Alcohol-assisted synthesis of high-silica zeolites in the absence of organic structure-directing agents

doi:10.1016/S1872-2067(20)63677-4

Abstract

Abstract:

In this work, we show for the first time that high-silica zeolites (MFI, TON, MTT, and *MRE) could be synthesized from a combined strategy of both zeolite seeding and alcohol filling in the absence of organic structure-directing agents (OSDAs). High-silica ZSM-5 zeolites with Si/Al ratios ranging from 38 to 240 (TF-Al-ZSM-5) could be synthesized via this route. The key to the success of this technique was the employment of an aluminosilicate precursor with a fully 4-coordinated aluminum species as the initial source, wherein the rearrangement and condensation of the silicate species, rather than the aluminate species, occurred during zeolite crystallization. In addition, heteroatoms, such as Fe and B, could be incorporated into the zeolite frameworks. Catalytic tests for the methanol-to-propylene (MTP) reaction exhibited good catalytic performance for TF-Al-ZSM-5, which was comparable to that of the aluminosilicate ZSM-5 zeolite synthesized with OSDAs. Hence, this method offers viable opportunities for the industrial production and catalytic application of high-silica zeolites in the future.

Key words: Zeolite, High silica, Seed directing, Alcohol filling, Catalytic performance

Huimin Luan, Chi Lei, Ye Ma, Qinming Wu, Longfeng Zhu, Hao Xu, Shichao Han, Qiuyan Zhu, Xiaolong Liu, Xiangju Meng, Feng-Shou Xiao. Alcohol-assisted synthesis of high-silica zeolites in the absence of organic structure-directing agents[J]. Chinese Journal of Catalysis, 2021, 42(4): 563-570.

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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(20)63677-4

https://www.cjcatal.com/EN/Y2021/V42/I4/563

Figures/Tables 7

Fig. 1. Schematic representation of the synthesis of high-silica zeolites.

Fig. 2. XRD pattern (a), SEM image (b), N2 sorption isotherms (c), 27Al MAS NMR spectrum (d), TG curve (e), and 13C MAS NMR spectrum (f) of the aluminosilicate ZSM-5 zeolite sample.

Table 1 The Si/Al ratios of the aluminosilicate precursors and zeolite.

Run ^a	Si/Al ratios of precursors	Si/Al ratios of products
1	38	35
2	60	60
3	80	80
4	191	180
5	240	230

Fig. 3. XRD patterns (a), 27Al MAS NMR spectra (b), and 29Si MAS NMR spectra (c) of the TF-Al-ZSM-5-80 zeolite crystallized at 0 (1), 6 (2), 12 (3), 18 (4), 24 (5), 36 (6), and 48 h (7). In Fig. 3(c), the red line is the original peak, and the black lines are the deconvoluted peaks. The original peak was deconvolved into several peaks using the Lorenz decomposition fitting model.

Fig. 4. Methanol conversion and product selectivities over the aluminosilicate TF-ZSM-5 zeolite with a Si/Al ratio of 80 in the product at 480 °C (▼, Conv.; ■, C2=; ●, C3=; ◆, C4=; ★, C5+).

Fig. 5. (a) XRD patterns of TF-Fe-ZSM-5 (1) and TF-B-ZSM-5 (2) zeolites; (b) UV-Vis spectrum of TF-Fe-ZSM-5 zeolite; (c) 11B MAS NMR spectrum of TF-B-ZSM-5 zeolite.

Fig. 6. XRD patterns (a), SEM images (b), and 27Al MAS NMR spectra (c) of TF-Al-TON (1), TF-Al-MTT (2), and TF-Al-*MRE (3) zeolites.

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