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The Synergy of Alloyed Pd and Ni Over H-NbOx: Enhancing Hydrogenation of Lignin Derivatives and Lignin Bio-Oil into Cyclic Hydrocarbons and Alcohols
ACS Sustainable Chemistry & Engineering ( IF 7.1 ) Pub Date : 2024-06-27 , DOI: 10.1021/acssuschemeng.4c03323
Ganesh Sunil More 1 , Rajaram Bal 2 , Rajendra Srivastava 1
Affiliation  

The study aims to investigate the hydrogenation of lignin-derived bio-oil (known as lignin bio-oil) and β-O-4 linkages, which are representative lignin model compounds. The hydrogenation of these molecules produces cyclic hydrocarbons and aromatic platform chemicals. H-NbOx was synthesized using a hydrothermal method, followed by an acid treatment of Nb2O5. Three wt % Pd and 3 wt % Ni were deposited over H-NbOx to form an alloyed PdNi/H-NbOx catalyst. XPS, NH3-TPD, and O2-TPD revealed intrinsic active sites, metal–support interactions, and modified oxygen vacancies, making it highly efficient for the hydrogenation of 2-phenoxy-1-phenylethanol (PPE-OL) in dodecane using 3 MPa hydrogen. The hydrogenation of PPE-OL yielded >98% cyclic hydrocarbons (cyclohexane and ethyl cyclohexane). In contrast, 3Pd/H-NbOx and 3Ni/H-NbOx showed varied selectivity, producing a mixture of ethylbenzene, phenol, ethyl cyclohexane, and cyclohexanol. Notably, catalytic transfer hydrogenation (CTH) resulted in the formation of >99% aromatics (phenol and ethylbenzene) in isopropanol. Expanding the investigation from model compounds, PdNi/H-NbOx was utilized to hydrogenate lignin bio-oil derived from wheat straw, yielding saturated cyclic alcohols with a high yield at 250 °C in isopropanol. It underscores the potential of the developed protocol to effectively meet energy demands by generating aromatics via catalytic transfer hydrogenation and cyclic hydrocarbons via hydrogenation.

中文翻译:


合金化 Pd 和 Ni 在 H-NbOx 上的协同作用:增强木质素衍生物和木质素生物油氢化成环状烃和醇



该研究旨在研究木质素衍生的生物油(称为木质素生物油)和β-O-4键的氢化,它们是代表性的木质素模型化合物。这些分子的氢化产生环烃和芳香族平台化学品。采用水热法合成H-NbO x ,然后对Nb 2 O 5 进行酸处理。将 3 wt% Pd 和 3 wt% Ni 沉积在 H-NbO x 上,形成合金化 PdNi/H-NbO x 催化剂。 XPS、NH 3 -TPD 和 O 2 -TPD 揭示了固有活性位点、金属-载体相互作用和修饰的氧空位,使其能够高效地氢化 2-苯氧基使用 3 MPa 氢气在十二烷中制备 -1-苯基乙醇 (PPE-OL)。 PPE-OL 的氢化产生 >98% 的环烃(环己烷和乙基环己烷)。相比之下,3Pd/H-NbO x 和 3Ni/H-NbO x 显示出不同的选择性,产生乙苯、苯酚、乙基环己烷和环己醇的混合物。值得注意的是,催化转移氢化 (CTH) 导致在异丙醇中形成 >99% 的芳烃(苯酚和乙苯)。从模型化合物扩展研究,PdNi/H-NbO x 被用来氢化源自麦秆的木质素生物油,在异丙醇中于250℃下高产率地产生饱和环醇。它强调了所开发的协议通过催化转移加氢生成芳烃和通过加氢生成环烃来有效满足能源需求的潜力。
更新日期:2024-06-27
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