Amine-bilayer-functionalized cellulose-chitosan composite hydrogel for the efficient uptake of hazardous metal cations and catalysis in polluted water

Herein, we represent a novel ecofriendly bilayer-amine group incorporated microcrystalline cellulose (MCC)/chitosan (CS) hydrogel, fabricated via integrating polydopamine (PDA) and polyethyleneimine (PEI) for reliable and effective extraction of copper (Cu²⁺), zinc (Zn²⁺), and nickel (Ni²⁺) ions from effluents. Owing to abundant adsorptive sites, the MCC-PDA-PEI/CS-PDA-PEI hydrogel showed excellent Cu²⁺, Zn²⁺, and Ni²⁺ adsorbabilities of ~434.8, ~277.7, and ~261.8 mg/g, respectively, in a single-ion adsorption system with the adsorption kinetics and isotherm complied with pseudo-second-order and Langmuir models, respectively. In a multi-ion adsorption system, hydrogel removes mixed metal cations with slightly higher selectivity for Cu²⁺. In accordance with X-ray photoelectron and Fourier-transform-infrared spectrometric analyses, a plausible binding mechanism of metal cations on the as-prepared hydrogel was proposed by chelation between hydrogel functional groups and metal ions. In the repetitive adsorption/desorption experiments, the hydrogel retained >40% metal ion adsorption and desorption capacities after four cycles. Furthermore, the Cu²⁺-adsorbing hydrogel could serve as a support for the in situ development of Cu nanoparticles, which showed excellent catalytic performance as demonstrated by the transformation of 4-nitrophenol (4-NP) to 4-aminophenol. This work provides a novel ecofriendly, reusable, and highly-efficient adsorbent, as well as a biocatalyst for remediation of heavy metal cations and 4-NP polluted effluents.