CeO2 形貌调控的 Rh/CeO2 催化剂上烯烃的高效催化加氢甲酰化,Industrial & Engineering Chemistry Research

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CeO2 形貌调控的 Rh/CeO2 催化剂上烯烃的高效催化加氢甲酰化
Industrial & Engineering Chemistry Research ( IF 3.8 ) Pub Date : 2024-02-12 , DOI: 10.1021/acs.iecr.3c03882
Gong Zeng ₁ , Yunfeng Zheng ₂ , Guoqiang He ₁ , Cheng Zhang _{1,

3} , Hangning Chen ₄ , Lixia Liang ₃ , Pan Liu ₃ , Jiantai Ma ₁ , Zhengping Dong ₁

Affiliation

烯烃的加氢甲酰化代表了高附加值醛制备的经济上可持续且广泛的工业应用。本文采用简单的浸渍还原方法制备了一系列具有不同形貌（棒状、多面体和八面体）的氧化铈（CeO _{2 ）催化剂，Rh活性位点均匀地分散在CeO}₂表面。由于催化剂中氧空位的存在，产生了不饱和位点，优化了催化剂表面CO的吸附能，降低了反应能垒。由此可见，所得催化剂表现出良好的催化性能。所制备的三种催化剂的氧空位浓度(D/F _2g )依次为：CeO ₂ -R-Rh (0.47) > CeO ₂ -P-Rh (0.42) > CeO ₂ -O-Rh (0.36)。CeO ₂ -R-Rh表现出优异的催化苯乙烯加氢甲酰化活性，在低合成气压力和无磷酸盐配体下苯乙烯转化率为99%，醛选择性为98%。同时，CeO ₂ -R-Rh对各种其他烯烃的加氢甲酰化表现出优异的通用性，意味着广泛的潜在应用。本文提出的通过金属氧化物负载界面的强相互作用来调节催化性能的策略为理解加氢甲酰化反应提供了新的视角。

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Efficient Catalytic Hydroformylation of Alkenes on Rh/CeO2 Catalysts Modulated by CeO2 Morphology

The hydroformylation of alkenes represents an economically sustainable and widespread industrial application for high-value-added aldehyde preparation. Herein, a series of cerium oxide (CeO₂) catalysts with various morphologies (rods, polyhedra, and octahedra) were prepared using a simple impregnation-reduction method, and Rh active sites were evenly dispersed on the CeO₂ surface. Due to the existence of oxygen vacancies in the catalysts, unsaturated sites were generated, the adsorption energy of CO on the catalyst surfaces was optimized, and the reaction energy barrier was reduced. Thus, the obtained catalysts showed a good catalytic performance. The oxygen vacancy concentration (D/F_2g) of the three prepared catalysts followed the order: CeO₂-R-Rh (0.47) > CeO₂-P-Rh (0.42) > CeO₂-O-Rh (0.36). CeO₂-R-Rh showed excellent catalytic styrene hydroformylation activity, with 99% styrene conversion and 98% aldehyde selectivity under a low syngas pressure and phosphate-free ligands. At the same time, CeO₂-R-Rh showed excellent general applicability for the hydroformylation of various other alkenes, implying a broad scope of potential applications. The strategy presented herein for adjusting catalytic performance through the strong interaction of the metal-oxide-supported interface contributes fresh perspectives to understanding the hydroformylation reaction.

更新日期：2024-02-12

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