaiti, Katabathini Narasimharao, Zaheer Khan, Jeffrey D. Rimer, Alexis T. Bell, Paul Dauenhauer, K. Andre Mkhoyan, and Michael Tsapatsis* Abstract: Synthesis of a pentasil-type zeolite with ultra-small adsorption performance compared to conventional zeo- few-unit-cell crystalline domains, which we call FDP (few-unit- lites.[5–10] In this context, the quest for synthetic methods to cell crystalline domain pentasil), is reported. FDP is made minimize the size of crystalline zeolitic domains while using bis-1,5(tributyl ammonium) pentamethylene cations as accomplishing their arrangement to form hierarchical porous structure directing agent (SDA). This di-quaternary ammoni- materials and thin film membranes persists.[11] Of particular um SDA combines butyl ammonium, in place of the one importance is the synthesis of MFI with crystalline domains commonly used for MFI synthesis, propyl ammonium, and on the order of one to few unit cells (ca. 10 nm or less) due to a five-carbon nitrogen-connecting chain, in place of the six- anticipated uses in catalysis, adsorption and membranes.[5,12] carbon connecting chain SDAs that are known to fit well within Moreover, since MFI in its all-silica (zeosil) form has been the MFI pores. X-ray diffraction analysis and electron studied extensively as a prototype for templated crystal microscopy imaging of FDP indicate ca. 10 nm crystalline growth,[13–15] the synthesis of MFI crystals as close as possible domains organized in hierarchical micro-/meso-porous aggre- to their nucleation stage is of fundamental significance. Ryoo gates exhibiting mesoscopic order with an aggregate particle and co-workers, soon after their discovery of gemini-type size up to ca. 5 mm. Al and Sn can be incorporated into the oligo-quaternary ammonium surfactants as organic structure- FDP zeolite framework to produce active and selective directing agents (SDAs) leading to multilamellar 2-dimen- methanol-to-hydrocarbon and glucose isomerization catalysts, sional MFI,[3] they reported the synthesis of mesoporous respectively. materials with walls composed of few-unit-cell domains with the zeolite beta (BEA) and MFI-like framework topolo- Introduction gies.[16,17] We have shown that simpler short chain mono- and di-quaternary SDAs (i.e., without the dual porogenic ability Zeolites composed of one- to few-unit-cell domains,[1–4] of tri- to penta-quaternary ammonium gemini-surfactant exhibit distinct, and for some uses superior, catalytic and SDAs with C18 alkyl chains) are also capable of directing [*] Dr. P. Lu, Dr. T. Luo, Prof. M. Tsapatsis Dr. J. A. Boscoboinik Department of Chemical and Biomolecular Engineering & Department of Materials Science and Chemical Engineering, State Institute for NanoBioTechnology, Johns Hopkins University University of New York at Stony Brook 3400 N. Charles Street, Baltimore, MD 21218 (USA) 100 Nicolls Rd, Stony Brook, NY 11794 (USA) E-mail: [email protected] Dr. L. Qi, Prof. A. T. Bell S. Ghosh, X. Li, G. Kumar, X. Duan, Prof. P. Dauenhauer, Chemical Sciences Division, Lawrence Berkeley National Laboratory Prof. K. A. Mkhoyan Berkeley, CA 94720 (USA) Department of Chemical Engineering and Materials Science and University of Minnesota Department of Chemical and Biomolecular Engineering 421 Washington Avenue SE, Minneapolis, MN 55455 (USA) University of California, Berkeley, CA 94720 (USA) Dr. M. Dorneles de Mello, Dr. J. A. Boscoboinik H. Dai, Prof. J. D. Rimer Catalysis Center for Energy Innovation, University of Delaware Department of Chemical and Biomolecular Engineering Newark, DE 19716 (USA) University of Houston, Houston, TX 77204 (USA) and Prof. M. Tsapatsis Center for Functional Nanomaterials Applied Physics Laboratory, Johns Hopkins University Brookhaven National Laboratory, Upton, NY 11973 (USA) 11100 Johns Hopkins Road, Laurel, MD 20723 (USA) Dr. H. S. Kamaluddin, Prof. S. Al-Thabaiti, Prof. K. Narasimharao, Supporting information and the ORCID identification number(s) for Prof. Z. Khan the author(s) of this article can be found under: Department of Chemistry, Faculty of Science https://doi.org/10.1002/anie.202104574. King Abdulaziz University, Jeddah 21589 (Saudi Arabia) 2021 The Authors. Angewandte Chemie International Edition Dr. M. Abeykoon published by Wiley-VCH GmbH. This is an open access article under National Synchrotron Light Source II the terms of the Creative Commons Attribution Non-Commercial Brookhaven National Laboratory, Upton, NY 11973 (USA) NoDerivs License, which permits use and distribution in any medium, provided the original work is properly cited, the use is non- commercial and no modifications or adaptations are made. &&&& 2021 The Authors. Angewandte Chemie International Edition published by Wiley-VCH GmbH Angew. Chem. Int. Ed. 2021, 60,2–10 Ü Ü These are not the final page numbers! Angewandte Research Articles Chemie the growth of single- to few-unit-cell thick nanosheets by hindering growth along the b-axis of MFI.