| Summary: | This study focused on a comparison of the adsorption properties of graphene oxide (GO) and its composites that were prepared via cross-linking with chitosan (CTS) or Al<sup>3+</sup> species, respectively. Comparative material characterization was achieved by several complementary methods: SEM, NMR spectroscopy, zeta-potential, dye-based adsorption, and gas adsorption at equilibrium and dynamic conditions. SEM, solids NMR, and zeta-potential results provided supporting evidence for cross-linking between GO and the respective cross-linker units. The zeta-potential of GO composites decreased upon cross-linking due to electrostatic interactions and charge neutralization. Equilibrium and kinetic adsorption profiles of the GO composites with methylene blue (MB) in aqueous media revealed superior uptake over pristine GO. The monolayer adsorption capacity (mg g<sup>−1</sup>) of MB are listed in descending order for each material: GO−CTS (408.6) > GO−Al (351.4) > GO (267.1). The gas adsorption results showed parallel trends, where the surface area and pore structure of the composites exceeded that for GO due to <i>pillaring effects</i> upon cross-linking. The green strategy reported herein for the preparation of tunable GO-based composites revealed versatile adsorption properties for diverse heterogeneous adsorption processes.
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