Advances in Fe-based catalysts for the hydrogenation of carbon dioxide toward higher alcohols
摘要
Global warming has intensified the urgency of reducing carbon dioxide (CO2) emissions and developing high-efficiency CO2 conversion technologies. The hydrogenation of CO2 to higher alcohols (HA) is a promising approach to realize carbon cycling and mitigate emissions, as HA is a class of compounds widely used as alternative fuels, gasoline additives, and organic solvents. This route confers notable environmental and economic values and has thus become a research hotspot in the field of CO2 resource utilization. Nevertheless, the large-scale synthesis of HA via CO2 hydrogenation is still constrained by inherent challenges. These include the high chemical inertness of CO2 that leads to difficult activation, intricate reaction pathways with numerous competing side reactions, and poor product selectivity accompanied by the formation of methane, light hydrocarbons, and other byproducts. These bottlenecks have hampered the industrialization process and promoted in-depth explorations worldwide. Moreover, in the catalytic system, noble metal catalysts represented by Rh-based ones exhibit excellent selectivity toward CO2 hydrogenation products, but suffer from low CO2 conversion and high cost, which limits their industrial application. In contrast, non-noble metal catalysts have the advantage of low raw material cost and tunable activity. Among them, Fe-based catalysts are considered one of the most promising catalytic systems for this reaction due to their excellent CO2 activation capability. Hence, this review focuses on Fe-based catalysts for CO2 hydrogenation to HA, systematically summarizing the latest research progress in their design principles and practical applications. Specifically, it sequentially elaborates on the regulation and modification of metal promoters, the screening and functional modification of carrier materials, and the fundamental regulatory principles of catalytic mechanisms. It comprehensively clarifies the influence mechanisms and optimization approaches of each key factor on catalytic performance. Finally, the critical issues remaining in current research and the prospective directions for future development in this field are discussed.