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    稠环芳烃选择性加氢的催化调控策略:机理、挑战与展望

    Catalytic regulation strategies for selective hydrogenation of polycyclic aromatic hydrocarbons: mechanisms, challenges and perspectives

    • 摘要: 煤焦油中富含稠环芳烃,其选择性加氢不仅是消除持久性环境污染的手段,更是制备高能量密度航空燃料和液态有机储氢载体的关键技术。然而,受限于中间体脱芳构化引发的复杂竞争反应路径,该过程在加氢深度的精准调控方面仍面临巨大挑战。机理分析表明:催化剂表面稠环芳烃的吸附构型(受金属电子结构与几何结构调控)以及加氢中间体稳定性降低,是影响选择性的关键因素。系统综述了稠环芳烃选择性加氢的催化调控策略。在活性金属方面,重点探讨了如何通过合金化设计、尺寸效应及金属–载体相互作用的优化,增强活性位点对目标中间体的特异性识别能力,以平衡产物生成与脱附速率;在载体方面,阐述了利用孔道择形催化特性及氢溢流机制调控氢源空间分布对反应路径的导向作用。目前该领域研究在反应路径可视化、中间体动态行为追踪以及氢迁移定量分析方面仍存在明显不足。未来研究需综合运用原位表征、理论模拟与机器学习等方法,构建精确的“结构–选择性”构效关系模型,以指导高效催化剂的理性设计,进而突破煤焦油高值化利用的技术壁垒,实现新型能源化学品的精准合成。

       

      Abstract: Coal tar is rich in polycyclic aromatic hydrocarbons (PAHs). The selective hydrogenation of PAHs is not only a means to eliminate persistent environmental pollutants but also a key technology for producing high-energy-density aviation fuels and liquid organic hydrogen carriers (LOHCs). However, owing to the complex competitive reaction pathways triggered by the dearomatization of intermediates, this process still faces significant challenges in the precise control of hydrogenation depth. Mechanistic analysis reveals that the adsorption configuration of PAHs on the catalyst surface (regulated by the electronic and geometric structures of the metal) and the reduced stability of hydrogenation intermediates are key factors affecting selectivity. This paper systematically reviews the catalytic regulation strategies for the selective hydrogenation of PAHs. Regarding active metals, the review highlights how alloying design, size effects, and the optimization of metal-support interactions (MSI) enhance the specific recognition capability of active sites for target intermediates, thereby balancing product generation and desorption rates. Regarding supports, it expounds on the guiding role of regulating the spatial distribution of hydrogen species via pore shape-selective catalysis and hydrogen spillover mechanisms in directing reaction pathways. Currently, research in this field still exhibits significant gaps in the visualization of reaction pathways, the tracking of the dynamic behavior of intermediates, and the quantitative analysis of hydrogen migration. Future studies need to integrate in-situ characterization, theoretical simulations, and machine learning to construct precise "structure-selectivity" relationship models. This will guide the rational design of high-efficiency catalysts, thereby breaking through the technical barriers to the high-value utilization of coal tar and achieving the precise synthesis of novel energy chemicals.

       

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