Citation: Zhongkui Zhao, Jinfeng Ran, Yongle Guo, Boyuan Miao, Guiru Wang. Tuning of the textural features and acidic properties of sulfated mesoporous lanthana-zirconia solid acid catalysts for alkenylation of diverse aromatics to their corresponding α-arylstyrenes[J]. Chinese Journal of Catalysis, ;2016, 37(8): 1303-1313. doi: 10.1016/S1872-2067(15)61118-4 shu

Tuning of the textural features and acidic properties of sulfated mesoporous lanthana-zirconia solid acid catalysts for alkenylation of diverse aromatics to their corresponding α-arylstyrenes

State Key Laboratory of Fine Chemicals, Department of Catalysis Chemistry and Engineering, School of Chemical Engineering, Dalian University of Technology, Dalian 116024, Liaoning, China

Received Date: 17 March 2016
Revised Date: 20 April 2016

Fund Project: This work was financially supported by the National Natural Science Foundation of China (21276041), the Program for New Century Excellent Talents in University of Ministry of Education (NCET-12-0079), the Natural Science Foundation of Liaoning Province (2015020200), and the Fundamental Research Funds for the Central Universities (DUT15LK41).

The textural features and acidic properties of sulfated mesoporous lanthana-zirconia solid acids (SO₄^2-/meso-La_0.1Zr_0.9O_δ) were efficiently tuned by modifying the conditions used to prepare the meso-La_0.1Zr_0.9O_δ composites, such as the molar ratio of the template to La and Zr metal ions (N_t/m), molar ratio of ammonia to La and Zr metal ions (N_a/m), hydrothermal temperature (T_hydro), and hydrothermal time (t_hydro). The effect of the textural features and acidic properties on the catalytic performance of solid acid catalysts for alkenylation of p-xylene with phenylacetylene was investigated. Various characterization techniques such as N₂ physisorption, X-ray diffraction, NH₃ temperature-programmed desorption, and thermogravimetric analysis were employed to reveal the relationship between the nature of catalyst and its catalytic performance. It was found that the catalytic performance significantly depended on the textural features and acidic properties, which were strongly affected by preparation conditions of the meso-La_0.1Zr_0.9O_δ composite. Appropriate acidic sites and high accessibility were required to obtain satisfactory catalytic reactions for this reaction. It was also found that the average crystallite size of t-ZrO₂ affected by the preparation conditions had significant influence on the ultrastrong acidic sites of the catalysts. The optimized SO₄^2-/meso-La_0.1Zr_0.9O_δ catalyst exhibited much superior catalytic activity and coke-resistant stability. Moreover, the developed SO₄^2-/meso-La_0.1Zr_0.9O_δ catalyst demonstrated excellent catalytic performance for alkenylation of diverse aromatics with phenylacetylene to their corresponding α-arylstyrenes. Combining the previously established complete regeneration of used catalysts by a facile calcination process with the improved catalytic properties, the developed SO₄^2-/meso-La_0.1Zr_0.9O_δ solid acid could be a potential catalyst for industrial production of α-arylstyrenes through clean and atom efficient solid-acid-mediated Friedel-Crafts alkenylation of diverse aromatics with phenylacetylene.
- Mesoporous solid acid,
- Alkenylation,
- Clean synthesis,
- Alkenyl aromatics,
- Textural and acidic properties,
- Tuning
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