Cascade upgrading of bio-based 4'-methoxypropiophenone to anethole enabled by hot-compressed alcohol over a Hf-phytic acid coordination catalyst

文献类型： 外文期刊

第一作者： Tan, Jinyu

作者： Tan, Jinyu;Wu, Hongguo;Huang, Jinshu;Jian, Yumei;Zhang, Heng;Li, Hu;Yang, Song;Tan, Jinyu

作者机构：

关键词： Hot-compressed alcohol; 4'-methoxypropiophenone; Anethole; Cascade reaction; Heterogeneous catalysts

期刊名称：JOURNAL OF SUPERCRITICAL FLUIDS （ 影响因子：4.514； 五年影响因子：4.303 ）

ISSN： 0896-8446

年卷期： 2022 年 189 卷

页码：

收录情况： SCI

摘要： Hot compressed solvents (alcohol, water) have been widely used in the production of value-added chemicals from biomass due to their sufficiently low viscosity, high diffusivity, and environmentally-benign features. Anethole (AN) is a unique kind of natural aromatic compound, while its green synthesis method still requires to be explored. Herein, a novel porous acid-base bifunctional phytic acid (PA)-hafnium (Hf)(1:2.5) catalyst was prepared by a simple assembly of PA with Hf under a one-pot hydrothermal method (120 C, 24 h). The PA-Hf(1: 2.5) possessed outstanding catalytic activity for the synthesis of AN from 4'-methoxypropiophenone (4-MOPP) at 220 C and 15 bar in 2-pentanol (4-MOPP conversion: 99.8%, AN yield: 98.8%), which can be ascribed to its moderate surface area (95.3 m2/g), pore volume (0.18 cm3/g), mesopores (4.0 nm), and acid-base couple sites (density: 3.6 vs 1.7 mmol/g). 2-Pentanol was determined to serve as the superior hydrogen donor and solvent for the overall conversion process, which can remarkably hinder side reactions in this hot-compressed medium. Moreover, the cooperative interaction of Lewis acid-base couple sites (Hf4+-O2-) and Bronsted acidic species (-OH) of PA-Hf(1:2.5) led to its excellent catalytic performance. PA-Hf(1:2.5) was highly reusable with constant activity after five reaction cycles.

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