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A half-century overview of heteroatom functionalized carbonaceous materials for aqueous redox flow batteries: from mechanism insights to design strategies
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DOI：10.1016/j.pmatsci.2026.101787.png)
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Abstract
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Redox flow batteries (RFBs) represent a cornerstone for large-scale long-duration energy storage; however, the sluggish redox kinetics of carbonaceous electrodes remain the primary bottleneck for high-power-density applications. Over the past half-century, while heteroatom functionalization has emerged as a pivotal strategy for electrode modification, the field is still challenged by a lack of mechanistic clarity and significant debates regarding the identification of active sites. This scientific impasse stems from the multi-dimensional coupling inherent in electrode modification: a single treatment typically triggers the simultaneous evolution of specific surface area, defects, functional groups, and doping elements, making it exceptionally challenging to decouple individual contributions to catalytic activity. This review aims to resolve these long-standing discrepancies by exploring advancements in heteroatom-functionalized carbonaceous materials and their significant impact on enhancing the electrochemical performance of RFBs. Various substrates are evaluated, ranging from traditional carbon felts, papers, and cloths to emerging electrospun and biomass-derived fibers, etc. Methodologies for their treatment are systematically discussed, including thermal, chemical, and electrochemical techniques. A key focus is placed on the roles of oxygen, nitrogen, and multi-element doping, alongside a forward-looking discussion on single-atom and dual-atom catalysts. The review highlights the current challenges in this field and potential future directions, underscoring the pivotal role of these advanced materials in enhancing the capabilities of RFBs for sustainable energy storage.
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