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Linear-regioselective hydromethoxycarbonylation of styrene using Ru-clusters/CeO2 catalyst

Chinese Journal of Catalysis 2020年第6期41卷 963-969页

作者： Jinghua An Yehong Wang Zhixin Zhang Jian Zhang Martin Gocyla Rafal EDunin-Borkowski Feng Wang State Key Laboratory of Catalysis Dalian National Laboratory for Clean EnergyDalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023LiaoningChina University of Chinese Academy of Sciences Beijing 100049China Ernst Ruska Centre for Microscopy and Spectroscopy with Electrons and Peter Grünberg Institute Forschungszentrum Juelich GmbHJuelich 52425Germany

Hydroalkoxycarbonylation of olefins has been considered to be one of the most attractive methods to synthesize esters. Controlling the regioselectivities of linear esters(L) and branched esters(B) is a challenging project for researchers working in this reaction. Although most of the attention has been paid to control the regioselectivity through ligand design in homogeneous catalytic systems, study in the area is still limited. Herein, Ru-clusters/CeO2 is employed as a heterogeneous catalyst for the hydromethoxycarbonylation of styrene without any additives. After optimization of the reaction conditions, the conversion of styrene is > 99% with 83% and 12% regioselectivity of linear and branched ester, respectively. By using different supports(CeO2(nanoparticle), CeO2-rod, and CeO2-cube), three catalysts including Ru-clusters/CeO2, Ru/CeO2-rod, and Ru/CeO2-cube are prepared and applied in the reaction. Structural characterizations demonstrate that the L/B ratio is related to the Ru size of supported Ru catalysts. Further Raman characterization and NH3-TPD demonstrate that the metal-support interaction and the concentration of oxygen vacancy of the catalyst have a great influence on the Ru size. The mechanism and kinetic analysis for this reaction are also investigated in this work.

关键词： Regioselectivity Ru-clusters/CeO2 Ester hydromethoxycarbonylation Olefins Heterogeneous catalysis

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