Cellulose-Based Composite Hydrogels for Heavy Metal Ion Removal: Recent Advances and Engineering Perspectives.

With the rapid intensification of industrial and agricultural activities, water contamination by heavy metal ions has emerged as a critical global challenge, gravely imperiling ecosystem stability and public health. Among the various remediation technologies, adsorption has been widely adopted due to its high efficiency, low-cost water treatment, and simplicity of operation. However, conventional inorganic or synthetic adsorbents often exhibit poor degradability and pose a risk of secondary contamination, substantially limiting their sustainable application. Consequently, the development of environmentally benign and renewable adsorbent materials has become a central research focus in this field. Recently, cellulose-based composite hydrogels, derived from renewable resources and characterized by excellent eco-friendliness and highly tunable three-dimensional porous structures, have attracted considerable attention as promising green adsorption materials. These hydrogels demonstrate outstanding performance in the efficient sequestration of heavy metal contaminants from aqueous environments. This review systematically summarizes recent advances in cellulose-based composite hydrogels for heavy metal removal, to elucidate the structure-performance relationships linking material fabrication strategies, structural modulation, and adsorption efficiency. First, we outline the principal construction approaches, including physical crosslinking, chemical modification, and supramolecular self-assembly, and comprehensively analyze how different synthesis routes regulate pore architecture, mechanical properties, and the distribution of surface functional groups. Second, the underlying adsorption mechanisms, primarily coordination complexation, electrostatic interactions, and ion exchange, are discussed in detail. Finally, recent studies on the adsorption of cationic heavy metals (e.g., Pb(II), Cu(II), and Cd(II)) and anionic oxyanions (e.g., As(III) and Cr(VI)) are critically reviewed, with particular emphasis on the relationships between selective adsorption performance, material design principles, and specific recognition mechanisms. Overall, this review provides a theoretical foundation and practical guidance for the design and development of next-generation water treatment materials with high adsorption capacity, excellent selectivity, non-toxicity, and strong environmental compatibility, followed by future research recommendations.