利用掺入 MoO3 的 Co-BTC MOF 衍生的 MoCoOx@C 提高香兰素及其同系化合物的加氢脱氧活性,Dalton Transactions

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利用掺入 MoO3 的 Co-BTC MOF 衍生的 MoCoOx@C 提高香兰素及其同系化合物的加氢脱氧活性
Dalton Transactions ( IF 3.5 ) Pub Date : 2023-02-03 , DOI: 10.1039/d2dt03744k
Ashish Kumar Kar _{1,

2} , Surinder Pal Kaur ₂ , T J Dhilip Kumar ₂ , Rajendra Srivastava _{1,

2}

Affiliation

木质素衍生的芳基醚和香草醛是满足可再生芳香化合物需求的重要平台化学品。在此，报道了一种高效的多相催化剂，用于通过选择性加氢脱氧途径将香兰素重整为 2-甲氧基-4-甲基苯酚 (MMP)，这是医药、食品和石化工业的前体。_{通过用不同含量的MoO 3}棒修饰Co-BTC MOF，然后进行碳化，合成了一系列MoCoO _{x @C催化剂。}在这些催化剂中，MoCoO _x @C-2 在 150 °C 下在水性介质中 1.5 小时内提供了～99% 的香草醛转化率和～99% 的 MMP 选择性。相反，CoO _x@C提供~75%的香草醛转化率和~85%的MMP选择性。详细的催化剂表征表明，CoO _x和 Co ₂ Mo ₃ O ₈是有助于提高 MoCoO _x @C-2 活性的活性物质。MoCoO _x @C-2优异的H ₂吸附特性和酸性有利于香兰素和其他同系化合物的加氢脱氧。DFT 吸附能计算表明香草醛和香草醇与MoCoO _x_{中的 Co 2} Mo ₃ O _{8位点有良好的相互作用}@C-2。该催化剂可有效循环 5 次，第 5 次循环后活性损失可忽略不计。这些发现系统地解释了基于混合金属氧化物的 MoCoO _x @C-2 催化剂的活性位点，用于香兰素选择性加氢脱氧为 MMP，这对于学术和工业催化界具有重要意义。

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Improving the hydrodeoxygenation activity of vanillin and its homologous compounds by employing MoO3-incorporated Co-BTC MOF-derived MoCoOx@C

Lignin-derived aryl ethers and vanillin are essential platform chemicals that fulfil the demands for renewable aromatic compounds. Herein, an efficient heterogeneous catalyst is reported for reforming vanillin via a selective hydrodeoxygenation route to 2-methoxy-4-methyl phenol (MMP), a precursor to medicinal, food, and petrochemical industries. A series of MoCoO_x@C catalysts were synthesized by decorating the Co-BTC MOF with different contents of MoO₃ rods, followed by carbonization. Among these catalysts, MoCoO_x@C-2 afforded ∼99% vanillin conversion and ∼99% MMP selectivity at 150 °C in 1.5 h in an aqueous medium. In contrast, CoO_x@C afforded ∼75% vanillin conversion and ∼85% MMP selectivity. Detailed catalyst characterization revealed that CoO_x and Co₂Mo₃O₈ were the active species contributing to the higher activity of MoCoO_x@C-2. The excellent H₂-adsorption characteristics and acidity of MoCoO_x@C-2 were beneficial to the hydrodeoxygenation of vanillin and other homologous compounds. The DFT adsorption energy calculations suggested the favourable interactions of vanillin and vanillyl alcohol with the Co₂Mo₃O₈ sites in MoCoO_x@C-2. The catalyst could be efficiently recycled 5 times, with a negligible loss in activity after the 5th cycle. These findings provide a systematic explication of the active sites of the mixed metal oxide-based MoCoO_x@C-2 catalyst for the selective hydrodeoxygenation of vanillin to MMP, which is important for the academic and industrial catalysis community.

更新日期：2023-02-03

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