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High-Efficiency Catalytic Hydrodeoxygenation of Lignin-Derived Vanillin with Nickel-Supported Metal Phosphate Catalysts
Chemical Engineering Journal ( IF 15.1 ) Pub Date : 2022-06-23 , DOI: 10.1016/j.cej.2022.137723
Jie Gao , Yang Cao , Gang Luo , Jiajun Fan , James H. Clark , Shicheng Zhang

Lignin is a natural and renewable aromatic raw material of aromatic chemicals and its depolymerization and downstream products conversion has drawn considerable attention. Herein, a series of Ni loaded metal phosphates (Ni/MP, M=Ti, Zr, Nb, La, or Ce) catalysts were fabricated for the hydrodeoxygenation (HDO) of lignin-derived vanillin (VAN) to produce 2-methoxy-4-methylphenol (MMP). It has been demonstrated that 97.25% VAN conversion could be obtained with a yield of 88.39% of MMP under the mild condition of 220 oC and 0.5 MPa H2 for 30 min with 15wt% Ni/ZrP. The highest activity of Ni/ZrP was attributed to its small Ni particle size, large specific surface area, strong metal-support interaction, and optimal acidity. It has been proven that Ni, Lewis acid sites (LAS) and Brønsted acid sites (BAS) have a synergistic effect in VAN conversion: Nano-sized Ni catalyze the dissociation of H2 to form active hydrogen species (H). LAS promote the adsorption and activation of VAN and isopropanol. BAS play a vital role in the dehydration reaction. Additionally, H2 was the primary hydrogen donor in the system, while isopropanol was the reaction medium as well as the secondary hydrogen donor, helping to reduce the external H2 supply requirement. By optimizing the reaction conditions and studying the promotion mechanism, we hope to provide an experimental basis for lignin catalytic hydrogenolysis.



中文翻译:

镍负载金属磷酸盐催化剂对木质素衍生香兰素的高效催化加氢脱氧

木质素是一种天然可再生的芳烃原料,其解聚及下游产品转化备受关注。本文制备了一系列负载镍的金属磷酸盐(Ni/MP、M=Ti、Zr、Nb、La 或 Ce)催化剂,用于木质素衍生的香草醛 (VAN) 的加氢脱氧 (HDO) 以生产 2-甲氧基- 4-甲基苯酚 (MMP)。已经证明,在 220 o C 和 0.5 MPa H 2的温和条件下,VAN 转化率为 97.25%,MMP 收率为 88.39%用 15wt% Ni/ZrP 处理 30 分钟。Ni/ZrP的最高活性归因于其小Ni粒径、大比表面积、强金属-载体相互作用和最佳酸度。已经证明Ni、Lewis酸位(LAS)和Brønsted酸位(BAS)在VAN转化中具有协同作用:纳米Ni催化H 2解离形成活性氢物种(H )。LAS促进VAN和异丙醇的吸附和活化。BAS在脱水反应中起着至关重要的作用。此外,H 2是系统中的主要供氢体,而异丙醇是反应介质和次要供氢体,有助于减少外部 H 2供应要求。通过优化反应条件和研究促进机理,希望为木质素催化氢解提供实验依据。

更新日期:2022-06-24
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