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Controlled hydrodeoxygenation of lignin-derived anisole over supported Pt on UiO-66 based-catalysts through defect engineering approach
Fuel Processing Technology ( IF 7.2 ) Pub Date : 2021-09-04 , DOI: 10.1016/j.fuproc.2021.107001
Dieu-Phuong Phan , Van Nhieu Le , Jinsoo Kim , Eun Yeol Lee

Herein, we report a series of Platinum (Pt) phase loading on the highly porous channels of the metal-organic framework (MOF) introduces open Lewis acid sites through a defective-effect, which are crucial for selective hydrodeoxygenation (HDO) process of anisole. Thereby, UiO-66 (University of Oslo) based-supports were synthesized by a microwave-assisted solvothermal method using isophthalic acid (IPA) as a mixed linker at different concentrations. The total amount of acid sites in the defective UiO-66 samples was 1.5–2.5 times higher than that of pristine UiO-66, with the corresponding linker deficiency increasing to 1.94 as the concentration of the mixed linker was increased to 30% in the starting material. Consequently, the 3Pt/defective UiO-66 catalysts achieved better catalytic performance for the anisole HDO process, with a turn-over frequency (TOF) value of the Pt site being 2–3 times higher than that of the pristine 3Pt/UiO-66. Notably, the reaction pathway shifted from producing cyclohexane to producing benzene through the demethoxylation of anisole. This resulted in an increase in the TOF value based on the benzene yield by over 10 times as the defective linker content increased from 0 to 20%. The catalytic stability was also investigated using a series of Pt/defective UiO-66 catalysts.



中文翻译:

通过缺陷工程方法在 UiO-66 基催化剂上控制木质素衍生苯甲醚在负载 Pt 上的加氢脱氧

在此,我们报告了金属有机骨架 (MOF) 的高多孔通道上的一系列铂 (Pt) 相负载通过缺陷效应引入了开放的路易斯酸位点,这对于苯甲醚的选择性加氢脱氧 (HDO) 过程至关重要. 因此,使用间苯二甲酸(IPA)作为不同浓度的混合接头,通过微波辅助溶剂热法合成了基于 UiO-66(奥斯陆大学)的载体。有缺陷的 UiO-66 样品中酸性位点的总量是原始 UiO-66 的 1.5-2.5 倍,相应的接头缺陷随着起始混合接头浓度增加到 30% 增加到 1.94材料。因此,3Pt/有缺陷的 UiO-66 催化剂对苯甲醚 HDO 工艺实现了更好的催化性能,Pt 位点的翻转频率 (TOF) 值是原始 3Pt/UiO-66 的 2-3 倍。值得注意的是,反应途径从生产环己烷转变为通过苯甲醚脱甲氧基生产苯。随着有缺陷的接头含量从 0% 增加到 20%,这导致基于苯产率的 TOF 值增加了 10 倍以上。还使用一系列 Pt/有缺陷的 UiO-66 催化剂研究了催化稳定性。

更新日期:2021-09-04
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