Carbon Microsphere-Coated Composites via Layer-by-Layer Self-Assembly with Enhanced Dye Adsorption Performance

In this work, monodisperse carbon microspheres with an average diameter of approximately 900 nm were successfully synthesized via a hydrothermal method. To further tailor their surface properties, the layer-by-layer (LbL) self-assembly technique was employed, where the cationic polyelectrolyte poly(diallyldimethylammonium chloride) (PDDA) and the anionic polyelectrolyte poly(styrene sulfonate) (PSS) were alternately deposited on the microsphere surface, forming two and four bilayer assemblies, respectively. The resulting composite microspheres exhibited remarkable adsorption performance toward representative dyes in water solution, such as rhodamine B (RhB) and methylene blue (MB). Experimental results demonstrated that the incorporation of a single bilayer significantly reduced the specific surface area but introduced additional active adsorption sites, thereby enhancing dye removal efficiency. However, when the number of bilayers was further increased to two, partial pore coverage and blockage occurred, leading to a reduced surface area and consequently diminished adsorption capacity. These findings highlight that in LbL surface modification, more layers do not necessarily yield better performance, but rather an optimal assembly thickness exists. This insight provides valuable guidance for the rational design of advanced adsorbent materials for wastewater treatment.