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    稠环芳烃基碳材料用于电催化CO2还原研究进展

    Recent advances in polycyclic aromatic hydrocarbon-based carbon materials for electrocatalytic CO2 reduction

    • 摘要: 电催化二氧化碳还原反应(eCO2RR)是实现碳循环和储存可再生能源的关键技术。开发高效和低成本的碳基电催化剂是当前研究的热点。源自煤炭、石油及其工业副产物等化石资源的稠环芳烃(PAHs),因其结构可调、成本低廉、资源丰富以及富含多环芳香结构等优势,成为构建高效eCO2RR催化剂的理想前驱体。系统梳理了基于化石资源衍生PAHs基碳材料在eCO2RR中的研究进展,首先阐述了不同化石资源衍生PAHs的组成特征及预处理方法,阐明了酸碱洗涤脱灰、预氧化交联改性及溶剂萃取分离等预处理工艺在提升碳纯度、优化组分分布和提升前驱体热稳定性方面的关键作用,为后续高性能碳材料的制备奠定基础;其次,重点总结了将化石资源衍生PAHs转化为高性能碳催化剂的核心构筑策略,包括活化法构建分级多孔结构、模板法调控形貌及缺陷工程优化电子结构与活性位点密度;随后,深入探讨了材料结构与eCO2RR性能之间的构效关系,阐明了比表面积、孔隙结构及活性位点配位环境对传质效率、中间体吸附能及产物选择性的调控作用,并强调了先进表征与理论计算在揭示反应机理中的关键作用。最后,讨论了化石资源衍生PAHs基碳材料在前驱体复杂性高、反应机理不明、多碳产物选择性低和规模化程度不足的挑战,并展望了分子结构设计、原位表征耦合理论计算、机器学习以及规模化应用等未来研究方向。

       

      Abstract: The electrocatalytic CO2 reduction reaction (eCO2RR) represents a pivotal technology for closing the anthropogenic carbon cycle and enabling renewable energy storage. Thus, the development of cost-effective, high-performance carbon-based electrocatalysts has emerged as a critical research frontier. Fossil resource-derived polycyclic aromatic hydrocarbons (PAHs) sourced from coal, petroleum, and their industrial byproducts have emerged as ideal precursors for constructing high-performance electrocatalysts for the CO2 reduction reaction (eCO2RR), owing to their structural tunability, low cost, abundant availability, and intrinsic richness in polycyclic aromatic frameworks. This review provides a comprehensive overview of recent advances in the conversion of fossil resource-derived PAHs into advanced carbon-based electrocatalysts for eCO2RR. It first outlines the physicochemical characteristics of diverse fossil resource-derived PAHs feedstocks and the associated pretreatment protocols, elucidating how processes-including acid-base deashing, pre-oxidative cross-linking, and selective solvent extraction-enhance carbon purity and thermal stability. Subsequently, key synthetic strategies are summarized, including the construction of hierarchical pores via chemical or physical activation, morphological regulation via templating, and the modulation of electronic structures and active sites via defect engineering. Furthermore, the intrinsic relationships between physicochemical properties (e.g., pore architecture, active site coordination) and catalytic performance (e.g., mass transfer, intermediate adsorption, selectivity) are analyzed. The indispensable role of advanced characterization and theoretical calculations in unraveling reaction mechanisms is also highlighted. Finally, the challenges associated with fossil resource-derived PAHs-based carbon materials are discussed, including the high complexity of precursors, insufficient understanding of reaction mechanisms, low selectivity toward multi-carbon products, and limited scalability. Future directions focusing on molecular design, integrated in-situ characterization and computation, machine learning, and scalable applications are also outlined.

       

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