Synergistic effect of Cu and Mo over Cu–Mo–SiO2 catalyst prepared by sol-gel method for high-efficient and stable de-methoxylation of lignin-derived 4-propylguaiacol

IF 3.9 2区 化学 Q2 CHEMISTRY, PHYSICAL Molecular Catalysis Pub Date : 2024-11-21 DOI:10.1016/j.mcat.2024.114697
Hexuan Zhang , Qi Zeng , Song Song , Wuyu Zhao , Xingang Li
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Abstract

Mo-based catalysts are promising candidates for the de-methoxylation reaction in lignin valorization due to their unique behavior toward the cleavage of C–O bonds. However, the catalytic activities of Mo-based catalysts currently are still unsatisfactory and suffer from severe deactivation. Herein, we report a novel approach for the construction of robust Cu-modified Mo–SiO2 catalysts by sol-gel method through the synergistic effect of Cu and Mo, among which 0.33Cu–Mo–SiO2-580 with a Cu/Mo molar ratio of 0.33 exhibited the best catalytic performance for the de-methoxylation of lignin-derived 4-propylguaiacol. Remarkably, the space time yield of 4-propylphenol is among the highest value in literature data. The detailed characterizations confirm that the introduction of Cu by sol-gel method leads to the formation of highly dispersed CuMoO4 on the as-calcined samples, which results in the enhanced interaction between Cu and Mo species and the formation of a large amount of electron-deficient Mo0 on the as-reduced catalyst. Mechanistic studies reveal that electron-deficient Mo0 on 0.33Cu–Mo–SiO2-580 will not only enhance the adsorption ability of substrate, but also improve the C–O bond cleavage ability for the de-methoxylation reaction. Meanwhile, the hydrogen spillover effect induced by Cu0 is beneficial to the enhancement of the catalytic activity and stability of 0.33Cu–Mo–SiO2-580 catalyst.

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溶胶-凝胶法制备的 Cu-Mo-SiO2 催化剂上 Cu 和 Mo 的协同效应用于木质素衍生的 4-丙基愈创木酚的高效稳定脱甲氧基化反应
由于钼基催化剂在 C-O 键裂解方面具有独特的行为,因此是木质素价值化过程中脱甲氧基反应的理想候选催化剂。然而,目前 Mo 基催化剂的催化活性仍不尽人意,存在严重的失活现象。在此,我们报告了一种新方法,即通过 Cu 和 Mo 的协同作用,利用溶胶-凝胶法构建稳健的 Cu 改性 Mo-SiO2 催化剂,其中 Cu/Mo 摩尔比为 0.33 的 0.33Cu-Mo-SiO2-580 在木质素衍生的 4-丙基愈创木酚的脱甲氧基反应中表现出最佳催化性能。值得注意的是,4-丙基苯酚的时空产率是文献数据中最高的。详细的表征结果证实,通过溶胶-凝胶法引入 Cu 后,在煅烧样品上形成了高度分散的 CuMoO4,从而增强了 Cu 和 Mo 物种之间的相互作用,并在还原催化剂上形成了大量的缺电子 Mo0。机理研究表明,0.33Cu-Mo-SiO2-580 上的缺电子 Mo0 不仅能增强对底物的吸附能力,还能提高脱甲氧基反应中 C-O 键的裂解能力。同时,Cu0 诱导的氢溢出效应有利于提高 0.33Cu-Mo-SiO2-580 催化剂的催化活性和稳定性。
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来源期刊
Molecular Catalysis
Molecular Catalysis Chemical Engineering-Process Chemistry and Technology
CiteScore
6.90
自引率
10.90%
发文量
700
审稿时长
40 days
期刊介绍: Molecular Catalysis publishes full papers that are original, rigorous, and scholarly contributions examining the molecular and atomic aspects of catalytic activation and reaction mechanisms. The fields covered are: Heterogeneous catalysis including immobilized molecular catalysts Homogeneous catalysis including organocatalysis, organometallic catalysis and biocatalysis Photo- and electrochemistry Theoretical aspects of catalysis analyzed by computational methods
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