Hydrodeoxygenation of lignin-derived phenolics to cycloalkanes over Ni–Co alloy coupled with oxophilic NbO

氢解 加氢脱氧 愈创木酚 双功能 自然键轨道 化学 合金 除氧 材料科学 有机化学 化学工程 无机化学 催化作用 分子 选择性 工程类
作者
Chengzhi Zhang,Xing Zhang,Jingfeng Wu,Lingjun Zhu,Shurong Wang
出处
期刊:Applied Energy [Elsevier BV]
卷期号:328: 120199-120199 被引量:75
标识
DOI:10.1016/j.apenergy.2022.120199
摘要

• The Ni–Co alloy and oxophilic species co-catalyzed deoxygenation by hydrogenolysis. • A high selectivity of cycloalkanes (98.9%) was obtained in the HDO of guaiacol. • The 5Ni–5Co/NbO x catalyst also showed high stability and applicability. Hydrodeoxygenation (HDO) of lignin-derived bio-oil is a promising route to produce advanced biofuels. However, the removal of oxygen-containing functional groups with high bond strength in bio-oil challenges the development of efficient, stable, and inexpensive catalysts. In this study, a series of bifunctional catalysts were synthesized by coupling Ni–Co alloy with an oxophilic NbO x support, which was used for the HDO of lignin-derived phenolics to produce cycloalkanes. The Ni–Co alloy formed on the bimetallic catalysts during calcination and reduction was verified by TEM, XPS, and H 2 -TPR measurements, which showed excellent hydrogenolysis activity. The composition of the Ni–Co alloy was the most uniform with a Ni/Co molar ratio of 1, and the catalyst achieved the highest catalytic activity. The oxygen vacancies provided by the NbO x support also enhanced the adsorption of phenolics and promoted the removal of oxygen-containing functional groups by forming a specific configuration. The synergistic catalysis of Ni–Co alloy and oxygen vacancies achieved complete conversion of guaiacol with a high cycloalkane selectivity of 98.9 % under optimal conditions (300 °C, 3 MPa H 2 , and 2 h). More importantly, only marginal deactivation occurred on the 5Ni–5Co/NbO x catalyst after 5 cycles and it was also successfully applied to the efficient conversion of other complex lignin-derived phenolics. Therefore, an efficient and economical strategy of coupling the Ni–Co alloy with an oxophilic NbO x support to catalyze the HDO of lignin-derived phenolics to produce cycloalkanes was prospective.
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