Amino acid-assisted synthesis of TS-1 zeolites containing highly catalytically active TiO6 species

doi:10.1016/S1872-2067(21)63882-2

Chinese Journal of Catalysis ›› 2021, Vol. 42 ›› Issue (12): 2189-2196.DOI: 10.1016/S1872-2067(21)63882-2

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Amino acid-assisted synthesis of TS-1 zeolites containing highly catalytically active TiO₆ species

Yuyao Wang^a, Li Li^a, Risheng Bai^a, Shiqin Gao^a, Zhaochi Feng^c, Qiang Zhang^a^,^#(), Jihong Yu^a^,^b^,^*()

^aState Key Laboratory of Inorganic Synthesis and Preparative Chemistry, College of Chemistry, Jilin University, Changchun 130012, Jilin, China
^bInternational Center of Future Science, Jilin University, Changchun 130012, Jilin, China
^cState Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, Liaoning, China

Received:2021-05-08 Accepted:2021-05-08 Online:2021-12-18 Published:2021-07-07
Contact: Qiang Zhang,Jihong Yu
About author:# E-mail: qiangz@jlu.edu.cn
* Tel/Fax: +86-431-85168608; E-mail: jihong@jlu.edu.cn;
Supported by:
National Natural Science Foundation of China(21920102005);National Natural Science Foundation of China(21835002);National Natural Science Foundation of China(21621001);111 Project(B17020)

Abstract

Abstract:

Tailoring the Ti coordination states in titanosilicate zeolites to simultaneously improve feedstock conversion and maximize the target product selectivity remains a challenge in the pursuit of high-performance catalysts for selective oxidation reactions. Herein, we provide a facile strategy to synthesize hierarchical anatase-free TS-1 (MFI-type) zeolites with tetrahedrally coordinated (TiO₄) and octahedrally coordinated Ti species (TiO₆). The TiO₄ species provide high epoxide selectivity, while the TiO₆ species afford improved alkene conversion. This strategy is achieved by synergistically using an L-lysine-assisted approach and a two-step crystallization; the two-step crystallization approach prevents the formation of anatase TiO₂, while L-lysine stabilizes the TiO₆ species and ensures efficient incorporation of TiO₆ into the anatase-free TS-1 zeolites. Compared with their conventional counterparts, which only contain TiO₄ species, the as-prepared TS-1 zeolites (Si/Ti = 36.9) result in a higher 1-hexene conversion (33%), higher TON value (153), and comparable epoxide selectivity (95%). This synthetic strategy provides avenues to tailor the amount and distribution of Ti species in titanosilicate zeolites to achieve high catalytic performances in various processes.

Key words: TS-1 zeolites, Ti species, L-Lysine-assisted approach, 1-Hexene epoxidation

Yuyao Wang, Li Li, Risheng Bai, Shiqin Gao, Zhaochi Feng, Qiang Zhang, Jihong Yu. Amino acid-assisted synthesis of TS-1 zeolites containing highly catalytically active TiO₆ species[J]. Chinese Journal of Catalysis, 2021, 42(12): 2189-2196.

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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(21)63882-2

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Figures/Tables 4

Fig. 1. XRD patterns (a), FTIR spectra (b), UV-vis spectra (c), and UV-Raman spectra excited at 266 nm (d) of the TS-1 zeolites.

Fig. 2. TEM images of TS-1-SL0-36 (a), TS-1-TL0-76 (b), TS-1-TL0.1-56 (c), and TS-1-TL0.2-36 (d).

Scheme 1. Proposed evolution of the TiO6 species stabilized by L-lysine in TS-1 zeolites.

Fig. 3. (a) Epoxidation reaction routes directed by TiO4 (closed sites) and TiO6 (open sites) species in the TS-1 zeolites, respectively; (b)1-Hexene conversion over the different TS-1 zeolites; (c) 1-Hexene conversion and product selectivity of the recycle test performed using TS-1-TL0.2-36.

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Amino acid-assisted synthesis of TS-1 zeolites containing highly catalytically active TiO₆ species

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