Zhong Yudan, Ma Yulong, Sun Yonggang, Wang Liqiong, Li Yuanyuan, Lin Feng, Zhu Yingbo
State Key Laboratory of High-efficiency Coal Utilization and Green Chemical Engineering, College of Chemistry and Chemical Engineering, Ningxia University Yinchuan China
RSC Adv. 2023 Jul 12;13(30):21063-21070. doi: 10.1039/d3ra01866k. eCollection 2023 Jul 7.
The lignin oil produced by rapid pyrolysis of lignin is considered a promising liquid fuel source. Hydrodeoxygenation (HDO) is a kind of efficient method to upgrade the lignin oil, and a high-performance catalyst is key to the hydrodeoxygenation of lignin oil. In this study, a high dispersion and small size Ru nanoparticle loaded N-doped carbon catalyst was derived by the direct pyrolysis of a mixture of ruthenium trichloride and melamine, and it could efficiently convert lignin oil. The lignin oil was completely transformed at 240 °C and 1 MPa H, and 36.58% cyclohexane was obtained. The formation, surface area, and nitrogen species of the catalyst could be controlled by changing the precursor of the nitrogen-doped carbon support. The percentage of pyridine nitrogen possessed with melamine as a nitrogen-carbon precursor (31.35%) was much higher than that with urea (16.47%) and dicyandiamide (8.20%) as nitrogen-carbon precursors. The presence of pyridine nitrogen could not only serve as the coordination site for even dispersity and stability of Ru nanoparticles but also regulated the electron density of Ru nanoparticles (NPs) and increased the active site Ru through electron transfer.
由木质素快速热解产生的木质素油被认为是一种很有前景的液体燃料来源。加氢脱氧（HDO）是提质木质素油的一种有效方法，而高性能催化剂是木质素油加氢脱氧的关键。在本研究中，通过三氯化钌和三聚氰胺混合物的直接热解制备了一种高分散、小尺寸的负载钌纳米颗粒的氮掺杂碳催化剂，该催化剂能有效转化木质素油。木质素油在240℃和1MPa氢气条件下完全转化，得到了36.58%的环己烷。通过改变氮掺杂碳载体的前驱体，可以控制催化剂的形成、表面积和氮物种。以三聚氰胺作为氮碳前驱体时吡啶氮的比例（31.35%）远高于以尿素（16.47%）和双氰胺（8.20%）作为氮碳前驱体时的比例。吡啶氮的存在不仅可以作为钌纳米颗粒均匀分散和稳定的配位位点，还能调节钌纳米颗粒（NPs）的电子密度，并通过电子转移增加活性位点钌。