[4,11] However, the use of such simple SDAs to reduce crystalline domains down to few unit cells in directions other than the MFI b-axis has not yet been achieved. Here, we demonstrate that few-unit- cell MFI, with a highly broadened XRD pattern, can be synthesized using a relatively simple di-quaternary ammoni- um (bis-1,5(tributyl ammonium) pentamethylene) cation (called here tri-Bu-dC5) as an SDA. All-silica, aluminosili- cate, and stannosilicate MFI synthesis is reported along with sorption and catalytic properties. Synthesis of MFI and MEL with different crystal habit, stacking fault sequence and presence of rotational inter- [18–20] Scheme 1. Hypothesized opposing trends of tri-Bu-dC5 for minimizing growths has been studied extensively. We have demon- growth along all directions to generate ultra-small crystallites. Black, strated that at early stages of crystal growth (i.e., before green and red colors denote propyl, five methylene chain, and butyl crystal facets develop) bis-1,5(tripropyl ammonium) pentam- groups, respectively. ethylene cations (called here tri-Pr-dC5) hinder all growth rates compared to those observed using tetrapropyl ammo- nium (TPA), the typical SDA for MFI synthesis. Moreover, confirmed our anticipation that the frustrated tri-Bu-dC5 we have shown that at early stages of growth, tri-Pr-dC5 SDAwill not be a very effective SDA for MFI or MEL. Below, favors growth along the b-axis compared to the other it is shown that it is possible to grow highly crystalline few- crystallographic directions of MFI, while stacking faults and unit-cell pentasil zeolite, which we call FDP (few-unit-cell rotational intergrowths attributable to the presence of MEL crystalline domain pentasil zeolite). are not observed.[11,19] This finding combined with the well- established trends in MFI synthesis using its most common SDA, TPA cations, which favor growth along the c- and a- Results and Discussion axes, lead us to hypothesize that at early stages of crystal growth (i.e., before well-developed crystal facets emerge) the Characterization of the tri-Bu-dC5 SDA and its synthesis pentamethylene moiety is responsible for reversing the crystal procedure are provided in the Supporting Information. The shape of MFI from thin to long platelets along its b-axis. The SDAwas used in hydroxide form (tri-Bu-dC5(OH)2) obtained hypothesis that the pentamethylene moiety is responsible for by anion exchange of its bromide form (tri-Bu-dC5(Br)2). The favoring growth along the b-axis, is further corroborated by synthesis parameters along with crystal size and composition the finding that MFI growth using bis-1,6(tripropyl ammoni- of the FDP zeolites synthesized at 1208C are summarized in um) hexamethylene cations (tri-Pr-dC6) retains the b-axis as Table 1. We note here that conventional MFI was obtained at a slower growing direction. We have also demonstrated that the higher synthesis temperature of 1508C (Figure S2). The when using tetrabutyl ammonium (TBA) or phosphonium SDA exhibits structure-directing role towards MFI and was (TBP) SDAs, growth along the b-axis is hindered while MEL found to be preserved intact in the as-made product (Fig- presence and rotational intergrowths are enhanced leading to ure S3). single-unit-cell thick intergrown MFI nanosheets, a material The wide angle XRD pattern of the calcined Si-FDP (1) we call SPP (self-pillared pentasil).[4] Scheme 1 illustrates zeolite (see Table 1 for sample denotation) shows two these hypothesized opposing trends coded on bis-1,5(tributyl ammonium) pentamethylene cat- Table 1: Summary of synthesis parameters and compositions of calcined FDP zeolites obtained at ions (tri-Bu-dC5). Specifically, the 1208C. favoring and hindering of (i) Material Sol composition Crystallite size Si/Al or t [days] Rotation growth along the b-axis, (ii) MEL [nm][a] Si/Sn[b] or not stacking faults, and (iii) rotational H2O/SiO2 SDA/SiO2 intergrowths by different parts of Si-FDP (1) 38 0.15 6.0 – 7 yes the molecule. Si-FDP (2) 38 0.25 5.3 – 9 yes We decided to test the hypoth- Si-FDP (3) 13 0.15 7.3 – 3 yes esis that these opposing trends will Si-FDP (4) 13 0.25 5.2 – 7 yes create frustration in the SDA char- Si-FDP (5) 8 0.15 4.0 – 3 yes Al-FDP (1) 8 0.15 6.6 157 (100) 3 yes acteristics hindering crystal growth Al-FDP (2) 8 0.15 7.5 172 (200) 3 yes in all directions and limiting the Al-FDP (3) 8 0.15 7.1 260 (300) 3 yes resulting crystal size to few-unit- Al-FDP (4) 8 0.15 7.7 42 (50) 3 yes cells.
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