Department of Environmental Science and Engineering, Fudan University
Shanghai Technical Service Platform for Pollution Control and Resource Utilization of Organic Waste
Shanghai Key Laboratory of Atmospheric Particle Pollution and Prevention(LAP3)
Shanghai Institute of Pollution Control and Ecological Security

由于化石能源的枯竭和环境污染的加剧,发展可再生能源和实现碳中和势在必行。木质素作为大量存在的天然芳香族聚合物,经过解聚升级可制备高附加值的化学品和燃料,有望替代化石资源。然而,木质素解聚产生的生物油和化合物因其高含氧量而限制了其直接应用。加氢脱氧策略为开发高价值的生物基燃料和化学品提供了一条潜在路径。传统高压分子氢气主导的木质素增值转化存在安全性隐患,阻碍了其工业化推广。木质素原位催化加氢脱氧作为其替代策略,采用溶剂和木质素自身基团作为氢源,在催化剂作用下原位产氢并作用于反应底物实现其高效增值转化。该方法不仅有效避免了外部高压供氢,而且能在温和条件下实现木质素原位升级,提高了原子利用率和产物选择性。通过对木质素原位催化加氢脱氧策略的研究,总结梳理了近年来原位供氢的研究进展,分析了联合水相重整加氢脱氧、联合金属水解加氢脱氧、催化转移氢化、自供氢氢解四种常用原位催化加氢脱氧策略的反应机理,讨论了几种策略的研究现状,并展望了木质素原位催化加氢脱氧策略的研究重点、难点和发展前景。

The development of renewable energy and carbon neutrality is imperative due to the depletion of fossil fuels and environmental pollution. Lignin, as the abundant natural aromatic polymer, can be converted into high-value chemicals and fuels, offering an alternative to fossil resources. The bio-oil and chemicals generated from lignin depolymerization have limited direct applications due to their high oxygen content. The strategy of hydrodeoxygenation (HDO) provides a pathway for the devel opment of high - value biobased fuels and chemicals. However, the traditional lignin conversion process, which is dominated by high-pressure molecular hydrogen, poses safety hazards, hindering its industrial promotion. In-situ catalytic HDO of lignin can be an alternative strategy. It utilizes solvents or lignin′s functional groups as hydrogen sources. During the catalytic process, hydrogen is generated in situ and acts on the substrate, achieving efficient value-added conversion. This method not only effec tively avoids the need for external high-pressure hydrogen supply but also enables in-situ upgrading of lignin under mild conditions, improving atomic utilization and product selectivity. Through the study of in-situ catalytic HDO strategies for lignin, the research progress of in-situ hydrogen supply in recent years is summarized. The analysis includes the reaction mechanisms of four commonly used in-situ cat alytic HDO strategies: combined reforming and HDO (RHDO), combined metal hydrolysis and HDO process ( HHDO ), catalytic transfer hydrogenation ( CTH ), and self - supported hydrogenolysis (SSH). The status of various strategies is discussed, and the research focus, challenges, and prospects of in-situ catalytic HDO strategies for lignin are explored.

国家自然科学基金资助项目(22278085)

赵玉莹,詹佳慧,胡锐,等.木质素原位催化加氢脱氧研究进展[J].能源环境保护,2024,38(2):32-42.

ZHAO Yuying, ZHAN Jiahui, HU Rui, et al. Research progress on in-situ catalytic hydrodeoxygenation of lignin[J]. Energy Environmental Protection, 2024, 38(2): 32-42.