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; Michael Tsapatsis

doi:10.1002/anie.202104574

Few-Unit-Cell MFI Zeolite Synthesized using a Simple Di-quaternary Ammonium Structure-Directing Agent

Angew Chem Int Ed Engl. 2021 Aug 23;60(35):19214-19221. doi: 10.1002/anie.202104574. Epub 2021 Aug 1.

Authors

Peng Lu¹, Supriya Ghosh², Matheus Dorneles de Mello^{3

4}, Huda Sharbini Kamaluddin⁵, Xinyu Li², Gaurav Kumar², Xuekui Duan², Milinda Abeykoon⁶, J Anibal Boscoboinik^{3

4

7}, Liang Qi^{8

9}, Heng Dai¹⁰, Tianyi Luo¹, Shaeel Al-Thabaiti⁵, Katabathini Narasimharao⁵, Zaheer Khan⁵, Jeffrey D Rimer¹⁰, Alexis T Bell^{8

9}, Paul Dauenhauer², K Andre Mkhoyan², Michael Tsapatsis^{1

11}

Affiliations

¹ Department of Chemical and Biomolecular Engineering &, Institute for NanoBioTechnology, Johns Hopkins University, 3400 N. Charles Street, Baltimore, MD, 21218, USA.
² Department of Chemical Engineering and Materials Science, University of Minnesota, 421 Washington Avenue SE, Minneapolis, MN, 55455, USA.
³ Catalysis Center for Energy Innovation, University of Delaware, Newark, DE, 19716, USA.
⁴ Center for Functional Nanomaterials, Brookhaven National Laboratory, Upton, NY, 11973, USA.
⁵ Department of Chemistry, Faculty of Science, King Abdulaziz University, Jeddah, 21589, Saudi Arabia.
⁶ National Synchrotron Light Source II, Brookhaven National Laboratory, Upton, NY, 11973, USA.
⁷ Department of Materials Science and Chemical Engineering, State University of New York at Stony Brook, 100 Nicolls Rd, Stony Brook, NY, 11794, USA.
⁸ Chemical Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, CA, 94720, USA.
⁹ Department of Chemical and Biomolecular Engineering, University of California, Berkeley, CA, 94720, USA.
¹⁰ Department of Chemical and Biomolecular Engineering, University of Houston, Houston, TX, 77204, USA.
¹¹ Applied Physics Laboratory, Johns Hopkins University, 11100 Johns Hopkins Road, Laurel, MD, 20723, USA.

Abstract

Synthesis of a pentasil-type zeolite with ultra-small few-unit-cell crystalline domains, which we call FDP (few-unit-cell crystalline domain pentasil), is reported. FDP is made using bis-1,5(tributyl ammonium) pentamethylene cations as structure directing agent (SDA). This di-quaternary ammonium SDA combines butyl ammonium, in place of the one commonly used for MFI synthesis, propyl ammonium, and a five-carbon nitrogen-connecting chain, in place of the six-carbon connecting chain SDAs that are known to fit well within the MFI pores. X-ray diffraction analysis and electron microscopy imaging of FDP indicate ca. 10 nm crystalline domains organized in hierarchical micro-/meso-porous aggregates exhibiting mesoscopic order with an aggregate particle size up to ca. 5 μm. Al and Sn can be incorporated into the FDP zeolite framework to produce active and selective methanol-to-hydrocarbon and glucose isomerization catalysts, respectively.

Keywords: adsorption; catalysis; di-quaternary structure directing agents; pentasil; ultrasmall crystalline domain.

Abstract

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