Deactivation mechanism of acetone to isobutene conversion over Y/Beta catalyst

doi:10.1016/S1872-2067(24)60097-5

Abstract

Abstract:

The conversion of acetone derived from biomass to isobutene has attracted extensive attentions. In comparison with Brønsted acidic catalyst, Lewis acidic catalyst could exhibit a better catalytic performance with a higher isobutene selectivity. However, the catalyst stability remains a key problem for the long-running acetone conversion and the reasons for catalyst deactivation are poorly understood up to now. Herein, the deactivation mechanism of Lewis acidic Y/Beta catalyst during the acetone to isobutene conversion was investigated by various characterization techniques, including acetone-temperature-programmed surface reaction, gas chromatography-mass spectrometry, in situ ultraviolet-visible, and ¹³C cross polarization magic angle spinning nuclear magnetic resonance spectroscopy. A successive aldol condensation and cyclization were observed as the main side-reactions during the acetone conversion at Lewis acidic Y sites. In comparison with the low reaction temperature, a rapid formation and accumulation of the larger cyclic unsaturated aldehydes/ketones and aromatics could be observed, and which could strongly adsorb on the Lewis acidic sites, and thus cause the catalyst deactivation eventually. After a simple calcination, the coke deposits could be easily removed and the catalytic activity could be well restored.

Key words: Deactivation mechanism, Acetone to isobutene, Lewis acid sites, Y/Beta, Spectroscopy

Chang Wang, Tingting Yan, Weili Dai. Deactivation mechanism of acetone to isobutene conversion over Y/Beta catalyst[J]. Chinese Journal of Catalysis, 2024, 64: 133-142.

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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(24)60097-5

https://www.cjcatal.com/EN/Y2024/V64/I9/133

Figures/Tables 8

Scheme 1. Reaction network of the acetone to isobutene conversion.

Fig. 1. Acetone conversion (a) and product selectivity (b) in the acetone to isobutene conversion over Y/Beta, [Si]Beta and Y2O3 catalysts. Reaction conditions: 573-773 K, WHSV = 1.0/h.

Fig. 2. Catalytic performance of fresh and regenerated Y/Beta zeolite in the acetone to isobutene conversion at 623 (a) and 723 K (b) with a TOS of 15 h.

Fig. 3. TPSR profiles recorded during the acetone (a), diacetone alcohol (b) and mesityl oxide (c) conversion. Reaction conditions: 303-773 K, WHSV = 1.0/h.

Fig. 4. (a) TP-UV-vis spectra recorded during the acetone conversion in the temperature range of 303-773 K over Y/Beta catalysts. In situ UV-vis spectra recorded during the acetone to isobutene conversion at 423 (b) and 623 K (c) with a TOS of 30 min over Y/Beta catalyst. Reaction conditions: WHSV = 1/h. (d) Possible assignments of UV-vis bands correspond to the acetone to isobutene conversion over Y/Beta catalyst.

Fig. 5. 13C CP MAS NMR spectra of [Si]Beta (a) and Y/Beta (b) recorded after adsorption of acetone-2-13C at different reaction temperature with a TOS of 5 min. 13C CPMAS NMR spectra of Y/Beta recorded after adsorption of acetone-2-13C for TOS of 30 min at 423 (c) and 623 K (d).

Fig. 6. GC-MS chromatograms of organic extracts from Y/Beta catalysts obtained after the conversion of acetone to isobutene with different TOS at 423 (a) and 623 K (b). (c) Structures of the organic compounds occluded in the spent Y/Beta catalysts after the conversion of acetone to isobutene.

Scheme 2. Proposed reaction pathway and the possible deactivation mechanism of the acetone to isobutene conversion over Y/Beta catalyst.

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