Abstract：
Bio-oil derived from biomass fast pyrolysis can be upgraded to gasoline and diesel alternatives by catalytic hydrodeoxygenation (HDO). Here, the novel nitrogen-doped carbon-alumina hybrid supported cobalt (Co/NCAn, n = 1, 2.5, 5) catalyst is established by a coagulation bath technique. The optimized Co/NCA2.5 catalyst presented 100 % conversion of guaiacol, high selectivity to cyclohexane (93.6 %), and extremely high deoxygenation degree (97.3 %), respectively. Therein, the formation of cyclohexanol was facilitated by stronger binding energy and greater charge transfer between Co and NC which was unraveled by density functional theory calculations. In addition, the appropriate amount of Lewis acid sites enhanced the cleavage of the C-O bond in cyclohexanol, finally resulting in a remarkable selectivity for cyclohexane. Finally, the Co/NCA2.5 catalyst also exhibited excellent selectivity (93.1 %) for high heating value hydrocarbon fuel in crude bio-oil HDO. This work provides a theoretical basis on N dopants collaborating alumina hybrid catalysts for efficient HDO reaction.
摘要：
来自生物质快速热解的生物油可以通过催化加氢脱氧（HDO）升级为汽油和柴油替代品。这里,新型氮掺杂碳-氧化铝杂化负载钴(Co/NCAn，n=1，2.5，5）催化剂是通过凝固浴技术建立的。优化的Co/NCA2.5催化剂的愈创木酚转化率为100%,对环己烷的高选择性（93.6％），和极高的脱氧度（97.3%），分别。其中,Co和NC之间更强的结合能和更大的电荷转移促进了环己醇的形成，这被密度泛函理论计算所揭示。此外,适量的路易斯酸位点增强了环己醇中C-O键的裂解，最终对环己烷产生显著的选择性。最后,Co/NCA2.5催化剂对粗生物油HDO中的高热值烃燃料也表现出优异的选择性(93.1%)。这项工作为N掺杂剂协同氧化铝杂化催化剂高效HDO反应提供了理论依据。
